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This publications-based thesis summarizes my contribution to the scientific field of ultrafast structural dynamics. It consists of 16 publications, about the generation, detection and coupling of coherent gigahertz longitudinal acoustic phonons, also called hypersonic waves. To generate such high frequency phonons, femtosecond near infrared laser pulses were used to heat nanostructures composed of perovskite oxides on an ultrashort timescale. As a consequence the heated regions of such a nanostructure expand and a high frequency acoustic phonon pulse is generated. To detect such coherent acoustic sound pulses I use ultrafast variants of optical Brillouin and x-ray scattering. Here an incident optical or x-ray photon is scattered by the excited sound wave in the sample. The scattered light intensity measures the occupation of the phonon modes.
The central part of this work is the investigation of coherent high amplitude phonon wave packets which can behave nonlinearly, quite similar to shallow water waves which show a steepening of wave fronts or solitons well known as tsunamis. Due to the high amplitude of the acoustic wave packets in the solid, the acoustic properties can change significantly in the vicinity of the sound pulse. This may lead to a shape change of the pulse. I have observed by time-resolved Brillouin scattering, that a single cycle hypersound pulse shows a wavefront steepening. I excited hypersound pulses with strain amplitudes until 1% which I have calibrated by ultrafast x-ray diffraction (UXRD).
On the basis of this first experiment we developed the idea of the nonlinear mixing of narrowband phonon wave packets which we call "nonlinear phononics" in analogy with the nonlinear optics, which summarizes a kaleidoscope of surprising optical phenomena showing up at very high electric fields. Such phenomena are for instance Second Harmonic Generation, four-wave-mixing or solitons. But in case of excited coherent phonons the wave packets have usually very broad spectra which make it nearly impossible to look at elementary scattering processes between phonons with certain momentum and energy.
For that purpose I tested different techniques to excite narrowband phonon wave packets which mainly consist of phonons with a certain momentum and frequency. To this end epitaxially grown metal films on a dielectric substrate were excited with a train of laser pulses. These excitation pulses drive the metal film to oscillate with the frequency given by their inverse temporal displacement and send a hypersonic wave of this frequency into the substrate. The monochromaticity of these wave packets was proven by ultrafast optical Brillouin and x-ray scattering.
Using the excitation of such narrowband phonon wave packets I was able to observe the Second Harmonic Generation (SHG) of coherent phonons as a first example of nonlinear wave mixing of nanometric phonon wave packets.
What are the physical laws of the mutual interactions of objects bound to cell membranes, such as various membrane proteins or elongated virus particles? To rationalise this, we here investigate by extensive computer simulations mutual interactions of rod-like particles adsorbed on the surface of responsive elastic two-dimensional sheets. Specifically, we quantify sheet deformations as a response to adhesion of such filamentous particles. We demonstrate that tip-to-tip contacts of rods are favoured for relatively soft sheets, while side-by-side contacts are preferred for stiffer elastic substrates. These attractive orientation-dependent substrate-mediated interactions between the rod-like particles on responsive sheets can drive their aggregation and self-assembly. The optimal orientation of the membrane-bound rods is established via responding to the elastic energy profiles created around the particles. We unveil the phase diagramme of attractive–repulsive rod–rod interactions in the plane of their separation and mutual orientation. Applications of our results to other systems featuring membrane-associated particles are also discussed.
What are the physical laws of the mutual interactions of objects bound to cell membranes, such as various membrane proteins or elongated virus particles? To rationalise this, we here investigate by extensive computer simulations mutual interactions of rod-like particles adsorbed on the surface of responsive elastic two-dimensional sheets. Specifically, we quantify sheet deformations as a response to adhesion of such filamentous particles. We demonstrate that tip-to-tip contacts of rods are favoured for relatively soft sheets, while side-by-side contacts are preferred for stiffer elastic substrates. These attractive orientation-dependent substrate-mediated interactions between the rod-like particles on responsive sheets can drive their aggregation and self-assembly. The optimal orientation of the membrane-bound rods is established via responding to the elastic energy profiles created around the particles. We unveil the phase diagramme of attractive–repulsive rod–rod interactions in the plane of their separation and mutual orientation. Applications of our results to other systems featuring membrane-associated particles are also discussed.
We demonstrate new fluorophore-labelled materials based on acrylamide and on oligo(ethylene glycol) (OEG) bearing thermoresponsive polymers for sensing purposes and investigate their thermally induced solubility transitions. It is found that the emission properties of the polarity-sensitive (solvatochromic) naphthalimide derivative attached to three different thermoresponsive polymers are highly specific to the exact chemical structure of the macromolecule. While the dye emits very weakly below the LCST when incorporated into poly(N-isopropylacrylamide) (pNIPAm) or into a polyacrylate backbone bearing only short OEG side chains, it is strongly emissive in polymethacrylates with longer OEG side chains. Heating of the aqueous solutions above their cloud point provokes an abrupt increase of the fluorescence intensity of the labelled pNIPAm, whereas the emission properties of the dye are rather unaffected as OEG-based polyacrylates and methacrylates undergo phase transition. Correlated with laser light scattering studies, these findings are ascribed to the different degrees of pre-aggregation of the chains at low temperatures and to the extent of dehydration that the phase transition evokes. It is concluded that although the temperature-triggered changes in the macroscopic absorption characteristics, related to large-scale alterations of the polymer chain conformation and aggregation, are well detectable and similar for these LCST-type polymers, the micro-environment provided to the dye within each polymer network differs substantially. Considering sensing applications, this finding is of great importance since the temperature-regulated fluorescence response of the polymer depends more on the macromolecular architecture than the type of reporter fluorophore.
Derivatization of fullerene (C60) with branched aliphatic chains softens C60-based materials and enables the formation of thermotropic liquid crystals and room temperature nonvolatile liquids. This work demonstrates that by carefully tuning parameters such as type, number and substituent position of the branched chains, liquid crystalline C60 materials with mesophase temperatures suited for photovoltaic cell fabrication and room temperature nonvolatile liquid fullerenes with tunable viscosity can be obtained. In particular, compound 1, with branched chains, exhibits a smectic liquid crystalline phase extending from 84 °C to room temperature. Analysis of bulk heterojunction (BHJ) organic solar cells with a ca. 100 nm active layer of compound 1 and poly(3-hexylthiophene) (P3HT) as an electron acceptor and an electron donor, respectively, reveals an improved performance (power conversion efficiency, PCE: 1.6 ± 0.1%) in comparison with another compound, 10 (PCE: 0.5 ± 0.1%). The latter, in contrast to 1, carries linear aliphatic chains and thus forms a highly ordered solid lamellar phase at room temperature. The solar cell performance of 1 blended with P3HT approaches that of PCBM/P3HT for the same active layer thickness. This indicates that C60 derivatives bearing branched tails are a promising class of electron acceptors in soft (flexible) photovoltaic devices.
Semi-empirical sea-level models (SEMs) exploit physically motivated empirical relationships between global sea level and certain drivers, in the following global mean temperature. This model class evolved as a supplement to process-based models (Rahmstorf (2007)) which were unable to fully represent all relevant processes. They thus failed to capture past sea-level change (Rahmstorf et al. (2012)) and were thought likely to underestimate future sea-level rise. Semi-empirical models were found to be a fast and useful tool for exploring the uncertainties in future sea-level rise, consistently giving significantly higher projections than process-based models.
In the following different aspects of semi-empirical sea-level modelling have been studied. Models were first validated using various data sets of global sea level and temperature. SEMs were then used on the glacier contribution to sea level, and to infer past global temperature from sea-level data via inverse modelling. Periods studied encompass the instrumental period, covered by tide gauges (starting 1700 CE (Common Era) in Amsterdam) and satellites (first launched in 1992 CE), the era from 1000 BCE (before CE) to present, and the full length of the Holocene (using proxy data). Accordingly different data, model formulations and implementations have been used. It could be shown in Bittermann et al. (2013) that SEMs correctly predict 20th century sea-level when calibrated with data until 1900 CE. SEMs also turned out to give better predictions than the Intergovernmental Panel on Climate Change (IPCC) 4th assessment report (AR4, IPCC (2007)) models, for the period from 1961–2003 CE.
With the first multi-proxy reconstruction of global sea-level as input, estimate of the human-induced component of modern sea-level change and projections of future sea-level rise were calculated (Kopp et al. (2016)). It turned out with 90% confidence that more than 40 % of the observed 20th century sea-level rise is indeed anthropogenic. With the new semi-empirical and IPCC (2013) 5th assessment report (AR5) projections the gap between SEM and process-based model projections closes, giving higher credibility to both. Combining all scenarios, from strong mitigation to business as usual, a global sea-level rise of 28–131 cm relative to 2000 CE, is projected with 90% confidence. The decision for a low carbon pathway could halve the expected global sea-level rise by 2100 CE.
Present day temperature and thus sea level are driven by the globally acting greenhouse-gas forcing. Unlike that, the Milankovich forcing, acting on Holocene timescales, results mainly in a northern-hemisphere temperature change. Therefore a semi-empirical model can be driven with northernhemisphere temperatures, which makes it possible to model the main subcomponent of sea-level change over this period. It showed that an additional positive constant rate of the order of the estimated Antarctic sea-level contribution is then required to explain the sea-level evolution over the Holocene. Thus the global sea level, following the climatic optimum, can be interpreted as the sum of a temperature induced sea-level drop and a positive long-term contribution, likely an ongoing response to deglaciation coming from Antarctica.
Changes in extratropical storm track activity and their implications for extreme weather events
(2016)
In this thesis, the two prototype catalysts Fe(CO)₅ and Cr(CO)₆ are investigated with time-resolved photoelectron spectroscopy at a high harmonic setup. In both of these metal carbonyls, a UV photon can induce the dissociation of one or more ligands of the complex. The mechanism of the dissociation has been debated over the last decades. The electronic dynamics of the first dissociation occur on the femtosecond timescale.
For the experiment, an existing high harmonic setup was moved to a new location, was extended, and characterized. The modified setup can induce dynamics in gas phase samples with photon energies of 1.55eV, 3.10eV, and 4.65eV. The valence electronic structure of the samples can be probed with photon energies between 20eV and 40eV. The temporal resolution is 111fs to 262fs, depending on the combination of the two photon energies.
The electronically excited intermediates of the two complexes, as well as of the reaction product Fe(CO)₄, could be observed with photoelectron spectroscopy in the gas phase for the first time. However, photoelectron spectroscopy gives access only to the final ionic states. Corresponding calculations to simulate these spectra are still in development. The peak energies and their evolution in time with respect to the initiation pump pulse have been determined, these peaks have been assigned based on literature data. The spectra of the two complexes show clear differences. The dynamics have been interpreted with the assumption that the motion of peaks in the spectra relates to the movement of the wave packet in the multidimensional energy landscape. The results largely confirm existing models for the reaction pathways. In both metal carbonyls, this pathway involves a direct excitation of the wave packet to a metal-to-ligand charge transfer state and the subsequent crossing to a dissociative ligand field state. The coupling of the electronic dynamics to the nuclear dynamics could explain the slower dissociation in Fe(CO)₅ as compared to Cr(CO)₆.
The cell interior is a highly packed environment in which biological macromolecules evolve and function. This crowded media has effects in many biological processes such as protein-protein binding, gene regulation, and protein folding. Thus, biochemical reactions that take place in such crowded conditions differ from diluted test tube conditions, and a considerable effort has been invested in order to understand such differences.
In this work, we combine different computationally tools to disentangle the effects of molecular crowding on biochemical processes. First, we propose a lattice model to study the implications of molecular crowding on enzymatic reactions. We provide a detailed picture of how crowding affects binding and unbinding events and how the separate effects of crowding on binding equilibrium act together. Then, we implement a lattice model to study the effects of molecular crowding on facilitated diffusion. We find that obstacles on the DNA impair facilitated diffusion. However, the extent of this effect depends on how dynamic obstacles are on the DNA. For the scenario in which crowders are only present in the bulk solution, we find that at some conditions presence of crowding agents can enhance specific-DNA binding. Finally, we make use of structure-based techniques to look at the impact of the presence of crowders on the folding a protein. We find that polymeric crowders have stronger effects on protein stability than spherical crowders. The strength of this effect increases as the polymeric crowders become longer. The methods we propose here are general and can also be applied to more complicated systems.
The cytoskeleton is an essential component of living cells. It is composed of different types of protein filaments that form complex, dynamically rearranging, and interconnected networks. The cytoskeleton serves a multitude of cellular functions which further depend on the cell context. In animal cells, the cytoskeleton prominently shapes the cell's mechanical properties and movement. In plant cells, in contrast, the presence of a rigid cell wall as well as their larger sizes highlight the role of the cytoskeleton in long-distance intracellular transport. As it provides the basis for cell growth and biomass production, cytoskeletal transport in plant cells is of direct environmental and economical relevance. However, while knowledge about the molecular details of the cytoskeletal transport is growing rapidly, the organizational principles that shape these processes on a whole-cell level remain elusive.
This thesis is devoted to the following question: How does the complex architecture of the plant cytoskeleton relate to its transport functionality? The answer requires a systems level perspective of plant cytoskeletal structure and transport. To this end, I combined state-of-the-art confocal microscopy, quantitative digital image analysis, and mathematically powerful, intuitively accessible graph-theoretical approaches.
This thesis summarizes five of my publications that shed light on the plant cytoskeleton as a transportation network: (1) I developed network-based frameworks for accurate, automated quantification of cytoskeletal structures, applicable in, e.g., genetic or chemical screens; (2) I showed that the actin cytoskeleton displays properties of efficient transport networks, hinting at its biological design principles; (3) Using multi-objective optimization, I demonstrated that different plant cell types sustain cytoskeletal networks with cell-type specific and near-optimal organization; (4) By investigating actual transport of organelles through the cell, I showed that properties of the actin cytoskeleton are predictive of organelle flow and provided quantitative evidence for a coordination of transport at a cellular level; (5) I devised a robust, optimization-based method to identify individual cytoskeletal filaments from a given network representation, allowing the investigation of single filament properties in the network context. The developed methods were made publicly available as open-source software tools.
Altogether, my findings and proposed frameworks provide quantitative, system-level insights into intracellular transport in living cells. Despite my focus on the plant cytoskeleton, the established combination of experimental and theoretical approaches is readily applicable to different organisms. Despite the necessity of detailed molecular studies, only a complementary, systemic perspective, as presented here, enables both understanding of cytoskeletal function in its evolutionary context as well as its future technological control and utilization.
The high-latitudinal thermospheric processes driven by the solar wind and Interplanetary Magnetic Field (IMF) interaction with the Earth magnetosphere are highly variable parts of the complex dynamic plasma environment, which represent the coupled Magnetosphere – Ionosphere – Thermosphere (MIT) system. The solar wind and IMF interactions transfer energy to the MIT system via reconnection processes at the magnetopause. The Field Aligned Currents (FACs) constitute the energetic links between the magnetosphere and the Earth ionosphere. The MIT system depends on the highly variable solar wind conditions, in particular on changes of the strength and orientation of the IMF.
In my thesis, I perform an investigation on the physical background of the complex MIT system using the global physical - numerical, three-dimensional, time-dependent and self-consistent Upper Atmosphere Model (UAM). This model describes the thermosphere, ionosphere, plasmasphere and inner magnetosphere as well as the electrodynamics of the coupled MIT system for the altitudinal range from 80 (60) km up to the 15 Earth radii.
In the present study, I developed and investigated several variants of the high-latitudinal electrodynamic coupling by including the IMF dependence of FACs into the UAM model. For testing, the various variants were applied to simulations of the coupled MIT system for different seasons, geomagnetic activities, various solar wind and IMF conditions. Additionally, these variants of the theoretical model with the IMF dependence were compared with global empirical models. The modelling results for the most important thermospheric parameters like neutral wind and mass density were compared with satellite measurements. The variants of the UAM model with IMF dependence show a good agreement with the satellite observations. In comparison with the empirical models, the improved variants of the UAM model reproduce a more realistic meso-scale structures and dynamics of the coupled MIT system than the empirical models, in particular at high latitudes. The new configurations of the UAM model with IMF dependence contribute to the improvement of space weather prediction.
The gravitational field of a laser pulse of finite lifetime, is investigated in the framework of linearized gravity. Although the effects are very small, they may be of fundamental physical interest. It is shown that the gravitational field of a linearly polarized light pulse is modulated as the norm of the corresponding electric field strength, while no modulations arise for circular polarization. In general, the gravitational field is independent of the polarization direction. It is shown that all physical effects are confined to spherical shells expanding with the speed of light, and that these shells are imprints of the spacetime events representing emission and absorption of the pulse. Nearby test particles at rest are attracted towards the pulse trajectory by the gravitational field due to the emission of the pulse, and they are repelled from the pulse trajectory by the gravitational field due to its absorption. Examples are given for the size of the attractive effect. It is recovered that massless test particles do not experience any physical effect if they are co-propagating with the pulse, and that the acceleration of massless test particles counter-propagating with respect to the pulse is four times stronger than for massive particles
at rest. The similarities between the gravitational effect of a laser pulse and Newtonian gravity in two dimensions are pointed out. The spacetime curvature close to the pulse is compared to that induced by gravitational waves from astronomical sources.
The gravitational field of a laser pulse of finite lifetime, is investigated in the framework of linearized gravity. Although the effects are very small, they may be of fundamental physical interest. It is shown that the gravitational field of a linearly polarized light pulse is modulated as the norm of the corresponding electric field strength, while no modulations arise for circular polarization. In general, the gravitational field is independent of the polarization direction. It is shown that all physical effects are confined to spherical shells expanding with the speed of light, and that these shells are imprints of the spacetime events representing emission and absorption of the pulse. Nearby test particles at rest are attracted towards the pulse trajectory by the gravitational field due to the emission of the pulse, and they are repelled from the pulse trajectory by the gravitational field due to its absorption. Examples are given for the size of the attractive effect. It is recovered that massless test particles do not experience any physical effect if they are co-propagating with the pulse, and that the acceleration of massless test particles counter-propagating with respect to the pulse is four times stronger than for massive particles at rest. The similarities between the gravitational effect of a laser pulse and Newtonian gravity in two dimensions are pointed out. The spacetime curvature close to the pulse is compared to that induced by gravitational waves from astronomical sources.
Organic bulk heterojunction (BHJ) solar cells based on polymer:fullerene blends are a promising alternative for a low-cost solar energy conversion. Despite significant improvements of the power conversion efficiency in recent years, the fundamental working principles of these devices are yet not fully understood. In general, the current output of organic solar cells is determined by the generation of free charge carriers upon light absorption and their transport to the electrodes in competition to the loss of charge carriers due to recombination.
The object of this thesis is to provide a comprehensive understanding of the dynamic processes and physical parameters determining the performance. A new approach for analyzing the characteristic current-voltage output was developed comprising the experimental determination of the efficiencies of charge carrier generation, recombination and transport, combined with numerical device simulations.
Central issues at the beginning of this work were the influence of an electric field on the free carrier generation process and the contribution of generation, recombination and transport to the current-voltage characteristics. An elegant way to directly measure the field dependence of the free carrier generation is the Time Delayed Collection Field (TDCF) method. In TDCF charge carriers are generated by a short laser pulse and subsequently extracted by a defined rectangular voltage pulse. A new setup was established with an improved time resolution compared to former reports in literature. It was found that charge generation is in general independent of the electric field, in contrast to the current view in literature and opposed to the expectations of the Braun-Onsager model that was commonly used to describe the charge generation process. Even in cases where the charge generation was found to be field-dependend, numerical modelling showed that this field-dependence is in general not capable to account for the voltage dependence of the photocurrent. This highlights the importance of efficient charge extraction in competition to non-geminate recombination, which is the second objective of the thesis.
Therefore, two different techniques were combined to characterize the dynamics and efficiency of non-geminate recombination under device-relevant conditions. One new approach is to perform TDCF measurements with increasing delay between generation and extraction of charges. Thus, TDCF was used for the first time to measure charge carrier generation, recombination and transport with the same experimental setup. This excludes experimental errors due to different measurement and preparation conditions and demonstrates the strength of this technique. An analytic model for the description of TDCF transients was developed and revealed the experimental conditions for which reliable results can be obtained. In particular, it turned out that the $RC$ time of the setup which is mainly given by the sample geometry has a significant influence on the shape of the transients which has to be considered for correct data analysis.
Secondly, a complementary method was applied to characterize charge carrier recombination under steady state bias and illumination, i.e. under realistic operating conditions. This approach relies on the precise determination of the steady state carrier densities established in the active layer. It turned out that current techniques were not sufficient to measure carrier densities with the necessary accuracy. Therefore, a new technique {Bias Assisted Charge Extraction} (BACE) was developed. Here, the charge carriers photogenerated under steady state illumination are extracted by applying a high reverse bias. The accelerated extraction compared to conventional charge extraction minimizes losses through non-geminate recombination and trapping during extraction. By performing numerical device simulations under steady state, conditions were established under which quantitative information on the dynamics can be retrieved from BACE measurements.
The applied experimental techniques allowed to sensitively analyse and quantify geminate and non-geminate recombination losses along with charge transport in organic solar cells. A full analysis was exemplarily demonstrated for two prominent polymer-fullerene blends.
The model system P3HT:PCBM spincast from chloroform (as prepared) exhibits poor power conversion efficiencies (PCE) on the order of 0.5%, mainly caused by low fill factors (FF) and currents. It could be shown that the performance of these devices is limited by the hole transport and large bimolecular recombination (BMR) losses, while geminate recombination losses are insignificant. The low polymer crystallinity and poor interconnection between the polymer and fullerene domains leads to a hole mobility of the order of 10^-7 cm^2/Vs which is several orders of magnitude lower than the electron mobility in these devices. The concomitant build up of space charge hinders extraction of both electrons and holes and promotes bimolecular recombination losses.
Thermal annealing of P3HT:PCBM blends directly after spin coating improves crystallinity and interconnection of the polymer and the fullerene phase and results in comparatively high electron and hole mobilities in the order of 10^-3 cm^2/Vs and 10^-4 cm^2/Vs, respectively. In addition, a coarsening of the domain sizes leads to a reduction of the BMR by one order of magnitude. High charge carrier mobilities and low recombination losses result in comparatively high FF (>65%) and short circuit current (J_SC ≈ 10 mA/cm^2). The overall device performance (PCE ≈ 4%) is only limited by a rather low spectral overlap of absorption and solar emission and a small V_OC, given by the energetics of the P3HT.
From this point of view the combination of the low bandgap polymer PTB7 with PCBM is a promising approach. In BHJ solar cells, this polymer leads to a higher V_OC due to optimized energetics with PCBM. However, the J_SC in these (unoptimized) devices is similar to the J_SC in the optimized blend with P3HT and the FF is rather low (≈ 50%). It turned out that the unoptimized PTB7:PCBM blends suffer from high BMR, a low electron mobility of the order of 10^-5 cm^2/Vs and geminate recombination losses due to field dependent charge carrier generation.
The use of the solvent additive DIO optimizes the blend morphology, mainly by suppressing the formation of very large fullerene domains and by forming a more uniform structure of well interconnected donor and acceptor domains of the order of a few nanometers. Our analysis shows that this results in an increase of the electron mobility by about one order of magnitude (3 x 10^-4 cm^2/Vs), while BMR and geminate recombination losses are significantly reduced. In total these effects improve the J_SC (≈ 17 mA/cm^2) and the FF (> 70%). In 2012 this polymer/fullerene combination resulted in a record PCE for a single junction OSC of 9.2%.
Remarkably, the numerical device simulations revealed that the specific shape of the J-V characteristics depends very sensitively to the variation of not only one, but all dynamic parameters. On the one hand this proves that the experimentally determined parameters, if leading to a good match between simulated and measured J-V curves, are realistic and reliable. On the other hand it also emphasizes the importance to consider all involved dynamic quantities, namely charge carrier generation, geminate and non-geminate recombination as well as electron and hole mobilities. The measurement or investigation of only a subset of these parameters as frequently found in literature will lead to an incomplete picture and possibly to misleading conclusions.
Importantly, the comparison of the numerical device simulation employing the measured parameters and the experimental $J-V$ characteristics allows to identify loss channels and limitations of OSC. For example, it turned out that inefficient extraction of charge carriers is a criticical limitation factor that is often disobeyed. However, efficient and fast transport of charges becomes more and more important with the development of new low bandgap materials with very high internal quantum efficiencies. Likewise, due to moderate charge carrier mobilities, the active layer thicknesses of current high-performance devices are usually limited to around 100 nm. However, larger layer thicknesses would be more favourable with respect to higher current output and robustness of production. Newly designed donor materials should therefore at best show a high tendency to form crystalline structures, as observed in P3HT, combined with the optimized energetics and quantum efficiency of, for example, PTB7.
The subject of the present thesis is the one-dimensional Bose gas. Since long-rang order is destroyed by infra-red fluctuations in one dimension, only the formation of a quasi-condensate is possible, which exhibits suppressed density fluctuations, but whose phase fluctuates strongly. It is shown that modified mean-field theories based on a symmetry-breaking approach can even characterise phase coherence properties of such a quasi-condensate properly. A correct description of the transition from the degenerate ideal Bose gas to the quasi-condensate, which is a smooth cross-over rather than a phase transition, is not possible though. Basic conditions for the applicability of the theories are not fulfilled in this regime, such that the existence of a critical point is predicted.
The theories are compared on the basis of their excitation sprectum, equation of state, density fluctuations and related correlation functions. High-temperature expansions of the corresponding integrals are derived analytically for the numerical evaluation of the self-consistent integral equations. Apart from that, the Stochastic Gross-Pitaevskii equation (SGPE), a non-linear Langevin equation, is analysed numerically by means of Monte-Carlo simulations and the results are compared to those of the mean-field theories. In this context, a lot of attention is payed to the appropriate choice of the parameters. The simulations prove that the SGPE is capable of describing the cross-over properly, but highlight the limitations of the widely used local density approximation as well.
Many chemical reactions in biological cells occur at very low concentrations of constituent molecules. Thus, transcriptional gene-regulation is often controlled by poorly expressed transcription-factors, such as E.coli lac repressor with few tens of copies. Here we study the effects of inherent concentration fluctuations of substrate-molecules on the seminal Michaelis-Menten scheme of biochemical reactions. We present a universal correction to the Michaelis-Menten equation for the reaction-rates. The relevance and validity of this correction for enzymatic reactions and intracellular gene-regulation is demonstrated. Our analytical theory and simulation results confirm that the proposed variance-corrected Michaelis-Menten equation predicts the rate of reactions with remarkable accuracy even in the presence of large non-equilibrium concentration fluctuations. The major advantage of our approach is that it involves only the mean and variance of the substrate-molecule concentration. Our theory is therefore accessible to experiments and not specific to the exact source of the concentration fluctuations.
The non-linear behaviour of the atmospheric dynamics is not well understood and makes the evaluation and usage of regional climate models (RCMs) difficult. Due to these non-linearities, chaos and internal variability (IV) within the RCMs are induced, leading to a sensitivity of RCMs to their initial conditions (IC). The IV is the ability of RCMs to realise different solutions of simulations that differ in their IC, but have the same lower and lateral boundary conditions (LBC), hence can be defined as the across-member spread between the ensemble members.
For the investigation of the IV and the dynamical and diabatic contributions generating the IV four ensembles of RCM simulations are performed with the atmospheric regional model HIRHAM5. The integration area is the Arctic and each ensemble consists of 20 members. The ensembles cover the time period from July to September for the years 2006, 2007, 2009 and 2012. The ensemble members have the same LBC and differ in their IC only. The different IC are arranged by an initialisation time that shifts successively by six hours. Within each ensemble the first simulation starts on 1st July at 00 UTC and the last simulation starts on 5th July at 18 UTC and each simulation runs until 30th September. The analysed time period ranges from 6th July to 30th September, the time period that is covered by all ensemble members. The model runs without any nudging to allow a free development of each simulation to get the full internal variability within the HIRHAM5.
As a measure of the model generated IV, the across-member standard deviation and the across-member variance is used and the dynamical and diabatic processes influencing the IV are estimated by applying a diagnostic budget study for the IV tendency of the potential temperature developed by Nikiema and Laprise [2010] and Nikiema and Laprise [2011]. The diagnostic budget study is based on the first law of thermodynamics for potential temperature and the mass-continuity equation. The resulting budget equation reveals seven contributions to the potential temperature IV tendency.
As a first study, this work analyses the IV within the HIRHAM5. Therefore, atmospheric circulation parameters and the potential temperature for all four ensemble years are investigated. Similar to previous studies, the IV fluctuates strongly in time. Further, due to the fact that all ensemble members are forced with the same LBC, the IV depends on the vertical level within the troposphere, with high values in the lower troposphere and at 500 hPa and low values in the upper troposphere and at the surface. By the same reason, the spatial distribution shows low values of IV at the boundaries of the model domain.
The diagnostic budget study for the IV tendency of potential temperature reveals that the seven contributions fluctuate in time like the IV. However, the individual terms reach different absolute magnitudes. The budget study identifies the horizontal and vertical ‘baroclinic’ terms as the main contributors to the IV tendency, with the horizontal ‘baroclinic’ term producing and the vertical ‘baroclinic’ term reducing the IV. The other terms fluctuate around zero, because they are small in general or are balanced due to the domain average.
The comparison of the results obtained for the four different ensembles (summers 2006, 2007, 2009 and 2012) reveals that on average the findings for each ensemble are quite similar concerning the magnitude and the general pattern of IV and its contributions. However, near the surface a weaker IV is produced with decreasing sea ice extent. This is caused by a smaller impact of the horizontal 'baroclinic' term over some regions and by the changing diabatic processes, particularly a more intense reducing tendency of the IV due to condensative heating. However, it has to be emphasised that the behaviour of the IV and its dynamical and diabatic contributions are influenced mainly by complex atmospheric feedbacks and large-scale processes and not by the sea ice distribution.
Additionally, a comparison with a second RCM covering the Arctic and using the same LBCs and IC is performed. For both models very similar results concerning the IV and its dynamical and diabatic contributions are found. Hence, this investigation leads to the conclusion that the IV is a natural phenomenon and is independent from the applied RCM.
The main goal of this cumulative thesis is the derivation of surface emissivity data in the infrared from radiance measurements of Venus. Since these data are diagnostic of the chemical composition and grain size of the surface material, they can help to improve knowledge of the planet’s geology. Spectrally resolved images of nightside emissions in the range 1.0-5.1 μm were recently acquired by the InfraRed Mapping channel of the Visible and InfraRed Thermal Imaging Spectrometer (VIRTIS-M-IR) aboard ESA’s Venus EXpress (VEX). Surface and deep atmospheric thermal emissions in this spectral range are strongly obscured by the extremely opaque atmosphere, but three narrow spectral windows at 1.02, 1.10, and 1.18 μm allow the sounding of the surface. Additional windows between 1.3 and 2.6 μm provide information on atmospheric parameters that is required to interpret the surface signals. Quantitative data on surface and atmosphere can be retrieved from the measured spectra by comparing them to simulated spectra. A numerical radiative transfer model is used in this work to simulate the observable radiation as a function of atmospheric, surface, and instrumental parameters. It is a line-by-line model taking into account thermal emissions by surface and atmosphere as well as absorption and multiple scattering by gases and clouds. The VIRTIS-M-IR measurements are first preprocessed to obtain an optimal data basis for the subsequent steps. In this process, a detailed detector responsivity analysis enables the optimization of the data consistency. The measurement data have a relatively low spectral information content, and different parameter vectors can describe the same measured spectrum equally well. A usual method to regularize the retrieval of the wanted parameters from a measured spectrum is to take into account a priori mean values and standard deviations of the parameters to be retrieved. This decreases the probability to obtain unreasonable parameter values. The multi-spectrum retrieval algorithm MSR is developed to additionally consider physically realistic spatial and temporal a priori correlations between retrieval parameters describing different measurements. Neglecting geologic activity, MSR also allows the retrieval of an emissivity map as a parameter vector that is common to several spectrally resolved images that cover the same surface target. Even applying MSR, it is difficult to obtain reliable emissivity maps in absolute values. A detailed retrieval error analysis based on synthetic spectra reveals that this is mainly due to interferences from parameters that cannot be derived from the spectra themselves, but that have to be set to assumed values to enable the radiative transfer simulations. The MSR retrieval of emissivity maps relative to a fixed emissivity is shown to effectively avoid most emissivity retrieval errors. Relative emissivity maps at 1.02, 1.10, and 1.18 μm are finally derived from many VIRTIS-M-IR measurements that cover a surface target at Themis Regio. They are interpreted as spatial variations relative to an assumed emissivity mean of the target. It is verified that the maps are largely independent of the choice of many interfering parameters as well as the utilized measurement data set. These are the first Venus IR emissivity data maps based on a consistent application of a full radiative transfer simulation and a retrieval algorithm that respects a priori information. The maps are sufficiently reliable for future geologic interpretations.
This thesis investigates the application of polyelectrolyte multilayers in plasmonics and picosecond acoustics. The observed samples were fabricated by the spin-assisted layer-by-layer deposition technique that allowed a precise tuning of layer thickness in the range of few nanometers.
The first field of interest deals with the interaction of light-induced localized surface plasmons (LSP) of rod-shaped gold nanoparticles with the particles' environment. The environment consists of an air phase and a phase of polyelectrolytes, whose ratio affects the spectral position of the LSP resonance.
Measured UV-VIS spectra showed the shift of the LSP absorption peak as a function of the cover layer thickness of the particles. The data are modeled using an average dielectric function instead of the dielectric functions of air and polyelectrolytes. In addition using a measured dielectric function of the gold nanoparticles, the position of the LSP absorption peak could be simulated with good agreement to the data.
The analytic model helps to understand the optical properties of metal nanoparticles in an inhomogeneous environment.
The second part of this work discusses the applicability of PAzo/PAH and dye-doped PSS/PAH polyelectrolyte multilayers as transducers to generate hypersound pulses. The generated strain pulses were detected by time-domain Brillouin scattering (TDBS) using a pump-probe laser setup. Transducer layers made of polyelectrolytes were compared qualitatively to common aluminum transducers in terms of measured TDBS signal amplitude, degradation due to laser excitation, and sample preparation.
The measurements proved that fast and easy prepared polyelectrolyte transducers provided stronger TDBS signals than the aluminum transducer. AFM topography measurements showed a degradation of the polyelectrolyte structures, especially for the PAzo/PAH sample.
To quantify the induced strain, optical barriers were introduced to separate the transducer material from the medium of the hypersound propagation. Difficulties in the sample preparation prohibited a reliable quantification. But the experiments showed that a coating with transparent polyelectrolytes increases the efficiency of aluminum transducers and modifies the excited phonon distribution.
The adoption of polyelectrolytes to the scientific field of picosecond acoustics enables a cheap and fast fabrication of transducer layers on most surfaces. In contrast to aluminum layers the polyelectrolytes are transparent over a wide spectral range. Thus, the strain modulation can be probed from surface and back.
Temperature-memory polymers remember the temperature, where they were deformed recently, enabled by broad thermal transitions. In this study, we explored a series of crosslinked poly[ethylene-co-(vinyl acetate)] networks (cPEVAs) comprising crystallizable polyethylene (PE) controlling units exhibiting a pronounced temperature-memory effect (TME) between 16 and 99 °C related to a broad melting transition (∼100 °C). The nanostructural changes in such cPEVAs during programming and activation of the TME were analyzed via in situ X-ray scattering and specific annealing experiments. Different contributions to the mechanism of memorizing high or low deformation temperatures (Tdeform) were observed in cPEVA, which can be associated to the average PE crystal sizes. At high deformation temperatures (>50 °C), newly formed PE crystals, which are established during cooling when fixing the temporary shape, dominated the TME mechanism. In contrast, at low Tdeform (<50 °C), corresponding to a cold drawing scenario, the deformation led preferably to a disruption of existing large crystals into smaller ones, which then fix the temporary shape upon cooling. The observed mechanism of memorizing a deformation temperature might enable the prediction of the TME behavior and the knowledge based design of other TMPs with crystallizable controlling units.
Temperature-memory polymers remember the temperature, where they were deformed recently, enabled by broad thermal transitions. In this study, we explored a series of crosslinked poly[ethylene-co-(vinyl acetate)] networks (cPEVAs) comprising crystallizable polyethylene (PE) controlling units exhibiting a pronounced temperature-memory effect (TME) between 16 and 99 °C related to a broad melting transition (∼100 °C). The nanostructural changes in such cPEVAs during programming and activation of the TME were analyzed via in situ X-ray scattering and specific annealing experiments. Different contributions to the mechanism of memorizing high or low deformation temperatures (Tdeform) were observed in cPEVA, which can be associated to the average PE crystal sizes. At high deformation temperatures (>50 °C), newly formed PE crystals, which are established during cooling when fixing the temporary shape, dominated the TME mechanism. In contrast, at low Tdeform (<50 °C), corresponding to a cold drawing scenario, the deformation led preferably to a disruption of existing large crystals into smaller ones, which then fix the temporary shape upon cooling. The observed mechanism of memorizing a deformation temperature might enable the prediction of the TME behavior and the knowledge based design of other TMPs with crystallizable controlling units.
Function by structure
(2015)
Synchronization of large ensembles of oscillators is an omnipresent phenomenon observed in different fields of science like physics, engineering, life sciences, etc. The most simple setup is that of globally coupled phase oscillators, where all the oscillators contribute to a global field which acts on all oscillators. This formulation of the problem was pioneered by Winfree and Kuramoto. Such a setup gives a possibility for the analysis of these systems in terms of global variables. In this work we describe nontrivial collective dynamics in oscillator populations coupled via mean fields in terms of global variables. We consider problems which cannot be directly reduced to standard Kuramoto and Winfree models.
In the first part of the thesis we adopt a method introduced by Watanabe and Strogatz. The main idea is that the system of identical oscillators of particular type can be described by a low-dimensional system of global equations. This approach enables us to perform a complete analytical analysis for a special but vast set of initial conditions. Furthermore, we show how the approach can be expanded for some nonidentical systems. We apply the Watanabe-Strogatz approach to arrays of Josephson junctions and systems of identical phase oscillators with leader-type coupling.
In the next parts of the thesis we consider the self-consistent mean-field theory method that can be applied to general nonidentical globally coupled systems of oscillators both with or without noise. For considered systems a regime, where the global field rotates uniformly, is the most important one. With the help of this approach such solutions of the self-consistency equation for an arbitrary distribution of frequencies and coupling parameters can be found analytically in the parametric form, both for noise-free and noisy cases.
We apply this method to deterministic Kuramoto-type model with generic coupling and an ensemble of spatially distributed oscillators with leader-type coupling. Furthermore, with the proposed self-consistent approach we fully characterize rotating wave solutions of noisy Kuramoto-type model with generic coupling and an ensemble of noisy oscillators with bi-harmonic coupling.
Whenever possible, a complete analysis of global dynamics is performed and compared with direct numerical simulations of large populations.
Recent experiments show that transcription factors (TFs) indeed use the facilitated diffusion mechanism to locate their target sequences on DNA in living bacteria cells: TFs alternate between sliding motion along DNA and relocation events through the cytoplasm. From simulations and theoretical analysis we study the TF-sliding motion for a large section of the DNA-sequence of a common E. coli strain, based on the two-state TF-model with a fast-sliding search state and a recognition state enabling target detection. For the probability to detect the target before dissociating from DNA the TF-search times self-consistently depend heavily on whether or not an auxiliary operator (an accessible sequence similar to the main operator) is present in the genome section. Importantly, within our model the extent to which the interconversion rates between search and recognition states depend on the underlying nucleotide sequence is varied. A moderate dependence maximises the capability to distinguish between the main operator and similar sequences. Moreover, these auxiliary operators serve as starting points for DNA looping with the main operator, yielding a spectrum of target detection times spanning several orders of magnitude. Auxiliary operators are shown to act as funnels facilitating target detection by TFs.
Stochastic Wilson
(2015)
We consider a simple Markovian class of the stochastic Wilson–Cowan type models of neuronal network dynamics, which incorporates stochastic delay caused by the existence of a refractory period of neurons. From the point of view of the dynamics of the individual elements, we are dealing with a network of non-Markovian stochastic two-state oscillators with memory, which are coupled globally in a mean-field fashion. This interrelation of a higher-dimensional Markovian and lower-dimensional non-Markovian dynamics is discussed in its relevance to the general problem of the network dynamics of complex elements possessing memory. The simplest model of this class is provided by a three-state Markovian neuron with one refractory state, which causes firing delay with an exponentially decaying memory within the two-state reduced model. This basic model is used to study critical avalanche dynamics (the noise sustained criticality) in a balanced feedforward network consisting of the excitatory and inhibitory neurons. Such avalanches emerge due to the network size dependent noise (mesoscopic noise). Numerical simulations reveal an intermediate power law in the distribution of avalanche sizes with the critical exponent around −1.16. We show that this power law is robust upon a variation of the refractory time over several orders of magnitude. However, the avalanche time distribution is biexponential. It does not reflect any genuine power law dependence.
We define and study in detail utraslow scaled Brownian motion (USBM) characterized by a time dependent diffusion coefficient of the form . For unconfined motion the mean squared displacement (MSD) of USBM exhibits an ultraslow, logarithmic growth as function of time, in contrast to the conventional scaled Brownian motion. In a harmonic potential the MSD of USBM does not saturate but asymptotically decays inverse-proportionally to time, reflecting the highly non-stationary character of the process. We show that the process is weakly non-ergodic in the sense that the time averaged MSD does not converge to the regular MSD even at long times, and for unconfined motion combines a linear lag time dependence with a logarithmic term. The weakly non-ergodic behaviour is quantified in terms of the ergodicity breaking parameter. The USBM process is also shown to be ageing: observables of the system depend on the time gap between initiation of the test particle and start of the measurement of its motion. Our analytical results are shown to agree excellently with extensive computer simulations.
Recent experiments show that transcription factors (TFs) indeed use the facilitated diffusion mechanism to locate their target sequences on DNA in living bacteria cells: TFs alternate between sliding motion along DNA and relocation events through the cytoplasm. From simulations and theoretical analysis we study the TF-sliding motion for a large section of the DNA-sequence of a common E. coli strain, based on the two-state TF-model with a fast-sliding search state and a recognition state enabling target detection. For the probability to detect the target before dissociating from DNA the TF-search times self-consistently depend heavily on whether or not an auxiliary operator (an accessible sequence similar to the main operator) is present in the genome section. Importantly, within our model the extent to which the interconversion rates between search and recognition states depend on the underlying nucleotide sequence is varied. A moderate dependence maximises the capability to distinguish between the main operator and similar sequences. Moreover, these auxiliary operators serve as starting points for DNA looping with the main operator, yielding a spectrum of target detection times spanning several orders of magnitude. Auxiliary operators are shown to act as funnels facilitating target detection by TFs.
We define and study in detail utraslow scaled Brownian motion (USBM) characterized by a time dependent diffusion coefficient of the form . For unconfined motion the mean squared displacement (MSD) of USBM exhibits an ultraslow, logarithmic growth as function of time, in contrast to the conventional scaled Brownian motion. In a harmonic potential the MSD of USBM does not saturate but asymptotically decays inverse-proportionally to time, reflecting the highly non-stationary character of the process. We show that the process is weakly non-ergodic in the sense that the time averaged MSD does not converge to the regular MSD even at long times, and for unconfined motion combines a linear lag time dependence with a logarithmic term. The weakly non-ergodic behaviour is quantified in terms of the ergodicity breaking parameter. The USBM process is also shown to be ageing: observables of the system depend on the time gap between initiation of the test particle and start of the measurement of its motion. Our analytical results are shown to agree excellently with extensive computer simulations.
Atmospheric interactions with land surface in the arctic based on regional climate model solutions
(2014)
Scientific inquiry requires that we formulate not only what we know, but also what we do not know and by how much. In climate data analysis, this involves an accurate specification of measured quantities and a consequent analysis that consciously propagates the measurement errors at each step. The dissertation presents a thorough analytical method to quantify errors of measurement inherent in paleoclimate data. An additional focus are the uncertainties in assessing the coupling between different factors that influence the global mean temperature (GMT).
Paleoclimate studies critically rely on `proxy variables' that record climatic signals in natural archives. However, such proxy records inherently involve uncertainties in determining the age of the signal. We present a generic Bayesian approach to analytically determine the proxy record along with its associated uncertainty, resulting in a time-ordered sequence of correlated probability distributions rather than a precise time series. We further develop a recurrence based method to detect dynamical events from the proxy probability distributions. The methods are validated with synthetic examples and
demonstrated with real-world proxy records. The proxy estimation step reveals the interrelations between proxy variability and uncertainty. The recurrence analysis of the East Asian Summer Monsoon during the last 9000 years confirms the well-known `dry' events at 8200 and 4400 BP, plus an additional significantly dry event at 6900 BP.
We also analyze the network of dependencies surrounding GMT. We find an intricate, directed network with multiple links between the different factors at multiple time delays. We further uncover a significant feedback from the GMT to the El Niño Southern Oscillation at quasi-biennial timescales. The analysis highlights the need of a more nuanced formulation of influences between different climatic factors, as well as the limitations in trying to estimate such dependencies.
In this thesis, I study ultrafast dynamics in perovskite oxides using time resolved broadband spectroscopy. I focus on the observation of coherent phonon propagation by time resolved Brillouin scattering: following the excition of metal transducer films with a femtosecond infrared pump pulse, coherent phonon dynamics in the GHz frequency range are triggered. Their propagation is monitored using a delayed white light probe pulse. The technique is illustrated on various thin films and multilayered samples. I apply the technique to investigate the linear and nonlinear acoustic response in bulk SrTiO_3, which displays a ferroelastic phase transition from a cubic to a tetragonal structural phase at T_a=105 K. In the linear regime, I observe a coupling of the observed acoustic phonon mode to the softening optic modes describing the phase transition. In the nonlinear regime, I find a giant slowing down of the sound velocity in the low temperature phase that is only observable for a strain amplitude exceeding the tetragonality of the material. It is attributed to a coupling of the high frequency phonons to ferroelastic domain walls in the material. I propose a new mechanism for the coupling of strain waves to the domain walls that is only effective for high amplitude strain. A detailed study of the phonon attenuation across a wide temperature range shows that the phonon attenuation at low temperatures is influenced by the domain configuration, which is determined by interface strain. Preliminary measurements on magnetic-ferroelectric multilayers reveal that the excitation fluence needs to be carefully controlled when dynamics at phase transitions are studied.
Untersuchungen zur pro-inflammatorischen Wirkung von Serum-Amyloid A in glatten Gefäßmuskelzellen
(2014)
Stochastic Wilson
(2015)
We consider a simple Markovian class of the stochastic Wilson–Cowan type models of neuronal network dynamics, which incorporates stochastic delay caused by the existence of a refractory period of neurons. From the point of view of the dynamics of the individual elements, we are dealing with a network of non-Markovian stochastic two-state oscillators with memory, which are coupled globally in a mean-field fashion. This interrelation of a higher-dimensional Markovian and lower-dimensional non-Markovian dynamics is discussed in its relevance to the general problem of the network dynamics of complex elements possessing memory. The simplest model of this class is provided by a three-state Markovian neuron with one refractory state, which causes firing delay with an exponentially decaying memory within the two-state reduced model. This basic model is used to study critical avalanche dynamics (the noise sustained criticality) in a balanced feedforward network consisting of the excitatory and inhibitory neurons. Such avalanches emerge due to the network size dependent noise (mesoscopic noise). Numerical simulations reveal an intermediate power law in the distribution of avalanche sizes with the critical exponent around −1.16. We show that this power law is robust upon a variation of the refractory time over several orders of magnitude. However, the avalanche time distribution is biexponential. It does not reflect any genuine power law dependence.
Molecular motors pulling cargos in the viscoelastic cytosol: how power strokes beat subdiffusion
(2014)
The discovery of anomalous diffusion of larger biopolymers and submicron tracers such as endogenous granules, organelles, or virus capsids in living cells, attributed to the viscoelastic nature of the cytoplasm, provokes the question whether this complex environment equally impacts the active intracellular transport of submicron cargos by molecular motors such as kinesins: does the passive anomalous diffusion of free cargo always imply its anomalously slow active transport by motors, the mean transport distance along microtubule growing sublinearly rather than linearly in time? Here we analyze this question within the widely used two-state Brownian ratchet model of kinesin motors based on the continuous-state diffusion along microtubules driven by a flashing binding potential, where the cargo particle is elastically attached to the motor. Depending on the cargo size, the loading force, the amplitude of the binding potential, the turnover frequency of the molecular motor enzyme, and the linker stiffness we demonstrate that the motor transport may turn out either normal or anomalous, as indeed measured experimentally. We show how a highly efficient normal active transport mediated by motors may emerge despite the passive anomalous diffusion of the cargo, and study the intricate effects of the elastic linker. Under different, well specified conditions the microtubule-based motor transport becomes anomalously slow and thus significantly less efficient.
Molecular motors pulling cargos in the viscoelastic cytosol: how power strokes beat subdiffusion
(2014)
The discovery of anomalous diffusion of larger biopolymers and submicron tracers such as endogenous granules, organelles, or virus capsids in living cells, attributed to the viscoelastic nature of the cytoplasm, provokes the question whether this complex environment equally impacts the active intracellular transport of submicron cargos by molecular motors such as kinesins: does the passive anomalous diffusion of free cargo always imply its anomalously slow active transport by motors, the mean transport distance along microtubule growing sublinearly rather than linearly in time? Here we analyze this question within the widely used two-state Brownian ratchet model of kinesin motors based on the continuous-state diffusion along microtubules driven by a flashing binding potential, where the cargo particle is elastically attached to the motor. Depending on the cargo size, the loading force, the amplitude of the binding potential, the turnover frequency of the molecular motor enzyme, and the linker stiffness we demonstrate that the motor transport may turn out either normal or anomalous, as indeed measured experimentally. We show how a highly efficient normal active transport mediated by motors may emerge despite the passive anomalous diffusion of the cargo, and study the intricate effects of the elastic linker. Under different, well specified conditions the microtubule-based motor transport becomes anomalously slow and thus significantly less efficient.
Anomalous diffusion is frequently described by scaled Brownian motion (SBM){,} a Gaussian process with a power-law time dependent diffusion coefficient. Its mean squared displacement is ?x2(t)? [similar{,} equals] 2K(t)t with K(t) [similar{,} equals] t[small alpha]-1 for 0 < [small alpha] < 2. SBM may provide a seemingly adequate description in the case of unbounded diffusion{,} for which its probability density function coincides with that of fractional Brownian motion. Here we show that free SBM is weakly non-ergodic but does not exhibit a significant amplitude scatter of the time averaged mean squared displacement. More severely{,} we demonstrate that under confinement{,} the dynamics encoded by SBM is fundamentally different from both fractional Brownian motion and continuous time random walks. SBM is highly non-stationary and cannot provide a physical description for particles in a thermalised stationary system. Our findings have direct impact on the modelling of single particle tracking experiments{,} in particular{,} under confinement inside cellular compartments or when optical tweezers tracking methods are used.
Anomalous diffusion is frequently described by scaled Brownian motion (SBM){,} a Gaussian process with a power-law time dependent diffusion coefficient. Its mean squared displacement is ?x2(t)? [similar{,} equals] 2K(t)t with K(t) [similar{,} equals] t[small alpha]-1 for 0 < [small alpha] < 2. SBM may provide a seemingly adequate description in the case of unbounded diffusion{,} for which its probability density function coincides with that of fractional Brownian motion. Here we show that free SBM is weakly non-ergodic but does not exhibit a significant amplitude scatter of the time averaged mean squared displacement. More severely{,} we demonstrate that under confinement{,} the dynamics encoded by SBM is fundamentally different from both fractional Brownian motion and continuous time random walks. SBM is highly non-stationary and cannot provide a physical description for particles in a thermalised stationary system. Our findings have direct impact on the modelling of single particle tracking experiments{,} in particular{,} under confinement inside cellular compartments or when optical tweezers tracking methods are used.
Probably no other field of statistical physics at the borderline of soft matter and biological physics has caused such a flurry of papers as polymer translocation since the 1994 landmark paper by Bezrukov, Vodyanoy, and Parsegian and the study of Kasianowicz in 1996. Experiments, simulations, and theoretical approaches are still contributing novel insights to date, while no universal consensus on the statistical understanding of polymer translocation has been reached. We here collect the published results, in particular, the famous–infamous debate on the scaling exponents governing the translocation process. We put these results into perspective and discuss where the field is going. In particular, we argue that the phenomenon of polymer translocation is non-universal and highly sensitive to the exact specifications of the models and experiments used towards its analysis.
Probably no other field of statistical physics at the borderline of soft matter and biological physics has caused such a flurry of papers as polymer translocation since the 1994 landmark paper by Bezrukov, Vodyanoy, and Parsegian and the study of Kasianowicz in 1996. Experiments, simulations, and theoretical approaches are still contributing novel insights to date, while no universal consensus on the statistical understanding of polymer translocation has been reached. We here collect the published results, in particular, the famous–infamous debate on the scaling exponents governing the translocation process. We put these results into perspective and discuss where the field is going. In particular, we argue that the phenomenon of polymer translocation is non-universal and highly sensitive to the exact specifications of the models and experiments used towards its analysis.
Diffusion of finite-size particles in two-dimensional channels with random wall configurations
(2014)
Diffusion of chemicals or tracer molecules through complex systems containing irregularly shaped channels is important in many applications. Most theoretical studies based on the famed Fick–Jacobs equation focus on the idealised case of infinitely small particles and reflecting boundaries. In this study we use numerical simulations to consider the transport of finite-size particles through asymmetrical two-dimensional channels. Additionally, we examine transient binding of the molecules to the channel walls by applying sticky boundary conditions. We consider an ensemble of particles diffusing in independent channels, which are characterised by common structural parameters. We compare our results for the long-time effective diffusion coefficient with a recent theoretical formula obtained by Dagdug and Pineda [J. Chem. Phys., 2012, 137, 024107].
Diffusion of finite-size particles in two-dimensional channels with random wall configurations
(2014)
Diffusion of chemicals or tracer molecules through complex systems containing irregularly shaped channels is important in many applications. Most theoretical studies based on the famed Fick–Jacobs equation focus on the idealised case of infinitely small particles and reflecting boundaries. In this study we use numerical simulations to consider the transport of finite-size particles through asymmetrical two-dimensional channels. Additionally, we examine transient binding of the molecules to the channel walls by applying sticky boundary conditions. We consider an ensemble of particles diffusing in independent channels, which are characterised by common structural parameters. We compare our results for the long-time effective diffusion coefficient with a recent theoretical formula obtained by Dagdug and Pineda [J. Chem. Phys., 2012, 137, 024107].
The atmosphere over the Arctic Ocean is strongly influenced by the distribution of sea ice and open water. Leads in the sea ice produce strong convective fluxes of sensible and latent heat and release aerosol particles into the atmosphere. They increase the occurrence of clouds and modify the structure and characteristics of the atmospheric boundary layer (ABL) and thereby influence the Arctic climate.
In the course of this study aircraft measurements were performed over the western Arctic Ocean as part of the campaign PAMARCMIP 2012 of the Alfred Wegener Institute for Polar and Marine Research (AWI). Backscatter from aerosols and clouds within the lower troposphere and the ABL were measured with the nadir pointing Airborne Mobile Aerosol Lidar (AMALi) and dropsondes were launched to obtain profiles of meteorological variables. Furthermore, in situ measurements of aerosol properties, meteorological variables and turbulence were part of the campaign. The measurements covered a broad range of atmospheric and sea ice conditions.
In this thesis, properties of the ABL over Arctic sea ice with a focus on the influence of open leads are studied based on the data from the PAMARCMIP campaign. The height of the ABL is determined by different methods that are applied to dropsonde and AMALi backscatter profiles. ABL heights are compared for different flights representing different conditions of the atmosphere and of sea ice and open water influence. The different criteria for ABL height that are applied show large variation in terms of agreement among each other, depending on the characteristics of the ABL and its history. It is shown that ABL height determination from lidar backscatter by methods commonly used under mid-latitude conditions is applicable to the Arctic ABL only under certain conditions. Aerosol or clouds within the ABL are needed as a tracer for ABL height detection from backscatter. Hence an aerosol source close to the surface is necessary, that is typically found under the present influence of open water and therefore convective conditions. However it is not always possible to distinguish residual layers from the actual ABL. Stable boundary layers are generally difficult to detect.
To illustrate the complexity of the Arctic ABL and processes therein, four case studies are analyzed each of which represents a snapshot of the interplay between atmosphere and underlying sea ice or water surface. Influences of leads and open water on the aerosol and clouds within the ABL are identified and discussed. Leads are observed to cause the formation of fog and cloud layers within the ABL by humidity emission. Furthermore they decrease the stability and increase the height of the ABL and consequently facilitate entrainment of air and aerosol layers from the free troposphere.
For the calculation of the work in an irreversible pressure-volume change, we propose approxima-tions, which in contrast to the usual representation in the literature reflect the work performed during expansion and compression symmetrically. The calculations are based on the Reversible-Share-Theorem: Is used the force to overcome for calculating the work, so it captures only the configurational reversible work share.
During this work I built a four wave mixing setup for the time-resolved femtosecond spectroscopy of Raman-active lattice modes. This setup enables to study the selective excitation of phonon polaritons. These quasi-particles arise from the coupling of electro-magnetic waves and transverse optical lattice modes, the so-called phonons. The phonon polaritons were investigated in the optically non-linear, ferroelectric crystals LiNbO₃ and LiTaO₃.
The direct observation of the frequency shift of the scattered narrow bandwidth probe pulses proofs the role of the Raman interaction during the probe and excitation process of phonon polaritons. I compare this experimental method with the measurement where ultra-short laser pulses are used. The frequency shift remains obscured by the relative broad bandwidth of these laser pulses. In an experiment with narrow bandwidth probe pulses, the Stokes and anti-Stokes intensities are spectrally separated. They are assigned to the corresponding counter-propagating wavepackets of phonon polaritons. Thus, the dynamics of these wavepackets was separately studied. Based on these findings, I develop the mathematical description of the so-called homodyne detection of light for the case of light scattering from counter propagating phonon polaritons.
Further, I modified the broad bandwidth of the ultra-short pump pulses using bandpass filters to generate two pump pulses with non-overlapping spectra. This enables the frequency-selective excitation of polariton modes in the sample, which allows me to observe even very weak polariton modes in LiNbO₃ or LiTaO₃ that belong to the higher branches of the dispersion relation of phonon polaritons. The experimentally determined dispersion relation of the phonon polaritons could therefore be extended and compared to theoretical models. In addition, I determined the frequency-dependent damping of phonon polaritons.
The origin of cosmic rays was the subject of several studies for over a century. The investigations done within this dissertation are one small step to shed some more light on this mystery.
Locating the sources of cosmic rays is not trivial due to the interstellar magnetic field. However, the Hillas criterion allows us to arrive at the conclusion that supernova remnants are our main suspect for the origin of galactic cosmic rays. The mechanism by which they are accelerating particles is found within the field of shock physics as diffusive shock acceleration. To allow particles to enter this process also known as Fermi acceleration pre-acceleration processes like shock surfing acceleration and shock drift acceleration are necessary. Investigating the processes happening in the plasma shocks of supernova remnants is possible by utilising a simplified model which can be simulated on a computer using Particle-in-Cell simulations.
We developed a new and clean setup to simulate the formation of a double shock, i.e., consisting of a forward and a reverse shock and a contact discontinuity, by the collision of two counter-streaming plasmas, in which a magnetic field can be woven into. In a previous work, we investigated the processes at unmagnetised and at magnetised parallel shocks, whereas in the current work, we move our investigation on to magnetised perpendicular shocks.
Due to a much stronger confinement of the particles to the collision region the perpendicular shock develops much faster than the parallel shock. On the other hand, this leads to much weaker turbulence. We are able to find indications for shock surfing acceleration and shock drift acceleration happening at the two shocks leading to populations of pre-accelerated particles that are suitable as a seed population to be injected into further diffusive shock acceleration to be accelerated to even higher energies. We observe the development of filamentary structures in the shock ramp of the forward shock, but not at the reverse shock. This leads to the conclusion that the development of such structures in the shock ramp of quasi-perpendicular collisionless shocks might not necessarily be determined by the existence of a critical sonic Mach number but by a critical shock speed.
The results of the investigations done within this dissertation might be useful for further studies of oblique shocks and for studies using hybrid or magnetohydrodynamic simulations. Together with more sophisticated observational methods, these studies will help to bring us closer to an answer as to how particles can be accelerated in supernova remnants and eventually become cosmic rays that can be detected on Earth.
Synchronization is a fundamental phenomenon in nature. It can be considered as a general property of self-sustained oscillators to adjust their rhythm in the presence of an interaction.
In this work we investigate complex regimes of synchronization phenomena by means of theoretical analysis, numerical modeling, as well as practical analysis of experimental data.
As a subject of our investigation we consider chimera state, where due to spontaneous symmetry-breaking of an initially homogeneous oscillators lattice split the system into two parts with different dynamics. Chimera state as a new synchronization phenomenon was first found in non-locally coupled oscillators system, and has attracted a lot of attention in the last decade. However, the recent studies indicate that this state is also possible in globally coupled systems. In the first part of this work, we show under which conditions the chimera-like state appears in a system of globally coupled identical oscillators with intrinsic delayed feedback. The results of the research explain how initially monostable oscillators became effectivly bistable in the presence of the coupling and create a mean field that sustain the coexistence of synchronized and desynchronized states. Also we discuss other examples, where chimera-like state appears due to frequency dependence of the phase shift in the bistable system.
In the second part, we make further investigation of this topic by modeling influence of an external periodic force to an oscillator with intrinsic delayed feedback. We made stability analysis of the synchronized state and constructed Arnold tongues. The results explain formation of the chimera-like state and hysteric behavior of the synchronization area. Also, we consider two sets of parameters of the oscillator with symmetric and asymmetric Arnold tongues, that correspond to mono- and bi-stable regimes of the oscillator.
In the third part, we demonstrate the results of the work, which was done in collaboration with our colleagues from Psychology Department of University of Potsdam. The project aimed to study the effect of the cardiac rhythm on human perception of time using synchronization analysis. From our part, we made a statistical analysis of the data obtained from the conducted experiment on free time interval reproduction task. We examined how ones heartbeat influences the time perception and searched for possible phase synchronization between heartbeat cycles and time reproduction responses. The findings support the prediction that cardiac cycles can serve as input signals, and is used for reproduction of time intervals in the range of several seconds.
A dramatic efficiency improvement of bulk heterojunction solar cells based on electron-donating conjugated polymers in combination with soluble fullerene derivatives has been achieved over the past years. Certified and reported power conversion efficiencies now reach over 9% for single junctions and exceed the 10% benchmark for tandem solar cells. This trend brightens the vision of organic photovoltaics becoming competitive with inorganic solar cells including the realization of low-cost and large-area organic photovoltaics. For the best performing organic materials systems, the yield of charge generation can be very efficient. However, a detailed understanding of the free charge carrier generation mechanisms at the donor acceptor interface and the energy loss associated with it needs to be established. Moreover, organic solar cells are limited by the competition between charge extraction and free charge recombination, accounting for further efficiency losses. A conclusive picture and the development of precise methodologies for investigating the fundamental processes in organic solar cells are crucial for future material design, efficiency optimization, and the implementation of organic solar cells into commercial products.
In order to advance the development of organic photovoltaics, my thesis focuses on the comprehensive understanding of charge generation, recombination and extraction in organic bulk heterojunction solar cells summarized in 6 chapters on the cumulative basis of 7 individual publications.
The general motivation guiding this work was the realization of an efficient hybrid inorganic/organic tandem solar cell with sub-cells made from amorphous hydrogenated silicon and organic bulk heterojunctions. To realize this project aim, the focus was directed to the low band-gap copolymer PCPDTBT and its derivatives, resulting in the examination of the charge carrier dynamics in PCPDTBT:PC70BM blends in relation to by the blend morphology. The phase separation in this blend can be controlled by the processing additive diiodooctane, enhancing domain purity and size. The quantitative investigation of the free charge formation was realized by utilizing and improving the time delayed collection field technique. Interestingly, a pronounced field dependence of the free carrier generation for all blends is found, with the field dependence being stronger without the additive. Also, the bimolecular recombination coefficient for both blends is rather high and increases with decreasing internal field which we suggest to be caused by a negative field dependence of mobility. The additive speeds up charge extraction which is rationalized by the threefold increase in mobility.
By fluorine attachment within the electron deficient subunit of PCPDTBT, a new polymer F-PCPDTBT is designed. This new material is characterized by a stronger tendency to aggregate as compared to non-fluorinated PCPDTBT. Our measurements show that for F-PCPDTBT:PCBM blends the charge carrier generation becomes more efficient and the field-dependence of free charge carrier generation is weakened. The stronger tendency to aggregate induced by the fluorination also leads to increased polymer rich domains, accompanied in a threefold reduction in the non-geminate recombination coefficient at conditions of open circuit. The size of the polymer domains is nicely correlated to the field-dependence of charge generation and the Langevin reduction factor, which highlights the importance of the domain size and domain purity for efficient charge carrier generation. In total, fluorination of PCPDTBT causes the PCE to increase from 3.6 to 6.1% due to enhanced fill factor, short circuit current and open circuit voltage. Further optimization of the blend ratio, active layer thickness, and polymer molecular weight resulted in 6.6% efficiency for F-PCPDTBT:PC70BM solar cells.
Interestingly, the double fluorinated version 2F-PCPDTBT exhibited poorer FF despite a further reduction of geminate and non-geminate recombination losses. To further analyze this finding, a new technique is developed that measures the effective extraction mobility under charge carrier densities and electrical fields comparable to solar cell operation conditions. This method involves the bias enhanced charge extraction technique. With the knowledge of the carrier density under different electrical field and illumination conditions, a conclusive picture of the changes in charge carrier dynamics leading to differences in the fill factor upon fluorination of PCPDTBT is attained. The more efficient charge generation and reduced recombination with fluorination is counterbalanced by a decreased extraction mobility. Thus, the highest fill factor of 60% and efficiency of 6.6% is reached for F-PCPDTBT blends, while 2F-PCPDTBT blends have only moderate fill factors of 54% caused by the lower effective extraction mobility, limiting the efficiency to 6.5%.
To understand the details of the charge generation mechanism and the related losses, we evaluated the yield and field-dependence of free charge generation using time delayed collection field in combination with sensitive measurements of the external quantum efficiency and absorption coefficients for a variety of blends. Importantly, both the yield and field-dependence of free charge generation is found to be unaffected by excitation energy, including direct charge transfer excitation below the optical band gap. To access the non-detectable absorption at energies of the relaxed charge transfer emission, the absorption was reconstructed from the CT emission, induced via the recombination of thermalized charges in electroluminescence. For a variety of blends, the quantum yield at energies of charge transfer emission was identical to excitations with energies well above the optical band-gap. Thus, the generation proceeds via the split-up of the thermalized charge transfer states in working solar cells. Further measurements were conducted on blends with fine-tuned energy levels and similar blend morphologies by using different fullerene derivatives. A direct correlation between the efficiency of free carrier generation and the energy difference of the relaxed charge transfer state relative to the energy of the charge separated state is found. These findings open up new guidelines for future material design as new high efficiency materials require a minimum energetic offset between charge transfer and the charge separated state while keeping the HOMO level (and LUMO level) difference between donor and acceptor as small as possible.
Bacteria respond to changing environmental conditions by switching the global pattern of expressed genes. In response to specific environmental stresses the cell activates several stress-specific molecules such as sigma factors. They reversibly bind the RNA polymerase to form the so-called holoenzyme and direct it towards the appropriate stress response genes. In exponentially growing E. coli cells, the majority of the transcriptional activity is carried out by the housekeeping sigma factor, while stress responses are often under the control of alternative sigma factors. Different sigma factors compete for binding to a limited pool of RNA polymerase (RNAP) core enzymes, providing a mechanism for cross talk between genes or gene classes via the sharing of expression machinery. To quantitatively analyze the contribution of sigma factor competition to global changes in gene expression, we develop a thermodynamic model that describes binding between sigma factors and core RNAP at equilibrium, transcription, non-specific binding to DNA and the modulation of the availability of the molecular components.
Association of housekeeping sigma factor to RNAP is generally favored by its abundance and higher binding affinity to the core. In order to promote transcription by alternative sigma subunits, the bacterial cell modulates the transcriptional efficiency in a reversible manner through several strategies such as anti-sigma factors, 6S RNA and generally any kind of transcriptional regulators (e.g. activators or inhibitors). By shifting the outcome of sigma factor competition for the core, these modulators bias the transcriptional program of the cell. The model is validated by comparison with in vitro competition experiments, with which excellent agreement is found. We observe that transcription is affected via the modulation of the concentrations of the different types of holoenzymes, so saturated promoters are only weakly affected by sigma factor competition. However, in case of overlapping promoters or promoters recognized by two types of sigma factors, we find that even saturated promoters are strongly affected.
Active transcription effectively lowers the affinity between the sigma factor driving it and the core RNAP, resulting in complex cross talk effects and raising the question of how their in vitro measure is relevant in the cell. We also estimate that sigma factor competition is not strongly affected by non-specific binding of core RNAPs, sigma factors, and holoenzymes to DNA. Finally, we analyze the role of increased core RNAP availability upon the shut-down of ribosomal RNA transcription during stringent response. We find that passive up-regulation of alternative sigma-dependent transcription is not only possible, but also displays hypersensitivity based on the sigma factor competition. Our theoretical analysis thus provides support for a significant role of passive control during that global switch of the gene expression program and gives new insights into RNAP partitioning in the cell.
Despite remarkable progress made in the past century, which has revolutionized our understanding of the universe, there are numerous open questions left in theoretical physics. Particularly important is the fact that the theories describing the fundamental interactions of nature are incompatible. Einstein's theory of general relative describes gravity as a dynamical spacetime, which is curved by matter and whose curvature determines the motion of matter. On the other hand we have quantum field theory, in form of the standard model of particle physics, where particles interact via the remaining interactions - electromagnetic, weak and strong interaction - on a flat, static spacetime without gravity. A theory of quantum gravity is hoped to cure this incompatibility by heuristically replacing classical spacetime by quantum spacetime'. Several approaches exist attempting to define such a theory with differing underlying premises and ideas, where it is not clear which is to be preferred. Yet a minimal requirement is the compatibility with the classical theory, they attempt to generalize. Interestingly many of these models rely on discrete structures in their definition or postulate discreteness of spacetime to be fundamental. Besides the direct advantages discretisations provide, e.g. permitting numerical simulations, they come with serious caveats requiring thorough investigation: In general discretisations break fundamental diffeomorphism symmetry of gravity and are generically not unique. Both complicates establishing the connection to the classical continuum theory. The main focus of this thesis lies in the investigation of this relation for spin foam models. This is done on different levels of the discretisation / triangulation, ranging from few simplices up to the continuum limit. In the regime of very few simplices we confirm and deepen the connection of spin foam models to discrete gravity. Moreover, we discuss dynamical, e.g. diffeomorphism invariance in the discrete, to fix the ambiguities of the models. In order to satisfy these conditions, the discrete models have to be improved in a renormalisation procedure, which also allows us to study their continuum dynamics. Applied to simplified spin foam models, we uncover a rich, non--trivial fixed point structure, which we summarize in a phase diagram. Inspired by these methods, we propose a method to consistently construct the continuum theory, which comes with a unique vacuum state.
The H.E.S.S. array is a third generation Imaging Atmospheric Cherenkov Telescope (IACT) array. It is located in the Khomas Highland in Namibia, and measures very high energy (VHE) gamma-rays. In Phase I, the array started data taking in 2004 with its four identical 13 m telescopes. Since then, H.E.S.S. has emerged as the most successful IACT experiment to date. Among the almost 150 sources of VHE gamma-ray radiation found so far, even the oldest detection, the Crab Nebula, keeps surprising the scientific community with unexplained phenomena such as the recently discovered very energetic flares of high energy gamma-ray radiation. During its most recent flare, which was detected by the Fermi satellite in March 2013, the Crab Nebula was simultaneously observed with the H.E.S.S. array for six nights. The results of the observations will be discussed in detail during the course of this work. During the nights of the flare, the new 24 m × 32 m H.E.S.S. II telescope was still being commissioned, but participated in the data taking for one night. To be able to reconstruct and analyze the data of the H.E.S.S. Phase II array, the algorithms and software used by the H.E.S.S. Phase I array had to be adapted. The most prominent advanced shower reconstruction technique developed by de Naurois and Rolland, the template-based model analysis, compares real shower images taken by the Cherenkov telescope cameras with shower templates obtained using a semi-analytical model. To find the best fitting image, and, therefore, the relevant parameters that describe the air shower best, a pixel-wise log-likelihood fit is done. The adaptation of this advanced shower reconstruction technique to the heterogeneous H.E.S.S. Phase II array for stereo events (i.e. air showers seen by at least two telescopes of any kind), its performance using MonteCarlo simulations as well as its application to real data will be described.
In the presented thesis, the most advanced photon reconstruction technique of ground-based γ-ray astronomy is adapted to the H.E.S.S. 28 m telescope. The method is based on a semi-analytical model of electromagnetic particle showers in the atmosphere. The properties of cosmic γ-rays are reconstructed by comparing the camera image of the telescope with the Cherenkov emission that is expected from the shower model. To suppress the dominant background from charged cosmic rays, events are selected based on several criteria. The performance of the analysis is evaluated with simulated events. The method is then applied to two sources that are known to emit γ-rays. The first of these is the Crab Nebula, the standard candle of ground-based γ-ray astronomy. The results of this source confirm the expected performance of the reconstruction method, where the much lower energy threshold compared to H.E.S.S. I is of particular importance. A second analysis is performed on the region around the Galactic Centre. The analysis results emphasise the capabilities of the new telescope to measure γ-rays in an energy range that is interesting for both theoretical and experimental astrophysics. The presented analysis features the lowest energy threshold that has ever been reached in ground-based γ-ray astronomy, opening a new window to the precise measurement of the physical properties of time-variable sources at energies of several tens of GeV.
In dieser Arbeit werden nichtlineare Kopplungsmechanismen von akustischen Oszillatoren untersucht, die zu Synchronisation führen können. Aufbauend auf die Fragestellungen vorangegangener Arbeiten werden mit Hilfe theoretischer und experimenteller Studien sowie mit Hilfe numerischer Simulationen die Elemente der Tonentstehung in der Orgelpfeife und die Mechanismen der gegenseitigen Wechselwirkung von Orgelpfeifen identifiziert. Daraus wird erstmalig ein vollständig auf den aeroakustischen und fluiddynamischen Grundprinzipien basierendes nichtlinear gekoppeltes Modell selbst-erregter Oszillatoren für die Beschreibung des Verhaltens zweier wechselwirkender Orgelpfeifen entwickelt. Die durchgeführten Modellrechnungen werden mit den experimentellen Befunden verglichen. Es zeigt sich, dass die Tonentstehung und die Kopplungsmechanismen von Orgelpfeifen durch das entwickelte Oszillatormodell in weiten Teilen richtig beschrieben werden. Insbesondere kann damit die Ursache für den nichtlinearen Zusammenhang von Kopplungsstärke und Synchronisation des gekoppelten Zwei-Pfeifen Systems, welcher sich in einem nichtlinearen Verlauf der Arnoldzunge darstellt, geklärt werden. Mit den gewonnenen Erkenntnissen wird der Einfluss des Raumes auf die Tonentstehung bei Orgelpfeifen betrachtet. Dafür werden numerische Simulationen der Wechselwirkung einer Orgelpfeife mit verschiedenen Raumgeometrien, wie z. B. ebene, konvexe, konkave, und gezahnte Geometrien, exemplarisch untersucht. Auch der Einfluss von Schwellkästen auf die Tonentstehung und die Klangbildung der Orgelpfeife wird studiert. In weiteren, neuartigen Synchronisationsexperimenten mit identisch gestimmten Orgelpfeifen, sowie mit Mixturen wird die Synchronisation für verschiedene, horizontale und vertikale Pfeifenabstände in der Ebene der Schallabstrahlung, untersucht. Die dabei erstmalig beobachteten räumlich isotropen Unstetigkeiten im Schwingungsverhalten der gekoppelten Pfeifensysteme, deuten auf abstandsabhängige Wechsel zwischen gegen- und gleichphasigen Sychronisationsregimen hin. Abschließend wird die Möglichkeit dokumentiert, das Phänomen der Synchronisation zweier Orgelpfeifen durch numerische Simulationen, also der Behandlung der kompressiblen Navier-Stokes Gleichungen mit entsprechenden Rand- und Anfangsbedingungen, realitätsnah abzubilden. Auch dies stellt ein Novum dar.
One of the most significant current discussions in Astrophysics relates to the origin of high-energy cosmic rays. According to our current knowledge, the abundance distribution of the elements in cosmic rays at their point of origin indicates, within plausible error limits, that they were initially formed by nuclear processes in the interiors of stars. It is also believed that their energy distribution up to 1018 eV has Galactic origins. But even though the knowledge about potential sources of cosmic rays is quite poor above „ 1015 eV, that is the “knee” of the cosmic-ray spectrum, up to the knee there seems to be a wide consensus that supernova remnants are the most likely candidates. Evidence of this comes from observations of non-thermal X-ray radiation, requiring synchrotron electrons with energies up to 1014 eV, exactly in the remnant of supernovae. To date, however, there is not conclusive evidence that they produce nuclei, the dominant component of cosmic rays, in addition to electrons. In light of this dearth of evidence, γ-ray observations from supernova remnants can offer the most promising direct way to confirm whether or not these astrophysical objects are indeed the main source of cosmic-ray nuclei below the knee. Recent observations with space- and ground-based observatories have established shell-type supernova remnants as GeV-to- TeV γ-ray sources. The interpretation of these observations is however complicated by the different radiation processes, leptonic and hadronic, that can produce similar fluxes in this energy band rendering ambiguous the nature of the emission itself. The aim of this work is to develop a deeper understanding of these radiation processes from a particular shell-type supernova remnant, namely RX J1713.7–3946, using observations of the LAT instrument onboard the Fermi Gamma-Ray Space Telescope. Furthermore, to obtain accurate spectra and morphology maps of the emission associated with this supernova remnant, an improved model of the diffuse Galactic γ-ray emission background is developed. The analyses of RX J1713.7–3946 carried out with this improved background show that the hard Fermi-LAT spectrum cannot be ascribed to the hadronic emission, leading thus to the conclusion that the leptonic scenario is instead the most natural picture for the high-energy γ-ray emission of RX J1713.7–3946. The leptonic scenario however does not rule out the possibility that cosmic-ray nuclei are accelerated in this supernova remnant, but it suggests that the ambient density may not be high enough to produce a significant hadronic γ-ray emission. Further investigations involving other supernova remnants using the improved back- ground developed in this work could allow compelling population studies, and hence prove or disprove the origin of Galactic cosmic-ray nuclei in these astrophysical objects. A break- through regarding the identification of the radiation mechanisms could be lastly achieved with a new generation of instruments such as CTA.
Organische Halbleiter besitzen neue, bemerkenswerte Materialeigenschaften, die sie für die grundlegende Forschung wie auch aktuelle technologische Entwicklung (bsw. org. Leuchtdioden, org. Solarzellen) interessant werden lassen. Aufgrund der starken konformative Freiheit der konjugierten Polymerketten führt die Vielzahl der möglichen Anordnungen und die schwache intermolekulare Wechselwirkung für gewöhnlich zu geringer struktureller Ordnung im Festkörper. Die Morphologie hat gleichzeitig direkten Einfluss auf die elektronische Struktur der organischen Halbleiter, welches sich meistens in einer deutlichen Reduktion der Ladungsträgerbeweglichkeit gegenüber den anorganischen Verwandten zeigt. So stellt die Beweglichkeit der Ladungen im Halbleiter einen der limitierenden Faktoren für die Leistungsfähigkeit bzw. den Wirkungsgrad von funktionellen organischen Bauteilen dar. Im Jahr 2009 wurde ein neues auf Naphthalindiimid und Bithiophen basierendes Dornor/Akzeptor Copolymer vorgestellt [P(NDI2OD‑T2)], welches sich durch seine außergewöhnlich hohe Ladungsträgermobilität auszeichnet. In dieser Arbeit wird die Ladungsträgermobilität in P(NDI2OD‑T2) bestimmt, und der Transport durch eine geringe energetischer Unordnung charakterisiert. Obwohl dieses Material zunächst als amorph beschrieben wurde zeigt eine detaillierte Analyse der optischen Eigenschaften von P(NDI2OD‑T2), dass bereits in Lösung geordnete Vorstufen supramolekularer Strukturen (Aggregate) existieren. Quantenchemische Berechnungen belegen die beobachteten spektralen Änderungen. Mithilfe der NMR-Spektroskopie kann die Bildung der Aggregate unabhängig von optischer Spektroskopie bestätigt werden. Die Analytische Ultrazentrifugation an P(NDI2OD‑T2) Lösungen legt nahe, dass sich die Aggregation innerhalb der einzelnen Ketten unter Reduktion des hydrodynamischen Radius vollzieht. Die Ausbildung supramolekularen Strukturen nimmt auch eine signifikante Rolle bei der Filmbildung ein und verhindert gleichzeitig die Herstellung amorpher P(NDI2OD‑T2) Filme. Durch chemische Modifikation der P(NDI2OD‑T2)-Kette und verschiedener Prozessierungs-Methoden wurde eine Änderung des Kristallinitätsgrades und gleichzeitig der Orientierung der kristallinen Domänen erreicht und mittels Röntgenbeugung quantifiziert. In hochauflösenden Elektronenmikroskopie-Messungen werden die Netzebenen und deren Einbettung in die semikristallinen Strukturen direkt abgebildet. Aus der Kombination der verschiedenen Methoden erschließt sich ein Gesamtbild der Nah- und Fernordnung in P(NDI2OD‑T2). Über die Messung der Elektronenmobilität dieser Schichten wird die Anisotropie des Ladungstransports in den kristallographischen Raumrichtungen von P(NDI2OD‑T2) charakterisiert und die Bedeutung der intramolekularen Wechselwirkung für effizienten Ladungstransport herausgearbeitet. Gleichzeitig wird deutlich, wie die Verwendung von größeren und planaren funktionellen Gruppen zu höheren Ladungsträgermobilitäten führt, welche im Vergleich zu klassischen semikristallinen Polymeren weniger sensitiv auf die strukturelle Unordnung im Film sind.
In processing and data storage mainly ferromagnetic (FM) materials are being used. Approaching physical limits, new concepts have to be found for faster, smaller switches, for higher data densities and more energy efficiency. Some of the discussed new concepts involve the material classes of correlated oxides and materials with antiferromagnetic coupling. Their applicability depends critically on their switching behavior, i.e., how fast and how energy efficient material properties can be manipulated. This thesis presents investigations of ultrafast non-equilibrium phase transitions on such new materials. In transition metal oxides (TMOs) the coupling of different degrees of freedom and resulting low energy excitation spectrum often result in spectacular changes of macroscopic properties (colossal magneto resistance, superconductivity, metal-to-insulator transitions) often accompanied by nanoscale order of spins, charges, orbital occupation and by lattice distortions, which make these material attractive. Magnetite served as a prototype for functional TMOs showing a metal-to-insulator-transition (MIT) at T = 123 K. By probing the charge and orbital order as well as the structure after an optical excitation we found that the electronic order and the structural distortion, characteristics of the insulating phase in thermal equilibrium, are destroyed within the experimental resolution of 300 fs. The MIT itself occurs on a 1.5 ps timescale. It shows that MITs in functional materials are several thousand times faster than switching processes in semiconductors. Recently ferrimagnetic and antiferromagnetic (AFM) materials have become interesting. It was shown in ferrimagnetic GdFeCo, that the transfer of angular momentum between two opposed FM subsystems with different time constants leads to a switching of the magnetization after laser pulse excitation. In addition it was theoretically predicted that demagnetization dynamics in AFM should occur faster than in FM materials as no net angular momentum has to be transferred out of the spin system. We investigated two different AFM materials in order to learn more about their ultrafast dynamics. In Ho, a metallic AFM below T ≈ 130 K, we found that the AFM Ho can not only be faster but also ten times more energy efficiently destroyed as order in FM comparable metals. In EuTe, an AFM semiconductor below T ≈ 10 K, we compared the loss of magnetization and laser-induced structural distortion in one and the same experiment. Our experiment shows that they are effectively disentangled. An exception is an ultrafast release of lattice dynamics, which we assign to the release of magnetostriction. The results presented here were obtained with time-resolved resonant soft x-ray diffraction at the Femtoslicing source of the Helmholtz-Zentrum Berlin and at the free-electron laser in Stanford (LCLS). In addition the development and setup of a new UHV-diffractometer for these experiments will be reported.
When azobenzene-modified photosensitive polymer films are irradiated with light interference patterns, topographic variations in the film develop that follow the electric field vector distribution resulting in the formation of surface relief grating (SRG). The exact correspondence of the electric field vector orientation in interference pattern in relation to the presence of local topographic minima or maxima of SRG is in general difficult to determine. In my thesis, we have established a systematic procedure to accomplish the correlation between different interference patterns and the topography of SRG. For this, we devise a new setup combining an atomic force microscope and a two-beam interferometer (IIAFM). With this set-up, it is possible to track the topography change in-situ, while at the same time changing polarization and phase of the impinging interference pattern. To validate our results, we have compared two photosensitive materials named in short as PAZO and trimer. This is the first time that an absolute correspondence between the local distribution of electric field vectors of interference pattern and the local topography of the relief grating could be established exhaustively. In addition, using our IIAFM we found that for a certain polarization combination of two orthogonally polarized interfering beams namely SP (↕, ↔) interference pattern, the topography forms SRG with only half the period of the interference patterns. Exploiting this phenomenon we are able to fabricate surface relief structures below diffraction limit with characteristic features measuring only 140 nm, by using far field optics with a wavelength of 491 nm. We have also probed for the stresses induced during the polymer mass transport by placing an ultra-thin gold film on top (5–30 nm). During irradiation, the metal film not only deforms along with the SRG formation, but ruptures in regular and complex manner. The morphology of the cracks differs strongly depending on the electric field distribution in the interference pattern even when the magnitude and the kinetic of the strain are kept constant. This implies a complex local distribution of the opto-mechanical stress along the topography grating. The neutron reflectivity measurements of the metal/polymer interface indicate the penetration of metal layer within the polymer resulting in the formation of bonding layer that confirms the transduction of light induced stresses in the polymer layer to a metal film.
LCST-type synthetic thermoresponsive polymers can reversibly respond to certain stimuli in aqueous media with a massive change of their physical state. When fluorophores, that are sensitive to such changes, are incorporated into the polymeric structure, the response can be translated into a fluorescence signal. Based on this idea, this thesis presents sensing schemes which transduce the stimuli-induced variations in the solubility of polymer chains with covalently-bound fluorophores into a well-detectable fluorescence output. Benefiting from the principles of different photophysical phenomena, i.e. of fluorescence resonance energy transfer and solvatochromism, such fluorescent copolymers enabled monitoring of stimuli such as the solution temperature and ionic strength, but also of association/disassociation mechanisms with other macromolecules or of biochemical binding events through remarkable changes in their fluorescence properties. For instance, an aqueous ratiometric dual sensor for temperature and salts was developed, relying on the delicate supramolecular assembly of a thermoresponsive copolymer with a thiophene-based conjugated polyelectrolyte. Alternatively, by taking advantage of the sensitivity of solvatochromic fluorophores, an increase in solution temperature or the presence of analytes was signaled as an enhancement of the fluorescence intensity. A simultaneous use of the sensitivity of chains towards the temperature and a specific antibody allowed monitoring of more complex phenomena such as competitive binding of analytes. The use of different thermoresponsive polymers, namely poly(N-isopropylacrylamide) and poly(meth)acrylates bearing oligo(ethylene glycol) side chains, revealed that the responsive polymers differed widely in their ability to perform a particular sensing function. In order to address questions regarding the impact of the chemical structure of the host polymer on the sensing performance, the macromolecular assembly behavior below and above the phase transition temperature was evaluated by a combination of fluorescence and light scattering methods. It was found that although the temperature-triggered changes in the macroscopic absorption characteristics were similar for these polymers, properties such as the degree of hydration or the extent of interchain aggregations differed substantially. Therefore, in addition to the demonstration of strategies for fluorescence-based sensing with thermoresponsive polymers, this work highlights the role of the chemical structure of the two popular thermoresponsive polymers on the fluorescence response. The results are fundamentally important for the rational choice of polymeric materials for a specific sensing strategy.
Donor-acceptor (D-A) copolymers have revolutionized the field of organic electronics over the last decade. Comprised of a electron rich and an electron deficient molecular unit, these copolymers facilitate the systematic modification of the material's optoelectronic properties. The ability to tune the optical band gap and to optimize the molecular frontier orbitals as well as the manifold of structural sites that enable chemical modifications has created a tremendous variety of copolymer structures. Today, these materials reach or even exceed the performance of amorphous inorganic semiconductors. Most impressively, the charge carrier mobility of D-A copolymers has been pushed to the technologically important value of 10 cm^{2}V^{-1}s^{-1}. Furthermore, owed to their enormous variability they are the material of choice for the donor component in organic solar cells, which have recently surpassed the efficiency threshold of 10%. Because of the great number of available D-A copolymers and due to their fast chemical evolution, there is a significant lack of understanding of the fundamental physical properties of these materials. Furthermore, the complex chemical and electronic structure of D-A copolymers in combination with their semi-crystalline morphology impede a straightforward identification of the microscopic origin of their superior performance. In this thesis, two aspects of prototype D-A copolymers were analysed. These are the investigation of electron transport in several copolymers and the application of low band gap copolymers as acceptor component in organic solar cells. In the first part, the investigation of a series of chemically modified fluorene-based copolymers is presented. The charge carrier mobility varies strongly between the different derivatives, although only moderate structural changes on the copolymers structure were made. Furthermore, rather unusual photocurrent transients were observed for one of the copolymers. Numerical simulations of the experimental results reveal that this behavior arises from a severe trapping of electrons in an exponential distribution of trap states. Based on the comparison of simulation and experiment, the general impact of charge carrier trapping on the shape of photo-CELIV and time-of-flight transients is discussed. In addition, the high performance naphthalenediimide (NDI)-based copolymer P(NDI2OD-T2) was characterized. It is shown that the copolymer posses one of the highest electron mobilities reported so far, which makes it attractive to be used as the electron accepting component in organic photovoltaic cells.\par Solar cells were prepared from two NDI-containing copolymers, blended with the hole transporting polymer P3HT. I demonstrate that the use of appropriate, high boiling point solvents can significantly increase the power conversion efficiency of these devices. Spectroscopic studies reveal that the pre-aggregation of the copolymers is suppressed in these solvents, which has a strong impact on the blend morphology. Finally, a systematic study of P3HT:P(NDI2OD-T2) blends is presented, which quantifies the processes that limit the efficiency of devices. The major loss channel for excited states was determined by transient and steady state spectroscopic investigations: the majority of initially generated electron-hole pairs is annihilated by an ultrafast geminate recombination process. Furthermore, exciton self-trapping in P(NDI2OD-T2) domains account for an additional reduction of the efficiency. The correlation of the photocurrent to microscopic morphology parameters was used to disclose the factors that limit the charge generation efficiency. Our results suggest that the orientation of the donor and acceptor crystallites relative to each other represents the main factor that determines the free charge carrier yield in this material system. This provides an explanation for the overall low efficiencies that are generally observed in all-polymer solar cells.
Unstetige Galerkin-Diskretisierung niedriger Ordnung in einem atmosphärischen Multiskalenmodell
(2014)
Die Dynamik der Atmosphäre der Erde umfasst einen Bereich von mikrophysikalischer Turbulenz über konvektive Prozesse und Wolkenbildung bis zu planetaren Wellenmustern. Für Wettervorhersage und zur Betrachtung des Klimas über Jahrzehnte und Jahrhunderte ist diese Gegenstand der Modellierung mit numerischen Verfahren. Mit voranschreitender Entwicklung der Rechentechnik sind Neuentwicklungen der dynamischen Kerne von Klimamodellen, die mit der feiner werdenden Auflösung auch entsprechende Prozesse auflösen können, notwendig. Der dynamische Kern eines Modells besteht in der Umsetzung (Diskretisierung) der grundlegenden dynamischen Gleichungen für die Entwicklung von Masse, Energie und Impuls, so dass sie mit Computern numerisch gelöst werden können. Die vorliegende Arbeit untersucht die Eignung eines unstetigen Galerkin-Verfahrens niedriger Ordnung für atmosphärische Anwendungen. Diese Eignung für Gleichungen mit Wirkungen von externen Kräften wie Erdanziehungskraft und Corioliskraft ist aus der Theorie nicht selbstverständlich. Es werden nötige Anpassungen beschrieben, die das Verfahren stabilisieren, ohne sogenannte „slope limiter” einzusetzen. Für das unmodifizierte Verfahren wird belegt, dass es nicht geeignet ist, atmosphärische Gleichgewichte stabil darzustellen. Das entwickelte stabilisierte Modell reproduziert eine Reihe von Standard-Testfällen der atmosphärischen Dynamik mit Euler- und Flachwassergleichungen in einem weiten Bereich von räumlichen und zeitlichen Skalen. Die Lösung der thermischen Windgleichung entlang der mit den Isobaren identischen charakteristischen Kurven liefert atmosphärische Gleichgewichtszustände mit durch vorgegebenem Grundstrom einstellbarer Neigung zu(barotropen und baroklinen)Instabilitäten, die für die Entwicklung von Zyklonen wesentlich sind. Im Gegensatz zu früheren Arbeiten sind diese Zustände direkt im z-System(Höhe in Metern)definiert und müssen nicht aus Druckkoordinaten übertragen werden.Mit diesen Zuständen, sowohl als Referenzzustand, von dem lediglich die Abweichungen numerisch betrachtet werden, und insbesondere auch als Startzustand, der einer kleinen Störung unterliegt, werden verschiedene Studien der Simulation von barotroper und barokliner Instabilität durchgeführt. Hervorzuheben ist dabei die durch die Formulierung von Grundströmen mit einstellbarer Baroklinität ermöglichte simulationsgestützte Studie des Grades der baroklinen Instabilität verschiedener Wellenlängen in Abhängigkeit von statischer Stabilität und vertikalem Windgradient als Entsprechung zu Stabilitätskarten aus theoretischen Betrachtungen in der Literatur.
In the presence of a solid-liquid or liquid-air interface, bacteria can choose between a planktonic and a sessile lifestyle. Depending on environmental conditions, cells swimming in close proximity to the interface can irreversibly attach to the surface and grow into three-dimensional aggregates where the majority of cells is sessile and embedded in an extracellular polymer matrix (biofilm). We used microfluidic tools and time lapse microscopy to perform experiments with the polarly flagellated soil bacterium Pseudomonas putida (P. putida), a bacterial species that is able to form biofilms. We analyzed individual trajectories of swimming cells, both in the bulk fluid and in close proximity to a glass-liquid interface. Additionally, surface related growth during the early phase of biofilm formation was investigated. In the bulk fluid, P.putida shows a typical bacterial swimming pattern of alternating periods of persistent displacement along a line (runs) and fast reorientation events (turns) and cells swim with an average speed around 24 micrometer per second. We found that the distribution of turning angles is bimodal with a dominating peak around 180 degrees. In approximately six out of ten turning events, the cell reverses its swimming direction. In addition, our analysis revealed that upon a reversal, the cell systematically changes its swimming speed by a factor of two on average. Based on the experimentally observed values of mean runtime and rotational diffusion, we presented a model to describe the spreading of a population of cells by a run-reverse random walker with alternating speeds. We successfully recover the mean square displacement and, by an extended version of the model, also the negative dip in the directional autocorrelation function as observed in the experiments. The analytical solution of the model demonstrates that alternating speeds enhance a cells ability to explore its environment as compared to a bacterium moving at a constant intermediate speed. As compared to the bulk fluid, for cells swimming near a solid boundary we observed an increase in swimming speed at distances below d= 5 micrometer and an increase in average angular velocity at distances below d= 4 micrometer. While the average speed was maximal with an increase around 15% at a distance of d= 3 micrometer, the angular velocity was highest in closest proximity to the boundary at d=1 micrometer with an increase around 90% as compared to the bulk fluid. To investigate the swimming behavior in a confinement between two solid boundaries, we developed an experimental setup to acquire three-dimensional trajectories using a piezo driven objective mount coupled to a high speed camera. Results on speed and angular velocity were consistent with motility statistics in the presence of a single boundary. Additionally, an analysis of the probability density revealed that a majority of cells accumulated near the upper and lower boundaries of the microchannel. The increase in angular velocity is consistent with previous studies, where bacteria near a solid boundary were shown to swim on circular trajectories, an effect which can be attributed to a wall induced torque. The increase in speed at a distance of several times the size of the cell body, however, cannot be explained by existing theories which either consider the drag increase on cell body and flagellum near a boundary (resistive force theory) or model the swimming microorganism by a multipole expansion to account for the flow field interaction between cell and boundary. An accumulation of swimming bacteria near solid boundaries has been observed in similar experiments. Our results confirm that collisions with the surface play an important role and hydrodynamic interactions alone cannot explain the steady-state accumulation of cells near the channel walls. Furthermore, we monitored the number growth of cells in the microchannel under medium rich conditions. We observed that, after a lag time, initially isolated cells at the surface started to grow by division into colonies of increasing size, while coexisting with a comparable smaller number of swimming cells. After 5:50 hours, we observed a sudden jump in the number of swimming cells, which was accompanied by a breakup of bigger clusters on the surface. After approximately 30 minutes where planktonic cells dominated in the microchannel, individual swimming cells reattached to the surface. We interpret this process as an emigration and recolonization event. A number of complementary experiments were performed to investigate the influence of collective effects or a depletion of the growth medium on the transition. Similar to earlier observations on another bacterium from the same family we found that the release of cells to the swimming phase is most likely the result of an individual adaption process, where syntheses of proteins for flagellar motility are upregulated after a number of division cycles at the surface.
Organic semiconductors combine the benefits of organic materials, i.e., low-cost production, mechanical flexibility, lightweight, and robustness, with the fundamental semiconductor properties light absorption, emission, and electrical conductivity. This class of material has several advantages over conventional inorganic semiconductors that have led, for instance, to the commercialization of organic light-emitting diodes which can nowadays be found in the displays of TVs and smartphones. Moreover, organic semiconductors will possibly lead to new electronic applications which rely on the unique mechanical and electrical properties of these materials. In order to push the development and the success of organic semiconductors forward, it is essential to understand the fundamental processes in these materials. This thesis concentrates on understanding how the charge transport in thiophene-based semiconductor layers depends on the layer morphology and how the charge transport properties can be intentionally modified by doping these layers with a strong electron acceptor. By means of optical spectroscopy, the layer morphologies of poly(3-hexylthiophene), P3HT, P3HT-fullerene bulk heterojunction blends, and oligomeric polyquaterthiophene, oligo-PQT-12, are studied as a function of temperature, molecular weight, and processing conditions. The analyses rely on the decomposition of the absorption contributions from the ordered and the disordered parts of the layers. The ordered-phase spectra are analyzed using Spano’s model. It is figured out that the fraction of aggregated chains and the interconnectivity of these domains is fundamental to a high charge carrier mobility. In P3HT layers, such structures can be grown with high-molecular weight, long P3HT chains. Low and medium molecular weight P3HT layers do also contain a significant amount of chain aggregates with high intragrain mobility; however, intergranular connectivity and, therefore, efficient macroscopic charge transport are absent. In P3HT-fullerene blend layers, a highly crystalline morphology that favors the hole transport and the solar cell efficiency can be induced by annealing procedures and the choice of a high-boiling point processing solvent. Based on scanning near-field and polarization optical microscopy, the morphology of oligo-PQT-12 layers is found to be highly crystalline which explains the rather high field-effect mobility in this material as compared to low molecular weight polythiophene fractions. On the other hand, crystalline dislocations and grain boundaries are identified which clearly limit the charge carrier mobility in oligo-PQT-12 layers. The charge transport properties of organic semiconductors can be widely tuned by molecular doping. Indeed, molecular doping is a key to highly efficient organic light-emitting diodes and solar cells. Despite this vital role, it is still not understood how mobile charge carriers are induced into the bulk semiconductor upon the doping process. This thesis contains a detailed study of the doping mechanism and the electrical properties of P3HT layers which have been p-doped by the strong molecular acceptor tetrafluorotetracyanoquinodimethane, F4TCNQ. The density of doping-induced mobile holes, their mobility, and the electrical conductivity are characterized in a broad range of acceptor concentrations. A long-standing debate on the nature of the charge transfer between P3HT and F4TCNQ is resolved by showing that almost every F4TCNQ acceptor undergoes a full-electron charge transfer with a P3HT site. However, only 5% of these charge transfer pairs can dissociate and induce a mobile hole into P3HT which contributes electrical conduction. Moreover, it is shown that the left-behind F4TCNQ ions broaden the density-of-states distribution for the doping-induced mobile holes, which is due to the longrange Coulomb attraction in the low-permittivity organic semiconductors.
Wir schlagen einen allgemein anwendbaren Algorithmus vor, der unter Verwendung des Skalarprodukts von Kraft und Weg zum richtigen Vorzeichen in den Gleichungen für die Arbeit und die Potentielle Energie bei reversiblen Prozessen (Druck-Volumen-Änderung, Dehnung, Elektrostatische Wechselwirkung, Hub)führt. Wir zeigen, dass es dabei möglich ist, systemimmanente oder externe Kräfte zu benutzen. Wir zeigen, dass bei Verwendung von systemimmanenten Kräften das Skalarprodukt mit negativem Vorzeichen anzusetzen ist. Zudem ist es sehr wichtig, nötige Vorzeichenwechsel bei den einzelnen Schritten zu beachten. Wir betonen dies, weil gelegentlich übersehen wird, dass ein Vorzeichenwechsel nötig ist, wenn das Wegdifferential ds durch das Höhendifferential dh beziehungsweise durch das Abstandsdifferential dx oder dr ersetzt werden muss.
The problem under consideration in the thesis is a two level atom in a photonic crystal and a pumping laser. The photonic crystal provides an environment for the atom, that modifies the decay of the exited state, especially if the atom frequency is close to the band gap. The population inversion is investigated als well as the emission spectrum. The dynamics is analysed in the context of open quantum systems. Due to the multiple reflections in the photonic crystal, the system has a finite memory that inhibits the Markovian approximation. In the Heisenberg picture the equations of motion for the system variables form a infinite hierarchy of integro-differential equations. To get a closed system, approximations like a weak coupling approximation are needed. The thesis starts with a simple photonic crystal that is amenable to analytic calculations: a one-dimensional photonic crystal, that consists of alternating layers. The Bloch modes inside and the vacuum modes outside a finite crystal are linked with a transformation matrix that is interpreted as a transfer matrix. Formulas for the band structure, the reflection from a semi-infinite crystal, and the local density of states in absorbing crystals are found; defect modes and negative refraction are discussed. The quantum optics section of the work starts with the discussion of three problems, that are related to the full resonance fluorescence problem: a pure dephasing model, the driven atom and resonance fluorescence in free space. In the lowest order of the system-environment coupling, the one-time expectation values for the full problem are calculated analytically and the stationary states are discussed for certain cases. For the calculation of the two time correlation functions and spectra, the additional problem of correlations between the two times appears. In the Markovian case, the quantum regression theorem is valid. In the general case, the fluctuation dissipation theorem can be used instead. The two-time correlation functions are calculated by the two different methods. Within the chosen approximations, both methods deliver the same result. Several plots show the dependence of the spectrum on the parameters. Some examples for squeezing spectra are shown with different approximations. A projection operator method is used to establish two kinds of Markovian expansion with and without time convolution. The lowest order is identical with the lowest order of system environment coupling, but higher orders give different results.
The life of microorganisms is characterized by two main tasks, rapid growth under conditions permitting growth and survival under stressful conditions. The environments, in which microorganisms dwell, vary in space and time. The microorganisms innovate diverse strategies to readily adapt to the regularly fluctuating environments. Phenotypic heterogeneity is one such strategy, where an isogenic population splits into subpopulations that respond differently under identical environments. Bacterial persistence is a prime example of such phenotypic heterogeneity, whereby a population survives under an antibiotic attack, by keeping a fraction of population in a drug tolerant state, the persister state. Specifically, persister cells grow more slowly than normal cells under growth conditions, but survive longer under stress conditions such as the antibiotic administrations. Bacterial persistence is identified experimentally by examining the population survival upon an antibiotic treatment and the population resuscitation in a growth medium. The underlying population dynamics is explained with a two state model for reversible phenotype switching in a cell within the population. We study this existing model with a new theoretical approach and present analytical expressions for the time scale observed in population growth and resuscitation, that can be easily used to extract underlying model parameters of bacterial persistence. In addition, we recapitulate previously known results on the evolution of such structured population under periodically fluctuating environment using our simple approximation method. Using our analysis, we determine model parameters for Staphylococcus aureus population under several antibiotics and interpret the outcome of cross-drug treatment. Next, we consider the expansion of a population exhibiting phenotype switching in a spatially structured environment consisting of two growth permitting patches separated by an antibiotic patch. The dynamic interplay of growth, death and migration of cells in different patches leads to distinct regimes in population propagation speed as a function of migration rate. We map out the region in parameter space of phenotype switching and migration rate to observe the condition under which persistence is beneficial. Furthermore, we present an extended model that allows mutation from the two phenotypic states to a resistant state. We find that the presence of persister cells may enhance the probability of resistant mutation in a population. Using this model, we explain the experimental results showing the emergence of antibiotic resistance in a Staphylococcus aureus population upon tobramycin treatment. In summary, we identify several roles of bacterial persistence, such as help in spatial expansion, development of multidrug tolerance and emergence of antibiotic resistance. Our study provides a theoretical perspective on the dynamics of bacterial persistence in different environmental conditions. These results can be utilized to design further experiments, and to develop novel strategies to eradicate persistent infections.
Within the course of this thesis, I have investigated the complex interplay between electron and lattice dynamics in nanostructures of perovskite oxides. Femtosecond hard X-ray pulses were utilized to probe the evolution of atomic rearrangement directly, which is driven by ultrafast optical excitation of electrons. The physics of complex materials with a large number of degrees of freedom can be interpreted once the exact fingerprint of ultrafast lattice dynamics in time-resolved X-ray diffraction experiments for a simple model system is well known. The motion of atoms in a crystal can be probed directly and in real-time by femtosecond pulses of hard X-ray radiation in a pump-probe scheme. In order to provide such ultrashort X-ray pulses, I have built up a laser-driven plasma X-ray source. The setup was extended by a stable goniometer, a two-dimensional X-ray detector and a cryogen-free cryostat. The data acquisition routines of the diffractometer for these ultrafast X-ray diffraction experiments were further improved in terms of signal-to-noise ratio and angular resolution. The implementation of a high-speed reciprocal-space mapping technique allowed for a two-dimensional structural analysis with femtosecond temporal resolution. I have studied the ultrafast lattice dynamics, namely the excitation and propagation of coherent phonons, in photoexcited thin films and superlattice structures of the metallic perovskite SrRuO3. Due to the quasi-instantaneous coupling of the lattice to the optically excited electrons in this material a spatially and temporally well-defined thermal stress profile is generated in SrRuO3. This enables understanding the effect of the resulting coherent lattice dynamics in time-resolved X-ray diffraction data in great detail, e.g. the appearance of a transient Bragg peak splitting in both thin films and superlattice structures of SrRuO3. In addition, a comprehensive simulation toolbox to calculate the ultrafast lattice dynamics and the resulting X-ray diffraction response in photoexcited one-dimensional crystalline structures was developed in this thesis work. With the powerful experimental and theoretical framework at hand, I have studied the excitation and propagation of coherent phonons in more complex material systems. In particular, I have revealed strongly localized charge carriers after above-bandgap femtosecond photoexcitation of the prototypical multiferroic BiFeO3, which are the origin of a quasi-instantaneous and spatially inhomogeneous stress that drives coherent phonons in a thin film of the multiferroic. In a structurally imperfect thin film of the ferroelectric Pb(Zr0.2Ti0.8)O3, the ultrafast reciprocal-space mapping technique was applied to follow a purely strain-induced change of mosaicity on a picosecond time scale. These results point to a strong coupling of in- and out-of-plane atomic motion exclusively mediated by structural defects.
Unter geeigneten Wachstumsbedingungen weisen Algenkulturen oft eine größere Produktivität der Zellen auf, als sie bei höheren Pflanzen zu beobachten ist. Chlamydomonas reinhardtii-Zellen sind vergleichsweise klein. So beträgt das Zellvolumen während des vegetativen Zellzyklus etwa 50–3500 µm³. Im Vergleich zu höheren Pflanzen ist in einer Algensuspension die Konzentration der Biomasse allerdings gering. So enthält beispielsweise 1 ml einer üblichen Konzentration zwischen 10E6 und 10E7 Algenzellen. Quantifizierungen von Metaboliten oder Makromolekülen, die zur Modellierung von zellulären Prozessen genutzt werden, werden meist im Zellensemble vorgenommen. Tatsächlich unterliegt jedoch jede Algenzelle einer individuellen Entwicklung, die die Identifizierung charakteristischer allgemeingültiger Systemparameter erschwert. Ziel dieser Arbeit war es, biochemisch relevante Messgrößen in-vivo und in-vitro mit Hilfe optischer Verfahren zu identifizieren und zu quantifizieren. Im ersten Teil der Arbeit wurde ein Puls-Amplituden-Modulation(PAM)-Fluorimetriemessplatz zur Messung der durch äußere Einflüsse bedingten veränderlichen Chlorophyllfluoreszenz an einzelnen Zellen vorgestellt. Die Verwendung eines kommerziellen Mikroskops, die Implementierung empfindlicher Nachweiselektronik und einer geeignete Immobilisierungsmethode ermöglichten es, ein Signal-zu-Rauschverhältnis zu erreichen, mit dem Fluoreszenzsignale einzelner lebender Chlamydomonas-Zellen gemessen werden konnten. Insbesondere wurden das Zellvolumen und der als Maß für die Effizienz des Photosyntheseapparats bzw. die Zellfitness geltende Chlorophyllfluoreszenzparameter Fv/Fm ermittelt und ein hohes Maß an Heterogenität dieser zellulären Parameter in verschiedenen Entwicklungsstadien der synchronisierten Chlamydomonas-Zellen festgestellt. Im zweiten Teil der Arbeit wurden die bildgebende Laser-Scanning-Mikroskopie und anschließende Bilddatenanalyse zur quantitativen Erfassung der wachstumsabhängigen zellulären Parameter angewandt. Ein kommerzielles konfokales Mikroskop wurde um die Möglichkeit der nichtlinearen Mikroskopie erweitert. Diese hat den Vorteil einer lokalisierten Anregung, damit verbunden einer höheren Ortsauflösung und insgesamt geringeren Probenbelastung. Weiterhin besteht neben der Signalgewinnung durch Fluoreszenzanregung die Möglichkeit der Erzeugung der Zweiten Harmonischen (SHG) an biophotonischen Strukturen, wie der zellulären Stärke. Anhand der Verteilungsfunktionen war es möglich mit Hilfe von modelltheoretischen Ansätzen zelluläre Parameter zu ermitteln, die messtechnisch nicht unmittelbar zugänglich sind. Die morphologischen Informationen der Bilddaten ermöglichten die Bestimmung der Zellvolumina und die Volumina subzellularer Strukturen, wie Nuclei, extranucleäre DNA oder Stärkegranula. Weiterhin konnte die Anzahl subzellulärer Strukturen innerhalb einer Zelle bzw. eines Zellverbunds ermittelt werden. Die Analyse der in den Bilddaten enthaltenen Signalintensitäten war Grundlage einer relativen Konzentrationsbestimmung von zellulären Komponenten, wie DNA bzw. Stärke. Mit dem hier vorgestellten Verfahren der nichtlinearen Mikroskopie und nachfolgender Bilddatenanalyse konnte erstmalig die Verteilung des zellulären Stärkegehalts in einer Chlamydomonas-Population während des Wachstums bzw. nach induziertem Stärkeabbau verfolgt werden. Im weiteren Verlauf wurde diese Methode auch auf Gefrierschnitte höherer Pflanzen, wie Arabidopsis thaliana, angewendet. Im Ergebnis wurde gezeigt, dass viele zelluläre Parameter, wie das Volumen, der zelluläre DNA- und Stärkegehalt bzw. die Anzahl der Stärkegranula durch eine Lognormalverteilung, mit wachstumsabhängiger Parametrisierung, beschrieben werden. Zelluläre Parameter, wie Stoffkonzentration und zelluläres Volumen, zeigen keine signifikanten Korrelationen zueinander, woraus geschlussfolgert werden muss, dass es ein hohes Maß an Heterogenität der zellulären Parameter innerhalb der synchronisierten Chlamydomonas-Populationen gibt. Diese Aussage gilt sowohl für die als homogenste Form geltenden Synchronkulturen von Chlamydomonas reinhardtii als auch für die gemessenen zellulären Parameter im intakten Zellverbund höherer Pflanzen. Dieses Ergebnis ist insbesondere für modelltheoretische Betrachtungen von Relevanz, die sich auf empirische Daten bzw. zelluläre Parameter stützen welche im Zellensemble gemessen wurden und somit nicht notwendigerweise den zellulären Status einer einzelnen Zelle repräsentieren.
Famously, Einstein read off the geometry of spacetime from Maxwell's equations. Today, we take this geometry that serious that our fundamental theory of matter, the standard model of particle physics, is based on it. However, it seems that there is a gap in our understanding if it comes to the physics outside of the solar system. Independent surveys show that we need concepts like dark matter and dark energy to make our models fit with the observations. But these concepts do not fit in the standard model of particle physics. To overcome this problem, at least, we have to be open to matter fields with kinematics and dynamics beyond the standard model. But these matter fields might then very well correspond to different spacetime geometries. This is the basis of this thesis: it studies the underlying spacetime geometries and ventures into the quantization of those matter fields independently of any background geometry. In the first part of this thesis, conditions are identified that a general tensorial geometry must fulfill to serve as a viable spacetime structure. Kinematics of massless and massive point particles on such geometries are introduced and the physical implications are investigated. Additionally, field equations for massive matter fields are constructed like for example a modified Dirac equation. In the second part, a background independent formulation of quantum field theory, the general boundary formulation, is reviewed. The general boundary formulation is then applied to the Unruh effect as a testing ground and first attempts are made to quantize massive matter fields on tensorial spacetimes.
Nucleation and growth of unsubstituted metal phthalocyanine films from solution on planar substrates
(2012)
In den vergangenen Jahren wurden kosteneffiziente nasschemische Beschichtungsverfahren für die Herstellung organischer Dünnfilme für verschiedene opto-elektronische Anwendungen entdeckt und weiterentwickelt. Unter anderem wurden Phthalocyanin-Moleküle in photoaktiven Schichten für die Herstellung von Solarzellen intensiv erforscht. Aufgrund der kleinen bzw. unbekannten Löslichkeit wurden Phthalocyanin-Schichten durch Aufdampfverfahren im Vakuum hergestellt. Des Weiteren wurde die Löslichkeit durch chemische Synthese erhöht, was aber die Eigenschaften von Pc beeinträchtigte. In dieser Arbeit wurde die Löslichkeit, optische Absorption und Stabilität von 8 verschiedenen unsubstituierten Metall-Phthalocyaninen in 28 verschiedenen Lösungsmitteln quantitativ gemessen. Wegen ausreichender Löslichkeit, Stabilität und Anwendbarkeit in organischen Solarzellen wurde Kupferphthalocyanin (CuPc) in Trifluoressigsäure (TFA) für weitere Untersuchungen ausgewählt. Durch die Rotationsbeschichtung von CuPc aus TFA Lösung wurde ein dünner Film aus der verdampfenden Lösung auf dem Substrat platziert. Nach dem Verdampfen des Lösungsmittels, die Nanobändern aus CuPc bedecken das Substrat. Die Nanobänder haben eine Dicke von etwa ~ 1 nm (typische Dimension eines CuPc-Molekül) und variierender Breite und Länge, je nach Menge des Materials. Solche Nanobändern können durch Rotationsbeschichtung oder auch durch andere Nassbeschichtungsverfahren, wie Tauchbeschichtung, erzeugt werden. Ähnliche Fibrillen-Strukturen entstehen durch Nassbeschichtung von anderen Metall-Phthalocyaninen, wie Eisen- und Magnesium-Phthalocyanin, aus TFA-Lösung sowie auf anderen Substraten, wie Glas oder Indium Zinnoxid. Materialeigenschaften von aufgebrachten CuPc aus TFA Lösung und CuPc in der Lösung wurden ausführlich mit Röntgenbeugung, Spektroskopie- und Mikroskopie Methoden untersucht. Es wird gezeigt, dass die Nanobänder nicht in der Lösung, sondern durch Verdampfen des Lösungsmittels und der Übersättigung der Lösung entstehen. Die Rasterkraftmikroskopie wurde dazu verwendet, um die Morphologie des getrockneten Films bei unterschiedlicher Konzentration zu studieren. Der Mechanismus der Entstehung der Nanobändern wurde im Detail studiert. Gemäß der Keimbildung und Wachstumstheorie wurde die Entstehung der CuPc Nanobänder aus einer übersättigt Lösung diskutiert. Die Form der Nanobändern wurde unter Berücksichtigung der Wechselwirkung zwischen den Molekülen und dem Substrat diskutiert. Die nassverarbeitete CuPc-Dünnschicht wurde als Donorschicht in organischen Doppelschicht Solarzellen mit C60-Molekül, als Akzeptor eingesetzt. Die Effizienz der Energieumwandlung einer solchen Zelle wurde entsprechend den Schichtdicken der CuPc Schicht untersucht.
In dieser Arbeit werden die Effekte der Synchronisation nichtlinearer, akustischer Oszillatoren am Beispiel zweier Orgelpfeifen untersucht. Aus vorhandenen, experimentellen Messdaten werden die typischen Merkmale der Synchronisation extrahiert und dargestellt. Es folgt eine detaillierte Analyse der Übergangsbereiche in das Synchronisationsplateau, der Phänomene während der Synchronisation, als auch das Austreten aus der Synchronisationsregion beider Orgelpfeifen, bei verschiedenen Kopplungsstärken. Die experimentellen Befunde werfen Fragestellungen nach der Kopplungsfunktion auf. Dazu wird die Tonentstehung in einer Orgelpfeife untersucht. Mit Hilfe von numerischen Simulationen der Tonentstehung wird der Frage nachgegangen, welche fluiddynamischen und aero-akustischen Ursachen die Tonentstehung in der Orgelpfeife hat und inwiefern sich die Mechanismen auf das Modell eines selbsterregten akustischen Oszillators abbilden lässt. Mit der Methode des Coarse Graining wird ein Modellansatz formuliert.
Estimation of the self-similarity exponent has attracted growing interest in recent decades and became a research subject in various fields and disciplines. Real-world data exhibiting self-similar behavior and/or parametrized by self-similarity exponent (in particular Hurst exponent) have been collected in different fields ranging from finance and human sciencies to hydrologic and traffic networks. Such rich classes of possible applications obligates researchers to investigate qualitatively new methods for estimation of the self-similarity exponent as well as identification of long-range dependencies (or long memory). In this thesis I present the Bayesian estimation of the Hurst exponent. In contrast to previous methods, the Bayesian approach allows the possibility to calculate the point estimator and confidence intervals at the same time, bringing significant advantages in data-analysis as discussed in this thesis. Moreover, it is also applicable to short data and unevenly sampled data, thus broadening the range of systems where the estimation of the Hurst exponent is possible. Taking into account that one of the substantial classes of great interest in modeling is the class of Gaussian self-similar processes, this thesis considers the realizations of the processes of fractional Brownian motion and fractional Gaussian noise. Additionally, applications to real-world data, such as the data of water level of the Nile River and fixational eye movements are also discussed.
Actin is one of the most abundant and highly conserved proteins in eukaryotic cells. The globular protein assembles into long filaments, which form a variety of different networks within the cytoskeleton. The dynamic reorganization of these networks - which is pivotal for cell motility, cell adhesion, and cell division - is based on cycles of polymerization (assembly) and depolymerization (disassembly) of actin filaments. Actin binds ATP and within the filament, actin-bound ATP is hydrolyzed into ADP on a time scale of a few minutes. As ADP-actin dissociates faster from the filament ends than ATP-actin, the filament becomes less stable as it grows older. Recent single filament experiments, where abrupt dynamical changes during filament depolymerization have been observed, suggest the opposite behavior, however, namely that the actin filaments become increasingly stable with time. Several mechanisms for this stabilization have been proposed, ranging from structural transitions of the whole filament to surface attachment of the filament ends. The key issue of this thesis is to elucidate the unexpected interruptions of depolymerization by a combination of experimental and theoretical studies. In new depolymerization experiments on single filaments, we confirm that filaments cease to shrink in an abrupt manner and determine the time from the initiation of depolymerization until the occurrence of the first interruption. This duration differs from filament to filament and represents a stochastic variable. We consider various hypothetical mechanisms that may cause the observed interruptions. These mechanisms cannot be distinguished directly, but they give rise to distinct distributions of the time until the first interruption, which we compute by modeling the underlying stochastic processes. A comparison with the measured distribution reveals that the sudden truncation of the shrinkage process neither arises from blocking of the ends nor from a collective transition of the whole filament. Instead, we predict a local transition process occurring at random sites within the filament. The combination of additional experimental findings and our theoretical approach confirms the notion of a local transition mechanism and identifies the transition as the photo-induced formation of an actin dimer within the filaments. Unlabeled actin filaments do not exhibit pauses, which implies that, in vivo, older filaments become destabilized by ATP hydrolysis. This destabilization can be identified with an acceleration of the depolymerization prior to the interruption. In the final part of this thesis, we theoretically analyze this acceleration to infer the mechanism of ATP hydrolysis. We show that the rate of ATP hydrolysis is constant within the filament, corresponding to a random as opposed to a vectorial hydrolysis mechanism.
This work investigates diffusion in nonlinear Hamiltonian systems. The diffusion, more precisely subdiffusion, in such systems is induced by the intrinsic chaotic behavior of trajectories and thus is called chaotic diffusion''. Its properties are studied on the example of one- or two-dimensional lattices of harmonic or nonlinear oscillators with nearest neighbor couplings. The fundamental observation is the spreading of energy for localized initial conditions. Methods of quantifying this spreading behavior are presented, including a new quantity called excitation time. This new quantity allows for a more precise analysis of the spreading than traditional methods. Furthermore, the nonlinear diffusion equation is introduced as a phenomenologic description of the spreading process and a number of predictions on the density dependence of the spreading are drawn from this equation. Two mathematical techniques for analyzing nonlinear Hamiltonian systems are introduced. The first one is based on a scaling analysis of the Hamiltonian equations and the results are related to similar scaling properties of the NDE. From this relation, exact spreading predictions are deduced. Secondly, the microscopic dynamics at the edge of spreading states are thoroughly analyzed, which again suggests a scaling behavior that can be related to the NDE. Such a microscopic treatment of chaotically spreading states in nonlinear Hamiltonian systems has not been done before and the results present a new technique of connecting microscopic dynamics with macroscopic descriptions like the nonlinear diffusion equation. All theoretical results are supported by heavy numerical simulations, partly obtained on one of Europe's fastest supercomputers located in Bologna, Italy. In the end, the highly interesting case of harmonic oscillators with random frequencies and nonlinear coupling is studied, which resembles to some extent the famous Discrete Anderson Nonlinear Schroedinger Equation. For this model, a deviation from the widely believed power-law spreading is observed in numerical experiments. Some ideas on a theoretical explanation for this deviation are presented, but a conclusive theory could not be found due to the complicated phase space structure in this case. Nevertheless, it is hoped that the techniques and results presented in this work will help to eventually understand this controversely discussed case as well.
We investigate properties of quantum mechanical systems in the light of quantum information theory. We put an emphasize on systems with infinite-dimensional Hilbert spaces, so-called continuous-variable systems'', which are needed to describe quantum optics beyond the single photon regime and other Bosonic quantum systems. We present methods to obtain a description of such systems from a series of measurements in an efficient manner and demonstrate the performance in realistic situations by means of numerical simulations. We consider both unconditional quantum state tomography, which is applicable to arbitrary systems, and tomography of matrix product states. The latter allows for the tomography of many-body systems because the necessary number of measurements scales merely polynomially with the particle number, compared to an exponential scaling in the generic case. We also present a method to realize such a tomography scheme for a system of ultra-cold atoms in optical lattices. Furthermore, we discuss in detail the possibilities and limitations of using continuous-variable systems for measurement-based quantum computing. We will see that the distinction between Gaussian and non-Gaussian quantum states and measurements plays an crucial role. We also provide an algorithm to solve the large and interesting class of naturally occurring Hamiltonians, namely frustration free ones, efficiently and use this insight to obtain a simple approximation method for slightly frustrated systems. To achieve this goals, we make use of, among various other techniques, the well developed theory of matrix product states, tensor networks, semi-definite programming, and matrix analysis.
The microscopic origin of ultrafast demagnetization, i.e. the quenching of the magnetization of a ferromagnetic metal on a sub-picosecond timescale after laser excitation, is still only incompletely understood, despite a large body of experimental and theoretical work performed since the discovery of the effect more than 15 years ago. Time- and element-resolved x-ray magnetic circular dichroism measurements can provide insight into the microscopic processes behind ultrafast demagnetization as well as its dependence on materials properties. Using the BESSY II Femtoslicing facility, a storage ring based source of 100 fs short soft x-ray pulses, ultrafast magnetization dynamics of ferromagnetic NiFe and GdTb alloys as well as a Au/Ni layered structure were investigated in laser pump – x-ray probe experiments. After laser excitation, the constituents of Ni50Fe50 and Ni80Fe20 exhibit distinctly different time constants of demagnetization, leading to decoupled dynamics, despite the strong exchange interaction that couples the Ni and Fe sublattices under equilibrium conditions. Furthermore, the time constants of demagnetization for Ni and Fe are different in Ni50Fe50 and Ni80Fe20, and also different from the values for the respective pure elements. These variations are explained by taking the magnetic moments of the Ni and Fe sublattices, which are changed from the pure element values due to alloying, as well as the strength of the intersublattice exchange interaction into account. GdTb exhibits demagnetization in two steps, typical for rare earths. The time constant of the second, slower magnetization decay was previously linked to the strength of spin-lattice coupling in pure Gd and Tb, with the stronger, direct spin-lattice coupling in Tb leading to a faster demagnetization. In GdTb, the demagnetization of Gd follows Tb on all timescales. This is due to the opening of an additional channel for the dissipation of spin angular momentum to the lattice, since Gd magnetic moments in the alloy are coupled via indirect exchange interaction to neighboring Tb magnetic moments, which are in turn strongly coupled to the lattice. Time-resolved measurements of the ultrafast demagnetization of a Ni layer buried under a Au cap layer, thick enough to absorb nearly all of the incident pump laser light, showed a somewhat slower but still sub-picosecond demagnetization of the buried Ni layer in Au/Ni compared to a Ni reference sample. Supported by simulations, I conclude that demagnetization can thus be induced by transport of hot electrons excited in the Au layer into the Ni layer, without the need for direct interaction between photons and spins.
Structural dynamics of photoexcited nanolayered perovskites studied by ultrafast x-ray diffraction
(2012)
This publication-based thesis represents a contribution to the active research field of ultrafast structural dynamics in laser-excited nanostructures. The investigation of such dynamics is mandatory for the understanding of the various physical processes on microscopic scales in complex materials which have great potentials for advances in many technological applications. I theoretically and experimentally examine the coherent, incoherent and anharmonic lattice dynamics of epitaxial metal-insulator heterostructures on timescales ranging from femtoseconds up to nanoseconds. To infer information on the transient dynamics in the photoexcited crystal lattices experimental techniques using ultrashort optical and x-ray pulses are employed. The experimental setups include table-top sources as well as large-scale facilities such as synchrotron sources. At the core of my work lies the development of a linear-chain model to simulate and analyze the photoexcited atomic-scale dynamics. The calculated strain fields are then used to simulate the optical and x-ray response of the considered thin films and multilayers in order to relate the experimental signatures to particular structural processes. This way one obtains insight into the rich lattice dynamics exhibiting coherent transport of vibrational energy from local excitations via delocalized phonon modes of the samples. The complex deformations in tailored multilayers are identified to give rise to highly nonlinear x-ray diffraction responses due to transient interference effects. The understanding of such effects and the ability to precisely calculate those are exploited for the design of novel ultrafast x-ray optics. In particular, I present several Phonon Bragg Switch concepts to efficiently generate ultrashort x-ray pulses for time-resolved structural investigations. By extension of the numerical models to include incoherent phonon propagation and anharmonic lattice potentials I present a new view on the fundamental research topics of nanoscale thermal transport and anharmonic phonon-phonon interactions such as nonlinear sound propagation and phonon damping. The former issue is exemplified by the time-resolved heat conduction from thin SrRuO3 films into a SrTiO3 substrate which exhibits an unexpectedly slow heat conductivity. Furthermore, I discuss various experiments which can be well reproduced by the versatile numerical models and thus evidence strong lattice anharmonicities in the perovskite oxide SrTiO3. The thesis also presents several advances of experimental techniques such as time-resolved phonon spectroscopy with optical and x-ray photons as well as concepts for the implementation of x-ray diffraction setups at standard synchrotron beamlines with largely improved time-resolution for investigations of ultrafast structural processes. This work forms the basis for ongoing research topics in complex oxide materials including electronic correlations and phase transitions related to the elastic, magnetic and polarization degrees of freedom.
In the western hemisphere, the piano is one of the most important instruments. While its evolution lasted for more than three centuries, and the most important physical aspects have already been investigated, some parts in the characterization of the piano remain not well understood. Considering the pivotal piano soundboard, the effect of ribs mounted on the board exerted on the sound radiation and propagation in particular, is mostly neglected in the literature. The present investigation deals exactly with the sound wave propagation effects that emerge in the presence of an array of equally-distant mounted ribs at a soundboard. Solid-state theory proposes particular eigenmodes and -frequencies for such arrangements, which are comparable to single units in a crystal. Following this 'linear chain model' (LCM), differences in the frequency spectrum are observable as a distinct band structure. Also, the amplitudes of the modes are changed, due to differences of the damping factor. These scattering effects were not only investigated for a well-understood conceptional rectangular soundboard (multichord), but also for a genuine piano resonance board manufactured by the piano maker company 'C. Bechstein Pianofortefabrik'. To obtain the possibility to distinguish between the characterizing spectra both with and without mounted ribs, the typical assembly plan for the Bechstein instrument was specially customized. Spectral similarities and differences between both boards are found in terms of damping and tone. Furthermore, specially prepared minimal-invasive piezoelectric polymer sensors made from polyvinylidene fluoride (PVDF) were used to record solid-state vibrations of the investigated system. The essential calibration and characterization of these polymer sensors was performed by determining the electromechanical conversion, which is represented by the piezoelectric coefficient. Therefore, the robust 'sinusoidally varying external force' method was applied, where a dynamic force perpendicular to the sensor's surface, generates movable charge carriers. Crucial parameters were monitored, with the frequency response function as the most important one for acousticians. Along with conventional condenser microphones, the sound was measured as solid-state vibration as well as airborne wave. On this basis, statements can be made about emergence, propagation, and also the overall radiation of the generated modes of the vibrating system. Ultimately, these results acoustically characterize the entire system.
Theory of mRNA degradation
(2012)
One of the central themes of biology is to understand how individual cells achieve a high fidelity in gene expression. Each cell needs to ensure accurate protein levels for its proper functioning and its capability to proliferate. Therefore, complex regulatory mechanisms have evolved in order to render the expression of each gene dependent on the expression level of (all) other genes. Regulation can occur at different stages within the framework of the central dogma of molecular biology. One very effective and relatively direct mechanism concerns the regulation of the stability of mRNAs. All organisms have evolved diverse and powerful mechanisms to achieve this. In order to better comprehend the regulation in living cells, biochemists have studied specific degradation mechanisms in detail. In addition to that, modern high-throughput techniques allow to obtain quantitative data on a global scale by parallel analysis of the decay patterns of many different mRNAs from different genes. In previous studies, the interpretation of these mRNA decay experiments relied on a simple theoretical description based on an exponential decay. However, this does not account for the complexity of the responsible mechanisms and, as a consequence, the exponential decay is often not in agreement with the experimental decay patterns. We have developed an improved and more general theory of mRNA degradation which provides a general framework of mRNA expression and allows describing specific degradation mechanisms. We have made an attempt to provide detailed models for the regulation in different organisms. In the yeast S. cerevisiae, different degradation pathways are known to compete and furthermore most of them rely on the biochemical modification of mRNA molecules. In bacteria such as E. coli, degradation proceeds primarily endonucleolytically, i.e. it is governed by the initial cleavage within the coding region. In addition, it is often coupled to the level of maturity and the size of the polysome of an mRNA. Both for S. cerevisiae and E. coli, our descriptions lead to a considerable improvement of the interpretation of experimental data. The general outcome is that the degradation of mRNA must be described by an age-dependent degradation rate, which can be interpreted as a consequence of molecular aging of mRNAs. Within our theory, we find adequate ways to address this much debated topic from a theoretical perspective. The improvements of the understanding of mRNA degradation can be readily applied to further comprehend the mRNA expression under different internal or environmental conditions such as after the induction of transcription or stress application. Also, the role of mRNA decay can be assessed in the context of translation and protein synthesis. The ultimate goal in understanding gene regulation mediated by mRNA stability will be to identify the relevance and biological function of different mechanisms. Once more quantitative data will become available, our description allows to elaborate the role of each mechanism by devising a suitable model.
Thermal and quantum fluctuations of the electromagnetic near field of atoms and macroscopic bodies play a key role in quantum electrodynamics (QED), as in the Lamb shift. They lead, e.g., to atomic level shifts, dispersion interactions (Van der Waals-Casimir-Polder interactions), and state broadening (Purcell effect) because the field is subject to boundary conditions. Such effects can be observed with high precision on the mesoscopic scale which can be accessed in micro-electro-mechanical systems (MEMS) and solid-state-based magnetic microtraps for cold atoms (‘atom chips’). A quantum field theory of atoms (molecules) and photons is adapted to nonequilibrium situations. Atoms and photons are described as fully quantized while macroscopic bodies can be included in terms of classical reflection amplitudes, similar to the scattering approach of cavity QED. The formalism is applied to the study of nonequilibrium two-body potentials. We then investigate the impact of the material properties of metals on the electromagnetic surface noise, with applications to atomic trapping in atom-chip setups and quantum computing, and on the magnetic dipole contribution to the Van der Waals-Casimir-Polder potential in and out of thermal equilibrium. In both cases, the particular properties of superconductors are of high interest. Surface-mode contributions, which dominate the near-field fluctuations, are discussed in the context of the (partial) dynamic atomic dressing after a rapid change of a system parameter and in the Casimir interaction between two conducting plates, where nonequilibrium configurations can give rise to repulsion.
In the course of this thesis gold nanoparticle/polyelectrolyte multilayer structures were prepared, characterized, and investigated according to their static and ultrafast optical properties. Using the dip-coating or spin-coating layer-by-layer deposition method, gold-nanoparticle layers were embedded in a polyelectrolyte environment with high structural perfection. Typical structures exhibit four repetition units, each consisting of one gold-particle layer and ten double layers of polyelectrolyte (cationic+anionic polyelectrolyte). The structures were characterized by X-ray reflectivity measurements, which reveal Bragg peaks up to the seventh order, evidencing the high stratication of the particle layers. In the same measurements pronounced Kiessig fringes were observed, which indicate a low global roughness of the samples. Atomic force microscopy (AFM) images veried this low roughness, which results from the high smoothing capabilities of polyelectrolyte layers. This smoothing effect facilitates the fabrication of stratified nanoparticle/polyelectrolyte multilayer structures, which were nicely illustrated in a transmission electron microscopy image. The samples' optical properties were investigated by static spectroscopic measurements in the visible and UV range. The measurements revealed a frequency shift of the reflectance and of the plasmon absorption band, depending on the thickness of the polyelectrolyte layers that cover a nanoparticle layer. When the covering layer becomes thicker than the particle interaction range, the absorption spectrum becomes independent of the polymer thickness. However, the reflectance spectrum continues shifting to lower frequencies (even for large thicknesses). The range of plasmon interaction was determined to be in the order of the particle diameter for 10 nm, 20 nm, and 150 nm particles. The transient broadband complex dielectric function of a multilayer structure was determined experimentally by ultrafast pump-probe spectroscopy. This was achieved by simultaneous measurements of the changes in the reflectance and transmittance of the excited sample over a broad spectral range. The changes in the real and imaginary parts of the dielectric function were directly deduced from the measured data by using a recursive formalism based on the Fresnel equations. This method can be applied to a broad range of nanoparticle systems where experimental data on the transient dielectric response are rare. This complete experimental approach serves as a test ground for modeling the dielectric function of a nanoparticle compound structure upon laser excitation.
Tensorial spacetime geometries carrying predictive, interpretable and quantizable matter dynamics
(2012)
Which tensor fields G on a smooth manifold M can serve as a spacetime structure? In the first part of this thesis, it is found that only a severely restricted class of tensor fields can provide classical spacetime geometries, namely those that can carry predictive, interpretable and quantizable matter dynamics. The obvious dependence of this characterization of admissible tensorial spacetime geometries on specific matter is not a weakness, but rather presents an insight: it was Maxwell theory that justified Einstein to promote Lorentzian manifolds to the status of a spacetime geometry. Any matter that does not mimick the structure of Maxwell theory, will force us to choose another geometry on which the matter dynamics of interest are predictive, interpretable and quantizable. These three physical conditions on matter impose three corresponding algebraic conditions on the totally symmetric contravariant coefficient tensor field P that determines the principal symbol of the matter field equations in terms of the geometric tensor G: the tensor field P must be hyperbolic, time-orientable and energy-distinguishing. Remarkably, these physically necessary conditions on the geometry are mathematically already sufficient to realize all kinematical constructions familiar from Lorentzian geometry, for precisely the same structural reasons. This we were able to show employing a subtle interplay of convex analysis, the theory of partial differential equations and real algebraic geometry. In the second part of this thesis, we then explore general properties of any hyperbolic, time-orientable and energy-distinguishing tensorial geometry. Physically most important are the construction of freely falling non-rotating laboratories, the appearance of admissible modified dispersion relations to particular observers, and the identification of a mechanism that explains why massive particles that are faster than some massless particles can radiate off energy until they are slower than all massless particles in any hyperbolic, time-orientable and energy-distinguishing geometry. In the third part of the thesis, we explore how tensorial spacetime geometries fare when one wants to quantize particles and fields on them. This study is motivated, in part, in order to provide the tools to calculate the rate at which superluminal particles radiate off energy to become infraluminal, as explained above. Remarkably, it is again the three geometric conditions of hyperbolicity, time-orientability and energy-distinguishability that allow the quantization of general linear electrodynamics on an area metric spacetime and the quantization of massive point particles obeying any admissible dispersion relation. We explore the issue of field equations of all possible derivative order in rather systematic fashion, and prove a practically most useful theorem that determines Dirac algebras allowing the reduction of derivative orders. The final part of the thesis presents the sketch of a truly remarkable result that was obtained building on the work of the present thesis. Particularly based on the subtle duality maps between momenta and velocities in general tensorial spacetimes, it could be shown that gravitational dynamics for hyperbolic, time-orientable and energy distinguishable geometries need not be postulated, but the formidable physical problem of their construction can be reduced to a mere mathematical task: the solution of a system of homogeneous linear partial differential equations. This far-reaching physical result on modified gravity theories is a direct, but difficult to derive, outcome of the findings in the present thesis. Throughout the thesis, the abstract theory is illustrated through instructive examples.
Particles in Saturn’s main rings range in size from dust to even kilometer-sized objects. Their size distribution is thought to be a result of competing accretion and fragmentation processes. While growth is naturally limited in tidal environments, frequent collisions among these objects may contribute to both accretion and fragmentation. As ring particles are primarily made of water ice attractive surface forces like adhesion could significantly influence these processes, finally determining the resulting size distribution. Here, we derive analytic expressions for the specific self-energy Q and related specific break-up energy Q⋆ of aggregates. These expressions can be used for any aggregate type composed of monomeric constituents. We compare these expressions to numerical experiments where we create aggregates of various types including: regular packings like the face-centered cubic (fcc), Ballistic Particle Cluster Aggregates (BPCA), and modified BPCAs including e.g. different constituent size distributions. We show that accounting for attractive surface forces such as adhesion a simple approach is able to: a) generally account for the size dependence of the specific break-up energy for fragmentation to occur reported in the literature, namely the division into “strength” and “gravity” regimes, and b) estimate the maximum aggregate size in a collisional ensemble to be on the order of a few meters, consistent with the maximum aggregate size observed in Saturn’s rings of about 10m.
One of the most exciting predictions of Einstein's theory of gravitation that have not yet been proven experimentally by a direct detection are gravitational waves. These are tiny distortions of the spacetime itself, and a world-wide effort to directly measure them for the first time with a network of large-scale laser interferometers is currently ongoing and expected to provide positive results within this decade. One potential source of measurable gravitational waves is the inspiral and merger of two compact objects, such as binary black holes. Successfully finding their signature in the noise-dominated data of the detectors crucially relies on accurate predictions of what we are looking for. In this thesis, we present a detailed study of how the most complete waveform templates can be constructed by combining the results from (A) analytical expansions within the post-Newtonian framework and (B) numerical simulations of the full relativistic dynamics. We analyze various strategies to construct complete hybrid waveforms that consist of a post-Newtonian inspiral part matched to numerical-relativity data. We elaborate on exsisting approaches for nonspinning systems by extending the accessible parameter space and introducing an alternative scheme based in the Fourier domain. Our methods can now be readily applied to multiple spherical-harmonic modes and precessing systems. In addition to that, we analyze in detail the accuracy of hybrid waveforms with the goal to quantify how numerous sources of error in the approximation techniques affect the application of such templates in real gravitational-wave searches. This is of major importance for the future construction of improved models, but also for the correct interpretation of gravitational-wave observations that are made utilizing any complete waveform family. In particular, we comprehensively discuss how long the numerical-relativity contribution to the signal has to be in order to make the resulting hybrids accurate enough, and for currently feasible simulation lengths we assess the physics one can potentially do with template-based searches.
Cargo transport by molecular motors is ubiquitous in all eukaryotic cells and is typically driven cooperatively by several molecular motors, which may belong to one or several motor species like kinesin, dynein or myosin. These motor proteins transport cargos such as RNAs, protein complexes or organelles along filaments, from which they unbind after a finite run length. Understanding how these motors interact and how their movements are coordinated and regulated is a central and challenging problem in studies of intracellular transport. In this thesis, we describe a general theoretical framework for the analysis of such transport processes, which enables us to explain the behavior of intracellular cargos based on the transport properties of individual motors and their interactions. Motivated by recent in vitro experiments, we address two different modes of transport: unidirectional transport by two identical motors and cooperative transport by actively walking and passively diffusing motors. The case of cargo transport by two identical motors involves an elastic coupling between the motors that can reduce the motors’ velocity and/or the binding time to the filament. We show that this elastic coupling leads, in general, to four distinct transport regimes. In addition to a weak coupling regime, kinesin and dynein motors are found to exhibit a strong coupling and an enhanced unbinding regime, whereas myosin motors are predicted to attain a reduced velocity regime. All of these regimes, which we derive both by analytical calculations and by general time scale arguments, can be explored experimentally by varying the elastic coupling strength. In addition, using the time scale arguments, we explain why previous studies came to different conclusions about the effect and relevance of motor-motor interference. In this way, our theory provides a general and unifying framework for understanding the dynamical behavior of two elastically coupled molecular motors. The second mode of transport studied in this thesis is cargo transport by actively pulling and passively diffusing motors. Although these passive motors do not participate in active transport, they strongly enhance the overall cargo run length. When an active motor unbinds, the cargo is still tethered to the filament by the passive motors, giving the unbound motor the chance to rebind and continue its active walk. We develop a stochastic description for such cooperative behavior and explicitly derive the enhanced run length for a cargo transported by one actively pulling and one passively diffusing motor. We generalize our description to the case of several pulling and diffusing motors and find an exponential increase of the run length with the number of involved motors.
Eumelanin ist ein Fluorophor mit teilweise recht ungewöhnlichen spektralen Eigenschaften. Unter anderem konnten in früheren Veröffentlichungen Unterschiede zwischen dem 1- und 2-photonen-angeregtem Fluoreszenzspektrum beobachtet werden, weshalb im nichtlinearen Anregungsfall ein schrittweiser Anregungsprozess vermutet wurde. Um diese und weitere optische Eigenschaften des Eumelanins besser zu verstehen, wurden in der vorliegenden Arbeit vielfältige messmethodische Ansätze der linearen und nichtlinearen Optik an synthetischem Eumelanin in 0,1M NaOH verfolgt. Aus den Ergebnissen wurde ein Modell abgeleitet, welches die beobachteten photonischen Eigenschaften konsistent beschreibt. In diesem kaskadierten Zustandsmodell (Kaskaden-Modell) wird die aufgenommene Photonenenergie schrittweise von Anregungszuständen hoher Übergangsenergien zu Anregungszuständen niedrigerer Übergangsenergien transferiert. Messungen der transienten Absorption ergaben dominante Anteile mit kurzen Lebensdauern im ps-Bereich und ließen damit auf eine hohe Relaxationsgeschwindigkeit entlang der Kaskade schließen. Durch Untersuchung der nichtlinear angeregten Fluoreszenz von verschieden großen Eumelanin-Aggregaten konnte gezeigt werden, dass Unterschiede zwischen dem linear und nichtlinear angeregten Fluoreszenzspektrum nicht nur durch einen schrittweisen Anregungsprozess bei nichtlinearer Anregung sondern auch durch Unterschiede in den Verhältnissen der Quantenausbeuten zwischen kleinen und großen Aggregaten beim Wechsel von linearer zu nichtlinearer Anregung begründet sein können. Durch Bestimmung des Anregungswirkungsquerschnitts und der Anregungspulsdauer-Abhängigkeit der nichtlinear angeregten Fluoreszenz von Eumelanin konnte jedoch ein schrittweiser 2-Photonen-Anregungsprozess über einen Zwischenzustand mit Lebendsdauern im ps-Bereich nachgewiesen werden.
A key non-destructive technique for analysis, optimization and developing of new functional materials such as sensors, transducers, electro-optical and memory devices is presented. The Thermal-Pulse Tomography (TPT) provides high-resolution three-dimensional images of electric field and polarization distribution in a material. This thermal technique use a pulsed heating by means of focused laser light which is absorbed by opaque electrodes. The diffusion of the heat causes changes in the sample geometry, generating a short-circuit current or change in surface potential, which contains information about the spatial distribution of electric dipoles or space charges. Afterwards, a reconstruction of the internal electric field and polarization distribution in the material is possible via Scale Transformation or Regularization methods. In this way, the TPT was used for the first time to image the inhomogeneous ferroelectric switching in polymer ferroelectric films (candidates to memory devices). The results shows the typical pinning of electric dipoles in the ferroelectric polymer under study and support the previous hypotheses of a ferroelectric reversal at a grain level via nucleation and growth. In order to obtain more information about the impact of the lateral and depth resolution of the thermal techniques, the TPT and its counterpart called Focused Laser Intensity Modulation Method (FLIMM) were implemented in ferroelectric films with grid-shaped electrodes. The results from both techniques, after the data analysis with different regularization and scale methods, are in total agreement. It was also revealed a possible overestimated lateral resolution of the FLIMM and highlights the TPT method as the most efficient and reliable thermal technique. After an improvement in the optics, the Thermal-Pulse Tomography method was implemented in polymer-dispersed liquid crystals (PDLCs) films, which are used in electro-optical applications. The results indicated a possible electrostatic interaction between the COH group in the liquid crystals and the fluorinate atoms of the used ferroelectric matrix. The geometrical parameters of the LC droplets were partially reproduced as they were compared with Scanning Electron Microscopy (SEM) images. For further applications, it is suggested the use of a non-strong-ferroelectric polymer matrix. In an effort to develop new polymerferroelectrets and for optimizing their properties, new multilayer systems were inspected. The results of the TPT method showed the non-uniformity of the internal electric-field distribution in the shaped-macrodipoles and thus suggested the instability of the sample. Further investigation on multilayers ferroelectrets was suggested and the implementation of less conductive polymers layers too.