Institut für Physik und Astronomie
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Based on extensive Monte Carlo simulations and analytical considerations we study the electrostatically driven adsorption of flexible polyelectrolyte chains onto charged Janus nanospheres. These net-neutral colloids are composed of two equally but oppositely charged hemispheres. The critical binding conditions for polyelectrolyte chains are analysed as function of the radius of the Janus particle and its surface charge density, as well as the salt concentration in the ambient solution. Specifically for the adsorption of finite-length polyelectrolyte chains onto Janus nanoparticles, we demonstrate that the critical adsorption conditions drastically differ when the size of the Janus particle or the screening length of the electrolyte are varied. We compare the scaling laws obtained for the adsorption–desorption threshold to the known results for uniformly charged spherical particles, observing significant disparities. We also contrast the changes to the polyelectrolyte chain conformations close to the surface of the Janus nanoparticles as compared to those for simple spherical particles. Finally, we discuss experimentally relevant physico-chemical systems for which our simulations results may become important. In particular, we observe similar trends with polyelectrolyte complexation with oppositely but heterogeneously charged proteins.
Herein, we report the chain-growth tin-free room temperature polymerization method to synthesize n-type perylene diimide-dithiophene-based conjugated polymers (PPDIT2s) suitable for solar cell and transistor applications. The palladium/electron-rich tri-tert-butylphosphine catalyst is effective to enable the chain-growth polymerization of anion-radical monomer Br-TPDIT-Br/Zn to PPDIT2 with a molecular weight up to Mw ≈ 50 kg mol−1 and moderate polydispersity. This is the second example of the polymerization of unusual anion-radical aromatic complexes formed in a reaction of active Zn and electron-deficient diimide-based aryl halides. As such, the discovered polymerization method is not a specific reactivity feature of the naphthalene-diimide derivatives but is rather a general polymerization tool. This is an important finding, given the significantly higher maximum external quantum efficiency that can be reached with PDI-based copolymers (32–45%) in all-polymer solar cells compared to NDI-based materials (15–30%). Our studies revealed that PPDIT2 synthesized by the new method and the previously published polymer prepared by step-growth Stille polycondensation show similar electron mobility and all-polymer solar cell performance. At the same time, the polymerization reported herein has several technological advantages as it proceeds relatively fast at room temperature and does not involve toxic tin-based compounds. Because several chain-growth polymerization reactions are well-suited for the preparation of well-defined multi-functional polymer architectures, the next target is to explore the utility of the discovered polymerization in the synthesis of end-functionalized polymers and block copolymers. Such materials would be helpful to improve the nanoscale morphology of polymer blends in all-polymer solar cells.
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.
It is generally agreed upon that stars typically form in open clusters and stellar associations, but little is known about the structure of the open cluster system. Do open clusters and stellar associations form isolated or do they prefer to form in groups and complexes? Open cluster groups and complexes could verify star forming regions to be larger than expected, which would explain the chemical homogeneity over large areas in the Galactic disk. They would also define an additional level in the hierarchy of star formation and could be used as tracers for the scales of fragmentation in giant molecular clouds? Furthermore, open cluster groups and complexes could affect Galactic dynamics and should be considered in investigations and simulations on the dynamical processes, such as radial migration, disc heating, differential rotation, kinematic resonances, and spiral structure.
In the past decade there were a few studies on open cluster pairs (de La Fuente Marcos & de La Fuente Marcos 2009a,b,c) and on open cluster groups and complexes (Piskunov et al. 2006). The former only considered spatial proximity for the identification of the pairs, while the latter also required tangential velocities to be similar for the members. In this work I used the full set of 6D phase-space information to draw a more detailed picture on these structures. For this purpose I utilised the most homogeneous cluster catalogue available, namely the Catalogue of Open Cluster Data (COCD; Kharchenko et al. 2005a,b), which contains parameters for 650 open clusters and compact associations, as well as for their uniformly selected members. Additional radial velocity (RV) and metallicity ([M/H]) information on the members were obtained from the RAdial Velocity Experiment (RAVE; Steinmetz et al. 2006; Kordopatis et al. 2013) for 110 and 81 clusters, respectively. The RAVE sample was cleaned considering quality parameters and flags provided by RAVE (Matijevič et al. 2012; Kordopatis et al. 2013). To ensure that only real members were included for the mean values, also the cluster membership, as provided by Kharchenko et al. (2005a,b), was considered for the stars cross-matched in RAVE.
6D phase-space information could be derived for 432 out of the 650 COCD objects and I used an adaption of the Friends-of-Friends algorithm, as used in cosmology, to identify potential groupings. The vast majority of the 19 identified groupings were pairs, but I also found four groups of 4-5 members and one complex with 15 members. For the verification of the identified structures, I compared the results to a randomly selected subsample of the catalogue for the Milky Way global survey of Star Clusters (MWSC; Kharchenko et al. 2013), which became available recently, and was used as reference sample. Furthermore, I implemented Monte-Carlo simulations with randomised samples created from two distinguished input distributions for the spatial and velocity parameters. On the one hand, assuming a uniform distribution in the Galactic disc and, on the other hand, assuming the COCD data distributions to be representative for the whole open cluster population.
The results suggested that the majority of identified pairs are rather by chance alignments, but the groups and the complex seemed to be genuine. A comparison of my results to the pairs, groups and complexes proposed in the literature yielded a partial overlap, which was most likely because of selection effects and different parameters considered. This is another verification for the existence of such structures.
The characteristics of the found groupings favour that members of an open cluster grouping originate from a common giant molecular cloud and formed in a single, but possibly sequential, star formation event. Moreover, the fact that the young open cluster population showed smaller spatial separations between nearest neighbours than the old cluster population indicated that the lifetime of open cluster groupings is most likely comparable to that of the Galactic open cluster population itself. Still even among the old open clusters I could identify groupings, which suggested that the detected structure could be in some cases more long lived as one might think.
In this thesis I could only present a pilot study on structures in the Galactic open cluster population, since the data sample used was highly incomplete. For further investigations a far more complete sample would be required. One step in this direction would be to use data from large current surveys, like SDSS, RAVE, Gaia-ESO and VVV, as well as including results from studies on individual clusters. Later the sample can be completed by data from upcoming missions, like Gaia and 4MOST. Future studies using this more complete open cluster sample will reveal the effect of open cluster groupings on star formation theory and their significance for the kinematics, dynamics and evolution of the Milky Way, and thereby of spiral galaxies.
The Epoch of Reionization marks after recombination the second major change in the ionization state of the universe, going from a neutral to an ionized state. It starts with the appearance of the first stars and galaxies; a fraction of high-energy photons emitted from galaxies permeate into the intergalactic medium (IGM) and gradually ionize the hydrogen, until the IGM is completely ionized at z~6 (Fan et al., 2006). While the progress of reionization is driven by galaxy evolution, it changes the ionization and thermal state of the IGM substantially and affects subsequent structure and galaxy formation by various feedback mechanisms.
Understanding this interaction between reionization and galaxy formation is further impeded by a lack of understanding of the high-redshift galactic properties such as the dust distribution and the escape fraction of ionizing photons. Lyman Alpha Emitters (LAEs) represent a sample of high-redshift galaxies that are sensitive to all these galactic properties and the effects of reionization.
In this thesis we aim to understand the progress of reionization by performing cosmological simulations, which allows us to investigate the limits of constraining reionization by high-redshift galaxies as LAEs, and examine how galactic properties and the ionization state of the IGM affect the visibility and observed quantities of LAEs and Lyman Break galaxies (LBGs).
In the first part of this thesis we focus on performing radiative transfer calculations to simulate reionization. We have developed a mapping-sphere-scheme, which, starting from spherically averaged temperature and density fields, uses our 1D radiative transfer code and computes the effect of each source on the IGM temperature and ionization (HII, HeII, HeIII) profiles, which are subsequently mapped onto a grid. Furthermore we have updated the 3D Monte-Carlo radiative transfer pCRASH, enabling detailed reionization simulations which take individual source characteristics into account.
In the second part of this thesis we perform a reionization simulation by post-processing a smoothed-particle hydrodynamical (SPH) simulation (GADGET-2) with 3D radiative transfer (pCRASH), where the ionizing sources are modelled according to the characteristics of the stellar populations in the hydrodynamical simulation. Following the ionization fractions of hydrogen (HI) and helium (HeII, HeIII), and temperature in our simulation, we find that reionization starts at z~11 and ends at z~6, and high density regions near sources are ionized earlier than low density regions far from sources.
In the third part of this thesis we couple the cosmological SPH simulation and the radiative transfer simulations with a physically motivated, self-consistent model for LAEs, in order to understand the importance of the ionization state of the IGM, the escape fraction of ionizing photons from galaxies and dust in the interstellar medium (ISM) on the visibility of LAEs. Comparison of our models results with the LAE Lyman Alpha (Lya) and UV luminosity functions at z~6.6 reveals a three-dimensional degeneracy between the ionization state of the IGM, the ionizing photons escape fraction and the ISM dust distribution, which implies that LAEs act not only as tracers of reionization but also of the ionizing photon escape fraction and of the ISM dust distribution. This degeneracy does not even break down when we compare simulated with observed clustering of LAEs at z~6.6. However, our results show that reionization has the largest impact on the amplitude of the LAE angular correlation functions, and its imprints are clearly distinguishable from those of properties on galactic scales. These results show that reionization cannot be constrained tightly by exclusively using LAE observations. Further observational constraints, e.g. tomographies of the redshifted hydrogen 21cm line, are required.
In addition we also use our LAE model to probe the question when a galaxy is visible as a LAE or a LBG. Within our model galaxies above a critical stellar mass can produce enough luminosity to be visible as a LBG and/or a LAE. By finding an increasing duty cycle of LBGs with Lya emission as the UV magnitude or stellar mass of the galaxy rises, our model reveals that the brightest (and most massive) LBGs most often show Lya emission.
Predicting the Lya equivalent width (Lya EW) distribution and the fraction of LBGs showing Lya emission at z~6.6, we reproduce the observational trend of the Lya EWs with UV magnitude. However, the Lya EWs of the UV brightest LBGs exceed observations and can only be reconciled by accounting for an increased Lya attenuation of massive galaxies, which implies that the observed Lya brightest LAEs do not necessarily coincide with the UV brightest galaxies. We have analysed the dependencies of LAE observables on the properties of the galactic and intergalactic medium and the LAE-LBG connection, and this enhances our understanding of the nature of LAEs.
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.
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].
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.