530 Physik
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- generalised langevin equation (2)
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- non-Gaussianity (2)
- non-Langevin recombination (2)
- non-destructive evaluation (2)
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- Überschwemmungen (2)
- 'Reduced-Form' Modellierung (1)
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Institute
- Institut für Physik und Astronomie (1486) (remove)
We study the adsorption–desorption transition of polyelectrolyte chains onto planar, cylindrical and spherical surfaces with arbitrarily high surface charge densities by massive Monte Carlo computer simulations. We examine in detail how the well known scaling relations for the threshold transition—demarcating the adsorbed and desorbed domains of a polyelectrolyte near weakly charged surfaces—are altered for highly charged interfaces. In virtue of high surface potentials and large surface charge densities, the Debye–Hückel approximation is often not feasible and the nonlinear Poisson–Boltzmann approach should be implemented. At low salt conditions, for instance, the electrostatic potential from the nonlinear Poisson–Boltzmann equation is smaller than the Debye–Hückel result, such that the required critical surface charge density for polyelectrolyte adsorption σc increases. The nonlinear relation between the surface charge density and electrostatic potential leads to a sharply increasing critical surface charge density with growing ionic strength, imposing an additional limit to the critical salt concentration above which no polyelectrolyte adsorption occurs at all. We contrast our simulations findings with the known scaling results for weak critical polyelectrolyte adsorption onto oppositely charged surfaces for the three standard geometries. Finally, we discuss some applications of our results for some physical–chemical and biophysical systems.
We study the adsorption–desorption transition of polyelectrolyte chains onto planar, cylindrical and spherical surfaces with arbitrarily high surface charge densities by massive Monte Carlo computer simulations. We examine in detail how the well known scaling relations for the threshold transition—demarcating the adsorbed and desorbed domains of a polyelectrolyte near weakly charged surfaces—are altered for highly charged interfaces. In virtue of high surface potentials and large surface charge densities, the Debye–Hückel approximation is often not feasible and the nonlinear Poisson–Boltzmann approach should be implemented. At low salt conditions, for instance, the electrostatic potential from the nonlinear Poisson–Boltzmann equation is smaller than the Debye–Hückel result, such that the required critical surface charge density for polyelectrolyte adsorption σc increases. The nonlinear relation between the surface charge density and electrostatic potential leads to a sharply increasing critical surface charge density with growing ionic strength, imposing an additional limit to the critical salt concentration above which no polyelectrolyte adsorption occurs at all. We contrast our simulations findings with the known scaling results for weak critical polyelectrolyte adsorption onto oppositely charged surfaces for the three standard geometries. Finally, we discuss some applications of our results for some physical–chemical and biophysical systems.
Employing extensive Monte Carlo computer simulations, we investigate in detail the properties of multichain adsorption of charged flexible polyelectrolytes (PEs) onto oppositely charged spherical nanoparticles (SNPs). We quantify the conditions of critical adsorption-the phase-separation curve between the adsorbed and desorbed states of the PEs-as a function of the SNP surface-charge density and the concentration of added salt. We study the degree of fluctuations of the PE-SNP electrostatic binding energy, which we use to quantify the emergence of the phase subtransitions, including a series of partially adsorbed PE configurations. We demonstrate how the phase-separation adsorption-desorption boundary shifts and splits into multiple subtransitions at low-salt conditions, thereby generalizing and extending the results for critical adsorption of a single PE onto the SNP. The current findings are relevant for finite concentrations of PEs around the attracting SNP, such as the conditions for PE adsorption onto globular proteins carrying opposite electric charges.
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.
Charge-density rearrangements after metal-to-ligand charge-transfer excitation in an iron photosensitizer are investigated by R. M Jay, A. Fohlisch et al. in their Communication (DOI: 10.1002/anie.201904761). By using time-resolved X-ray absorption spectroscopy, surprising covalency-effects are revealed that inhibit charge-separation at the intra-molecular level. Furthermore, the underlying mechanism is proposed to be generally in effect for all commonly used photosensitizers in light-harvesting applications, which challenges the common perception of electronic charge-transfer.
Coupling of the electrical, mechanical and optical response in polymer/liquid-crystal composites
(2010)
Micrometer-sized liquid-crystal (LC) droplets embedded in a polymer matrix may enable optical switching in the composite film through the alignment of the LC director along an external electric field. When a ferroelectric material is used as host polymer, the electric field generated by the piezoelectric effect can orient the director of the LC under an applied mechanical stress, making these materials interesting candidates for piezo-optical devices. In this work, polymer-dispersed liquid crystals (PDLCs) are prepared from poly(vinylidene fluoride-trifluoroethylene) (P(VDF-TrFE)) and a nematic liquid crystal (LC). The anchoring effect is studied by means of dielectric relaxation spectroscopy. Two dispersion regions are observed in the dielectric spectra of the pure P(VDF-TrFE) film. They are related to the glass transition and to a charge-carrier relaxation, respectively. In PDLC films containing 10 and 60 wt% LC, an additional, bias-field-dependent relaxation peak is found that can be attributed to the motion of LC molecules. Due to the anchoring effect of the LC molecules, this relaxation process is slowed down considerably, when compared with the related process in the pure LC. The electro-optical and piezo-optical behavior of PDLC films containing 10 and 60 wt% LCs is investigated. In addition to the refractive-index mismatch between the polymer matrix and the LC molecules, the interaction between the polymer dipoles and the LC molecules at the droplet interface influences the light-scattering behavior of the PDLC films. For the first time, it was shown that the electric field generated by the application of a mechanical stress may lead to changes in the transmittance of a PDLC film. Such a piezo-optical PDLC material may be useful e.g. in sensing and visualization applications. Compared to a non-polar matrix polymer, the polar matrix polymer exhibits a strong interaction with the LC molecules at the polymer/LC interface which affects the electro-optical effect of the PDLC films and prevents a larger increase in optical transmission.
Motivated by recent proposals on the experimental detectability of quantum gravity effects, the present thesis investigates assumptions and methods which might be used for the prediction of such effects within the framework of loop quantum gravity. To this end, a scalar field coupled to gravity is considered as a model system. Starting from certain assumptions about the dynamics of the coupled gravity-matter system, a quantum theory for the scalar field is proposed. Then, assuming that the gravitational field is in a semiclassical state, a "QFT on curved space-time limit" of this theory is defined. In contrast to ordinary quantum field theory on curved space-time however, in this limit the theory describes a quantum scalar field propagating on a (classical) random lattice. Then, methods to obtain the low energy limit of such a lattice theory, especially regarding the resulting modified dispersion relations, are discussed and applied to simple model systems. Finally, under certain simplifying assumptions, using the methods developed before as well as a specific class of semiclassical states, corrections to the dispersion relations for the scalar and the electromagnetic field are computed within the framework of loop quantum gravity. These calculations are of preliminary character, as many assumptions enter whose validity remains to be studied more thoroughly. However they exemplify the problems and possibilities of making predictions based on loop quantum gravity that are in principle testable by experiment.
Aims. To gain a realistic picture of the donor star in Vela X-1, we constructed a hydrodynamically consistent atmosphere model describing the wind stratification while properly reproducing the observed donor spectrum. To investigate how X-ray illumination affects the stellar wind, we calculated additional models for different X-ray luminosity regimes. Methods. We used the recently updated version of the Potsdam Wolf-Rayet code to consistently solve the hydrodynamic equation together with the statistical equations and the radiative transfer. Results. The wind flow in Vela X-1 is driven by ions from various elements, with Fe III and S III leading in the outer wind. The model-predicted mass-loss rate is in line with earlier empirical studies. The mass-loss rate is almost unaffected by the presence of the accreting NS in the wind. The terminal wind velocity is confirmed at u(infinity) approximate to 600 km s(-1). On the other hand, the wind velocity in the inner region where the NS is located is only approximate to 100 km s(-1), which is not expected on the basis of a standard beta-velocity law. In models with an enhanced level of X-rays, the velocity field in the outer wind can be altered. If the X-ray flux is too high, the acceleration breaks down because the ionization increases. Conclusions. Accounting for radiation hydrodynamics, our Vela X-1 donor atmosphere model reveals a low wind speed at the NS location, and it provides quantitative information on wind driving in this important HMXB.
Modelling of an open quantum system requires knowledge of parameters that specify how it couples to its environment. However, beyond relaxation rates, realistic parameters for specific environments and materials are rarely known. Here we present a method of inferring the coupling between a generic system and its bosonic (e.g., phononic) environment from the experimentally measurable density of states (DOS). With it we confirm that the DOS of the well-known Debye model for three-dimensional solids is physically equivalent to choosing an Ohmic bath. We further match a real phonon DOS to a series of Lorentzian coupling functions, allowing us to determine coupling parameters for gold, yttrium iron garnet (YIG) and iron as examples. The results illustrate how to obtain material-specific dynamical properties, such as memory kernels. The proposed method opens the door to more accurate modelling of relaxation dynamics, for example for phonon-dominated spin damping in magnetic materials.
We propose Mobius maps as a tool to model synchronization phenomena in coupled phase oscillators. Not only does the map provide fast computation of phase synchronization, it also reflects the underlying group structure of the sinusoidally coupled continuous phase dynamics. We study map versions of various known continuous-time collective dynamics, such as the synchronization transition in the Kuramoto-Sakaguchi model of nonidentical oscillators, chimeras in two coupled populations of identical phase oscillators, and Kuramoto-Battogtokh chimeras on a ring, and demonstrate similarities and differences between the iterated map models and their known continuous-time counterparts.
Many solar wind observations at 1 au indicate that the proton (as well as electron) temperature anisotropy is limited. The data distribution in the (A(a), beta(a),(parallel to))-plane have a rhombic-shaped form around beta(a),(parallel to) similar to 1. The boundaries of the temperature anisotropy at beta(a),(parallel to) > 1 can be well explained by the threshold conditions of the mirror (whistler) and oblique proton (electron) firehose instabilities in a bi-Maxwellian plasma, whereas the physical mechanism of the similar restriction at beta(a),(parallel to) < 1 is still under debate. One possible option is Coulomb collisions, which we revisit in the current work. We derive the relaxation rate nu(A)(aa) of the temperature anisotropy in a bi-Maxwellian plasma that we then study analytically and by observed proton data from WIND. We found that nu(A)(pp) increases toward small beta(p),(parallel to) < 1. We matched the data distribution in the (A(p), beta(p),(parallel to))-plane with the constant contour nu(A)(pp) = 2.8 . 10(-6) s(-1), corresponding to the minimum value for collisions to play a role. This contour fits rather well the left boundary of the rhombic-shaped data distribution in the (A(p), beta(p),(parallel to))-plane. Thus, Coulomb collisions are an interesting candidate for explaining the limitations of the temperature anisotropy in the solar wind with small beta(a),(parallel to) < 1 at 1 au.
In this thesis the gravitational lensing effect is used to explore a number of cosmological topics. We determine the time delay in the gravitationally lensed quasar system HE1104-1805 using different techniques. We obtain a time delay Delta_t(A-B) Delta_t(A-B) =-310 +- 20 days (2 sigma errors) between the two components. We also study the double quasar Q0957+561 during a three years monitoring campaign. The fluctuations we find in the difference light curves are completely consistent with noise and no microlensing is needed to explain these fluctuations. Microlensing is also studied in the quadruple quasar Q2237+0305 during the GLITP collaboration (Oct.1999-Feb.2000). We use the absence of a strong microlensing signal to obtain an upper limit of v=600 km/s for the effective transverse velocity of the lens galaxy (considering microlenses with 0.1 solar masses). The distribution of dark matter in galaxy clusters is also studied in the second part of the thesis. In the cluster of galaxies Cl0024+1654 we obtain a mass-to-light ratio of M/L = 200 M_sun/L_sun (within a radius of 3 arcminutes). In the galaxy cluster RBS380 we find a relatively low X-ray luminosity for a massive cluster of L =2*10^(44) erg/s, but a rich distribution of galaxies in the optical band.
In this thesis we use the gravitational lensing effect as a tool to tackle two rather different cosmological topics: the nature of the dark matter in galaxy halos, and the rotation of the universe. Firstly, we study the microlensing effect in the gravitational lens systems Q0957+561 and Q2237+0305. In these systems the light from the quasar shines directly through the lensing galaxy. Due to the relative motion of the quasar, the lensing galaxy, and the observer compact objects in the galaxy or galaxy halo cause brightness fluctuations of the light from the background quasar. We compare light curve data from a monitoring program of the double quasar Q0957+561 at the 3.5m telescope at Apache Point Observatory from 1995 to 1998 (Colley, Kundic & Turner 2000) with numerical simulations to test whether the halo of the lensing galaxy consists of massive compact objects (MACHOs). This test was first proposed by Gott (1981). We can exclude MACHO masses from 10^-6 M_sun up to 10^-2 M_sun for quasar sizes of less than 3x10^14 h_60^-0.5 cm if the MACHOs make up at least 50% of the dark halo. Secondly, we present new light curve data for the gravitationally lensed quadruple quasar Q2237+0305 taken at the 3.5m telescope at Apache Point Observatory from June 1995 to January 1998. Although the images were taken under variable, often poor seeing conditions and with coarse pixel sampling, photometry is possible for the two brighter quasar images A and B with the help from HST observations. We find independent evidence for a brightness peak in image A of 0.4 to 0.5 mag with a duration of at least 100 days, which indicates that microlensing has taken place in the lensing galaxy. Finally, we use the weak gravitational lensing effect to put limits on a class of Goedel-type rotating cosmologies described by Korotky & Obukhov (1996). In weak lensing studies the shapes of thousands of background galaxies are measured and averaged to reveal coherent gravitational distortions of the galaxy shapes by foreground matter distributions, or by the large-scale structure of space-time itself. We calculate the predicted shear as a function of redshift in Goedel-type rotating cosmologies and compare this to the upper limit on cosmic shear gamma_limit of approximately 0.04 from weak lensing studies. We find that Goedel-type models cannot have larger rotations omega than H_0=6.1x10^-11 h_60/year if this shear limit is valid for the whole sky.
A comprehensive analysis of the variable temporal and spatial responses of tropical-subtropical high-altitude glaciers to climate change is critical for successful model predictions and environmental risk assessment in the Himalayan-Tibetan orogen. High-frequency Holocene glacier chronostratigraphies are therefore reconstructed in 79 glaciated valleys across the orogen using 519 published and 16 new terrestrial cosmogenic 10Be exposure age dataset. Published 10Be ages are compiled only for moraine boulders (excluding bedrock ages). These ages are recalculated using the latest ICE-D production rate calibration database and the scaling scheme models. Outliers for the individual moraine are detected using the Chauvenet's criterion. In addition, past equilibrium-line altitudes (ELAs) are determined using the area-altitude (AA), area accumulation ratio (AAR), and toe-headwall accumulation ratio (THAR) methods for each glacier advance. The modern maximum elevations of lateral moraines (MELM) are also used to estimate modern ELAs and as an independent check on mean ELAs derived using the above three methods. These data may serve as an essential archive for future studies focusing on the cryospheric and environmental changes in the Himalayan-Tibetan orogen. A more comprehensive analysis of the published and new 10Be ages and ELA results and a list of references are presented in Saha et al. (2019, High-frequency Holocene glacier fluctuations in the Himalayan-Tibetan orogen. Quaternary Science Reviews, 220, 372–400).
This paper studies cosmic-ray (CR) transport in magnetohydrodynamic (MHD) turbulence. CR transport is strongly dependent on the properties of the magnetic turbulence.
We perform test particle simulations to study the interactions of CR with both total MHD turbulence and decomposed MHD modes.
The spatial diffusion coefficients and the pitch angle scattering diffusion coefficients are calculated from the test particle trajectories in turbulence.
Our results confirm that the fast modes dominate the CR propagation, whereas Alfven and slow modes are much less efficient and have shown similar pitch-angle scattering rates.
We investigate the cross field transport on large and small scales. On large/global scales, normal diffusion is observed and the diffusion coefficient is suppressed by M-A(zeta) compared to the parallel diffusion coefficients, with zeta closer to 4 in Alfven modes than that in total turbulence, as theoretically expected.
For the CR transport on scales smaller than the turbulence injection scale, both the local and global magnetic reference frames are adopted. Superdiffusion is observed on such small scales in all the cases. Particularly, CR transport in Alfven modes show clear Richardson diffusion in the local reference frame. The diffusion transitions smoothly from the Richardson's one with index 1.5 to normal diffusion as the particle mean free path decreases from lambda(parallel to) >> L to lambda(parallel to) << L, where L is the injection/coherence length of turbulence.
Our results have broad applications to CRs in various astrophysical environments.
The origin and structure of magnetic fields in the Galaxy are largely unknown. What is known is that they are essential for several astrophysical processes, in particular the propagation of cosmic rays. Our ability to describe the propagation of cosmic rays through the Galaxy is severely limited by the lack of observational data needed to probe the structure of the Galactic magnetic field on many different length scales. This is particularly true for modelling the propagation of cosmic rays into the Galactic halo, where our knowledge of the magnetic field is particularly poor.
In the last decade, observations of the Galactic halo in different frequency regimes have revealed the existence of out-of-plane bubble emission in the Galactic halo. In gamma rays these bubbles have been termed Fermi bubbles with a radial extent of ≈ 3 kpc and an azimuthal height of ≈ 6 kpc. The radio counterparts of the Fermi bubbles were seen by both the S-PASS telescopes and the Planck satellite, and showed a clear spatial overlap. The X-ray counterparts of the Fermi bubbles were named eROSITA bubbles after the eROSITA satellite, with a radial width of ≈ 7 kpc and an azimuthal height of ≈ 14 kpc. Taken together, these observations suggest the presence of large extended Galactic Halo Bubbles (GHB) and have stimulated interest in exploring the less explored Galactic halo.
In this thesis, a new toy model (GHB model) for the magnetic field and non-thermal electron distribution in the Galactic halo has been proposed. The new toy model has been used to produce polarised synchrotron emission sky maps. Chi-square analysis was used to compare the synthetic skymaps with the Planck 30 GHz polarised skymaps. The obtained constraints on the strength and azimuthal height were found to be in agreement with the S-PASS radio observations.
The upper, lower and best-fit values obtained from the above chi-squared analysis were used to generate three separate toy models. These three models were used to propagate ultra-high energy cosmic rays. This study was carried out for two potential sources, Centaurus A and NGC 253, to produce magnification maps and arrival direction skymaps. The simulated arrival direction skymaps were found to be consistent with the hotspots of Centaurus A and NGC 253 as seen in the observed arrival direction skymaps provided by the Pierre Auger Observatory (PAO).
The turbulent magnetic field component of the GHB model was also used to investigate the extragalactic dipole suppression seen by PAO. UHECRs with an extragalactic dipole were forward-tracked through the turbulent GHB model at different field strengths. The suppression in the dipole due to the varying diffusion coefficient from the simulations was noted. The results could also be compared with an analytical analogy of electrostatics. The simulations of the extragalactic dipole suppression were in agreement with similar studies carried out for galactic cosmic rays.
We recently discovered that the luminous radio-quiet (QSO) LBQS 0302-0019 at z=3.286 is likely accompanied by an obscured AGN at 20 kpc projected distance, which we dubbed Jil. It represents the tightest candidate obscured/unobscured dual AGN system at z >3. To verify the dual AGN scenario we obtained deep K-s band (rest-frame V band) imaging with the VLT/HAWK-I+GRAAL instrument at 0 '.4 resolution during science verification in January 2018. Indeed, we detect the individual host galaxies of the QSO and Jil with estimated stellar masses of log(M-*/M-circle dot)=11.4 +/- 0.5 and log(M-*/M-circle dot)=10.9 +/- 0.5, respectively. Near-IR spectra obtained with VLT-KMOS reveal a clear [O-III] lambda 5007 line detection at the location of Jil which does not contribute significantly to the Ks band flux. Both observations therefore corroborate the dual AGN scenario. A comparison to Illustris cosmological simulations suggests a parent halo mass of log(M-halo/M-*)=13.2 +/- 0.5 for this interacting galaxy system, corresponding to a very massive dark matter halo at that epoch.
We present a sample of 34 weak metal line absorbers at z < 0.3 selected by the simultaneous >3σ detections of the Si iiλ1260 and C iiλ1334 absorption lines, with Wr(SiII)<0.2 Å and Wr(CII)<0.3 Å, in archival HST/COS spectra. Our sample increases the number of known low-z ‘weak absorbers’ by a factor of >5. The column densities of H i and low-ionization metal lines obtained from Voigt profile fitting are used to build simple photoionization models. The inferred densities and line-of-sight thicknesses of the absorbers are in the ranges of −3.3 < log nH/cm−3 < −2.4 and ∼1 pc–50 kpc (median ≈500 pc), respectively. Most importantly, 85 per cent (50 per cent) of these absorbers show a metallicity of [Si/H]>−1.0(0.0). The fraction of systems showing near-/supersolar metallicity in our sample is significantly higher than in the H i-selected sample of Wotta et al., and the galaxy-selected sample of Prochaska et al., of absorbers probing the circum-galactic medium at similar redshift. A search for galaxies has revealed a significant galaxy-overdensity around these weak absorbers compared to random positions with a median impact parameter of 166 kpc from the nearest galaxy. Moreover, we find the presence of multiple galaxies in ≈80 per cent of the cases, suggesting group environments. The observed dN/dz of 0.8 ± 0.2 indicates that such metal-enriched, compact, dense structures are ubiquitous in the haloes of low-z group galaxies. We suggest that these are transient structures that are related to galactic outflows and/or stripping of metal-rich gas from galaxies.
We consider the dynamics of the Kuramoto ensemble oscillators not included in a common synchronized cluster, where the mean field is subject to fluctuations. The fluctuations can be either related to the finite size of the ensemble or superimposed on the mean field in the form of common noise due to the constructive features of the system. It is shown that the states of such oscillators with close natural frequencies appear correlated with each other, since the mean-field fluctuations act as common noise. We quantify the effect with the synchronization index of two oscillators, which is calculated numerically and analytically as a function of the frequency difference and noise intensity. The results are rigorous for large ensembles with additional noise superimposed on the mean field and are qualitatively true for the systems where the mean-field fluctuations are due to the finite size of the ensemble. In the latter case, the effect is found to be independent of the number of oscillators in the ensemble.
The complex hierarchical structure of bone undergoes a lifelong remodeling process, where it adapts to mechanical needs. Hereby, bone resorption by osteoclasts and bone formation by osteoblasts have to be balanced to sustain a healthy and stable organ. Osteocytes orchestrate this interplay by sensing mechanical strains and translating them into biochemical signals. The osteocytes are located in lacunae and are connected to one another and other bone cells via cell processes through small channels, the canaliculi. Lacunae and canaliculi form a network (LCN) of extracellular spaces that is able to transport ions and enables cell-to-cell communication. Osteocytes might also contribute to mineral homeostasis by direct interactions with the surrounding matrix. If the LCN is acting as a transport system, this should be reflected in the mineralization pattern. The central hypothesis of this thesis is that osteocytes are actively changing their material environment. Characterization methods of material science are used to achieve the aim of detecting traces of this interaction between osteocytes and the extracellular matrix. First, healthy murine bones were characterized. The properties analyzed were then compared with three murine model systems: 1) a loading model, where a bone of the mouse was loaded during its life time; 2) a healing model, where a bone of the mouse was cut to induce a healing response; and 3) a disease model, where the Fbn1 gene is dysfunctional causing defects in the formation of the extracellular tissue.
The measurement strategy included routines that make it possible to analyze the organization of the LCN and the material components (i.e., the organic collagen matrix and the mineral particles) in the same bone volumes and compare the spatial distribution of different data sets. The three-dimensional network architecture of the LCN is visualized by confocal laser scanning microscopy (CLSM) after rhodamine staining and is then subsequently quantified. The calcium content is determined via quantitative backscattered electron imaging (qBEI), while small- and wide-angle X-ray scattering (SAXS and WAXS) are employed to determine the thickness and length of local mineral particles.
First, tibiae cortices of healthy mice were characterized to investigate how changes in LCN architecture can be attributed to interactions of osteocytes with the surrounding bone matrix. The tibial mid-shaft cross-sections showed two main regions, consisting of a band with unordered LCN surrounded by a region with ordered LCN. The unordered region is a remnant of early bone formation and exhibited short and thin mineral particles. The surrounding, more aligned bone showed ordered and dense LCN as well as thicker and longer mineral particles. The calcium content was unchanged between the two regions.
In the mouse loading model, the left tibia underwent two weeks of mechanical stimulation, which results in increased bone formation and decreased resorption in skeletally mature mice. Here the specific research question addressed was how do bone material characteristics change at (re)modeling sites? The new bone formed in response to mechanical stimulation showed similar properties in terms of the mineral particles, like the ordered calcium region but lower calcium content compared to the right, non-loaded control bone of the same mice. There was a clear, recognizable border between mature and newly formed bone. Nevertheless, some canaliculi went through this border connecting the LCN of mature and newly formed bone.
Additionally, the question should be answered whether the LCN topology and the bone matrix material properties adapt to loading. Although, mechanically stimulated bones did not show differences in calcium content compared to controls, different correlations were found between the local LCN density and the local Ca content depending on whether the bone was loaded or not. These results suggest that the LCN may serve as a mineral reservoir.
For the healing model, the femurs of mice underwent an osteotomy, stabilized with an external fixator and were allowed to heal for 21 days. Thus, the spatial variations in the LCN topology with mineral properties within different tissue types and their interfaces, namely calcified cartilage, bony callus and cortex, could be simultaneously visualized and compared in this model. All tissue types showed structural differences across multiple length scales. Calcium content increased and became more homogeneous from calcified cartilage to bony callus to lamellar cortical bone. The degree of LCN organization increased as well, while the lacunae became smaller, as did the lacunar density between these different tissue types that make up the callus. In the calcified cartilage, the mineral particles were short and thin. The newly formed callus exhibited thicker mineral particles, which still had a low degree of orientation. While most of the callus had a woven-like structure, it also served as a scaffold for more lamellar tissue at the edges. The lamelar bone callus showed thinner mineral particles, but a higher degree of alignment in both, mineral particles and the LCN. The cortex showed the highest values for mineral length, thickness and degree of orientation. At the same time, the lacunae number density was 34% lower and the lacunar volume 40% smaller compared to bony callus. The transition zone between cortical and callus regions showed a continuous convergence of bone mineral properties and lacunae shape. Although only a few canaliculi connected callus and the cortical region, this indicates that communication between osteocytes of both tissues should be possible. The presented correlations between LCN architecture and mineral properties across tissue types may suggest that osteocytes have an active role in mineralization processes of healing.
A mouse model for the disease marfan syndrome, which includes a genetic defect in the fibrillin-1 gene, was investigated. In humans, Marfan syndrome is characterized by a range of clinical symptoms such as long bone overgrowth, loose joints, reduced bone mineral density, compromised bone microarchitecture, and increased fracture rates. Thus, fibrillin-1 seems to play a role in the skeletal homeostasis. Therefore, the present work studied how marfan syndrome alters LCN architecture and the surrounding bone matrix. The mice with marfan syndrome showed longer tibiae than their healthy littermates from an age of seven weeks onwards. In contrast, the cortical development appeared retarded, which was observed across all measured characteristics, i. e. lower endocortical bone formation, looser and less organized lacuno-canalicular network, less collagen orientation, thinner and shorter mineral particles.
In each of the three model systems, this study found that changes in the LCN architecture spatially correlated with bone matrix material parameters. While not knowing the exact mechanism, these results provide indications that osteocytes can actively manipulate a mineral reservoir located around the canaliculi to make a quickly accessible contribution to mineral homeostasis. However, this interaction is most likely not one-sided, but could be understood as an interplay between osteocytes and extra-cellular matrix, since the bone matrix contains biochemical signaling molecules (e.g. non-collagenous proteins) that can change osteocyte behavior. Bone (re)modeling can therefore not only be understood as a method for removing defects or adapting to external mechanical stimuli, but also for increasing the efficiency of possible osteocyte-mineral interactions during bone homeostasis. With these findings, it seems reasonable to consider osteocytes as a target for drug development related to bone diseases that cause changes in bone composition and mechanical properties. It will most likely require the combined effort of materials scientists, cell biologists, and molecular biologists to gain a deeper understanding of how bone cells respond to their material environment.
This paper is concerned with correlation functions of stochastic systems with memory, a prominent example being a molecule or colloid moving through a complex (e.g. viscoelastic) fluid environment. Analytical investigations of such systems based on non-Markovian stochastic equations are notoriously difficult. A common approximation is that of a single-exponential memory, corresponding to the introduction of one auxiliary variable coupled to the Markovian dynamics of the main variable. As a generalization, we here investigate a class of 'toy' models with altogether three degrees of freedom, giving rise to more complex forms of memory. Specifically, we consider, mainly on an analytical basis, the under- and overdamped motion of a colloidal particle coupled linearly to two auxiliary variables, where the coupling between variables can be either reciprocal or non-reciprocal. Projecting out the auxiliary variables, we obtain non-Markovian Langevin equations with friction kernels and colored noise, whose structure is similar to that of a generalized Langevin equation. For the present systems, however, the non-Markovian equations may violate the fluctuation-dissipation relation as well as detailed balance, indicating that the systems are out of equilibrium. We then study systematically the connection between the coupling topology of the underlying Markovian system and various autocorrelation functions. We demonstrate that already two auxiliary variables can generate surprisingly complex (e.g. non-monotonic or oscillatory) memory and correlation functions. Finally, we show that a minimal overdamped model with two auxiliary variables and suitable non-reciprocal coupling yields correlation functions resembling those describing hydrodynamic backflow in an optical trap.
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.
Corona and the climate
(2020)
In this paper, we report X-ray absorption and core-level electron spectra of the nucleobase derivative 2-thiouracil at the sulfur L1- and L2,3-edges. We used soft X-rays from the free-electron laser FLASH2 for the excitation of isolated molecules and dispersed the outgoing electrons with a magnetic bottle spectrometer. We identified photoelectrons from the 2p core orbital, accompanied by an electron correlation satellite, as well as resonant and non-resonant Coster–Kronig and Auger–Meitner emission at the L1- and L2,3-edges, respectively. We used the electron yield to construct X-ray absorption spectra at the two edges. The experimental data obtained are put in the context of the literature currently available on sulfur core-level and 2-thiouracil spectroscopy.
In this paper, we report X-ray absorption and core-level electron spectra of the nucleobase derivative 2-thiouracil at the sulfur L1- and L2,3-edges. We used soft X-rays from the free-electron laser FLASH2 for the excitation of isolated molecules and dispersed the outgoing electrons with a magnetic bottle spectrometer. We identified photoelectrons from the 2p core orbital, accompanied by an electron correlation satellite, as well as resonant and non-resonant Coster–Kronig and Auger–Meitner emission at the L1- and L2,3-edges, respectively. We used the electron yield to construct X-ray absorption spectra at the two edges. The experimental data obtained are put in the context of the literature currently available on sulfur core-level and 2-thiouracil spectroscopy.
We present new, contemporaneous Hubble Space Telescope STIS and XMM-Newton observations of the O7. III(n) ((f)) star xi Per. We supplement the new data with archival IUE spectra, to analyze the variability of the wind lines and X-ray flux of xi Per. The variable wind of this star is known to have a 2.086-day periodicity. We use a simple, heuristic spot model that fits the low-velocity (near-surface) IUE wind line variability very well, to demonstrate that the low-velocity absorption in the new STIS spectra of N IV lambda 1718 and Si IV lambda 1402 vary with the same 2.086-day period. It is remarkable that the period and amplitude of the STIS data agree with those of the IUE spectra obtained 22 yr earlier. We also show that the time variability of the new XMM-Newton fluxes is also consistent with the 2.086-day period. Thus, our new, multiwavelength coordinated observations demonstrate that the mechanism that causes the UV wind line variability is also responsible for a significant fraction of the X-rays in single O stars. The sequence of events for the multiwavelength light-curve minima is Si IV lambda 1402, N IV lambda 1718, and X-ray flux, each separated by a phase of about 0.06 relative to the 2.086-day period. Analysis of the X-ray fluxes shows that they become softer as they weaken. This is contrary to expectations if the variability is caused by periodic excess absorption. Furthermore, the high-resolution X-ray spectra suggest that the individual emission lines at maximum are more strongly blueshifted. If we interpret the low-velocity wind line light curves in terms of our model, it implies that there are two bright regions, i.e., regions with less absorption, separated by 180 degrees, on the surface of the star. We note that the presence and persistence of two spots separated by 180 degrees suggest that a weak dipole magnetic field is responsible for the variability of the UV wind line absorption and X-ray flux in xi Per.
We present a general analysis of the cooling produced by losses on condensates or quasi-condensates. We study how the occupations of the collective phonon modes evolve in time, assuming that the loss process is slow enough so that each mode adiabatically follows the decrease of the mean density. The theory is valid for any loss process whose rate is proportional to the jth power of the density, but otherwise spatially uniform. We cover both homogeneous gases and systems confined in a smooth potential. For a low-dimensional gas, we can take into account the modified equation of state due to the broadening of the cloud width along the tightly confined directions, which occurs for large interactions. We find that at large times, the temperature decreases proportionally to the energy scale mc2, where m is the mass of the particles and c the sound velocity. We compute the asymptotic ratio of these two quantities for different limiting cases: a homogeneous gas in any dimension and a one-dimensional gas in a harmonic trap.
We present a general analysis of the cooling produced by losses on condensates or quasi-condensates. We study how the occupations of the collective phonon modes evolve in time, assuming that the loss process is slow enough so that each mode adiabatically follows the decrease of the mean density. The theory is valid for any loss process whose rate is proportional to the jth power of the density, but otherwise spatially uniform. We cover both homogeneous gases and systems confined in a smooth potential. For a low-dimensional gas, we can take into account the modified equation of state due to the broadening of the cloud width along the tightly confined directions, which occurs for large interactions. We find that at large times, the temperature decreases proportionally to the energy scale mc(2), where m is the mass of the particles and c the sound velocity. We compute the asymptotic ratio of these two quantities for different limiting cases: a homogeneous gas in any dimension and a one-dimensional gas in a harmonic trap.
In the present study, we employ the angle-resolved photoemission spectroscopy (ARPES) technique to study the electronic structure of topological states of matter. In particular, the so-called topological crystalline insulators (TCIs) Pb1-xSnxSe and Pb1-xSnxTe, and the Mn-doped Z2 topological insulators (TIs) Bi2Te3 and Bi2Se3. The Z2 class of strong topological insulators is protected by time-reversal symmetry and is characterized by an odd number of metallic Dirac type surface states in the surface Brillouin zone. The topological crystalline insulators on the other hand are protected by the individual crystal symmetries and exhibit an even number of Dirac cones.
The topological properties of the lead tin chalcogenides topological crystalline insulators can be tuned by temperature and composition. Here, we demonstrate that Bi-doping of the Pb1-xSnxSe(111) epilayers induces a quantum phase transition from a topological crystalline insulator to a Z2 topological insulator. This occurs because Bi-doping lifts the fourfold valley degeneracy in the bulk. As a consequence a gap appears at ⌈¯, while the three Dirac cones at the M̅ points of the surface Brillouin zone remain intact. We interpret this new phase transition is caused by lattice distortion. Our findings extend the topological phase diagram enormously and make strong topological insulators switchable by distortions or electric field. In contrast, the bulk Bi doping of epitaxial Pb1-xSnxTe(111) films induces a giant Rashba splitting at the surface that can be tuned by the doping level. Tight binding calculations identify their origin as Fermi level pinning by trap states at the surface.
Magnetically doped topological insulators enable the quantum anomalous Hall effect (QAHE) which provide quantized edge states for lossless charge transport applications. The edge states are hosted by a magnetic energy gap at the Dirac point which has not been experimentally observed to date. Our low temperature ARPES studies unambiguously reveal the magnetic gap of Mn-doped Bi2Te3. Our analysis shows a five times larger gap size below the Tc than theoretically predicted. We assign this enhancement to a remarkable structure modification induced by Mn doping. Instead of a disordered impurity system, a self-organized alternating sequence of MnBi2Te4 septuple and Bi2Te3quintuple layers is formed. This enhances the wave-function overlap and gives rise to a large magnetic gap. Mn-doped Bi2Se3 forms similar heterostructure, but only a nonmagnetic gap is observed in this system. This correlates with the difference in magnetic anisotropy due to the much larger spin-orbit interaction in Bi2Te3 compared to Bi2Se3. These findings provide crucial insights for pushing lossless transport in topological insulators towards room-temperature applications.
The influence of different parameters on the silicification procedure using lysozyme is reported. When polyethoxysiloxane (PEOS), an internally crosslinked silica reservoir, is used, regular structures with a narrow size distribution could be obtained only via introducing the silica precursor in two steps including initial dropping and subsequent addition of residual oil phase in one portion. We found that mixing sequence of mineralizing agents in the presence of a positively charged surfactant plays a key role in terms of silica precipitation when tetraethoxyorthosilicate (TEOS) is the oil phase. In contrast, well mineralized crumpled features with high specific surface area could be synthesized in the presence of PEOS as a silica precursor polymer, regardless of mixing sequence. Moreover, introducing sodium dodecyl sulfate (SDS) as a negatively charged surfactant resulted in regular silica sphere formation only in combination with hexylene glycol (MPD) as a specific co-solvent. Finally, it is demonstrated that by inclusion of different nanoparticles even more sophisticated hybrid materials can be generated.
Manipulating spin waves is highly required for the development of innovative data transport and processing technologies. Recently, the possibility of triggering high-frequency standing spin waves in magnetic insulators using femtosecond laser pulses was discovered, raising the question about how one can manipulate their dynamics. Here we explore this question by investigating the ultrafast magnetiza-tion and spin-wave dynamics induced by double-pulse laser excitation. We demonstrate a suppression or enhancement of the amplitudes of the standing spin waves by precisely tuning the time delay between the two pulses. The results can be understood as the constructive or destructive interference of the spin waves induced by the first and second laser pulses. Our findings open exciting perspectives towards generating single-mode standing spin waves that combine high frequency with large amplitude and low magnetic damping.
We present an efficient technique for control of synchrony in a globally coupled ensemble by pulsatile action. We assume that we can observe the collective oscillation and can stimulate all elements of the ensemble simultaneously. We pay special attention to the minimization of intervention into the system. The key idea is to stimulate only at the most sensitive phase. To find this phase, we implement an adaptive feedback control. Estimating the instantaneous phase of the collective mode on the fly, we achieve efficient suppression using a few pulses per oscillatory cycle. We discuss the possible relevance of the results for neuroscience, namely, for the development of advanced algorithms for deep brain stimulation, a medical technique used to treat Parkinson's disease.
Control over spin and electronic structure of MoS₂ monolayer via interactions with substrates
(2023)
The molybdenum disulfide (MoS2) monolayer is a semiconductor with a direct bandgap while it is a robust and affordable material.
It is a candidate for applications in optoelectronics and field-effect transistors.
MoS2 features a strong spin-orbit coupling which makes its spin structure promising for acquiring the Kane-Mele topological concept with corresponding applications in spintronics and valleytronics.
From the optical point of view, the MoS2 monolayer features two valleys in the regions of K and K' points. These valleys are differentiated by opposite spins and a related valley-selective circular dichroism.
In this study we aim to manipulate the MoS2 monolayer spin structure in the vicinity of the K and K' points to explore the possibility of getting control over the optical and electronic properties.
We focus on two different substrates to demonstrate two distinct routes: a gold substrate to introduce a Rashba effect and a graphene/cobalt substrate to introduce a magnetic proximity effect in MoS2.
The Rashba effect is proportional to the out-of-plane projection of the electric field gradient. Such a strong change of the electric field occurs at the surfaces of a high atomic number materials and effectively influence conduction electrons as an in-plane magnetic field. A molybdenum and a sulfur are relatively light atoms, thus, similar to many other 2D materials, intrinsic Rashba effect in MoS2 monolayer is vanishing small. However, proximity of a high atomic number substrate may enhance Rashba effect in a 2D material as it was demonstrated for graphene previously.
Another way to modify the spin structure is to apply an external magnetic field of high magnitude (several Tesla), and cause a Zeeman splitting, the conduction electrons.
However, a similar effect can be reached via magnetic proximity which allows us to reduce external magnetic fields significantly or even to zero. The graphene on cobalt interface is ferromagnetic and stable for MoS2 monolayer synthesis. Cobalt is not the strongest magnet; therefore, stronger magnets may lead to more significant results.
Nowadays most experimental studies on the dichalcogenides (MoS2 included) are performed on encapsulated heterostructures that are produced by mechanical exfoliation.
While mechanical exfoliation (or scotch-tape method) allows to produce a huge variety of structures, the shape and the size of the samples as well as distance between layers in heterostructures are impossible to control reproducibly.
In our study we used molecular beam epitaxy (MBE) methods to synthesise both MoS2/Au(111) and MoS2/graphene/Co systems.
We chose to use MBE, as it is a scalable and reproducible approach, so later industry may adapt it and take over.
We used graphene/cobalt instead of just a cobalt substrate because direct contact of MoS2\ monolayer and a metallic substrate may lead to photoluminescence (PL) quenching in the metallic substrate. Graphene and hexagonal boron nitride monolayer are considered building blocks of a new generation of electronics also commonly used as encapsulating materials for PL studies. Moreover graphene is proved to be a suitable substrate for the MBE growth of transitional metal dichalcogenides (TMDCs).
In chapter 1,
we start with an introduction to TMDCs. Then we focus on MoS2 monolayer state of the art research in the fields of application scenario; synthesis approaches; electronic, spin, and optical properties; and interactions with magnetic fields and magnetic materials.
We briefly touch the basics of magnetism in solids and move on to discuss various magnetic exchange interactions and magnetic proximity effect.
Then we describe MoS2 optical properties in more detail. We start from basic exciton physics and its manifestation in the MoS2 monolayer. We consider optical selection rules in the MoS2 monolayer and such properties as chirality, spin-valley locking, and coexistence of bright and dark excitons.
Chapter 2 contains an overview of the employed surface science methods: angle-integrated, angle-resolved, and spin-resolved photoemission; low energy electron diffraction and scanning tunneling microscopy.
In chapter 3, we describe MoS2 monolayer synthesis details for two substrates: gold monocrystal with (111) surface and graphene on cobalt thin film with Co(111) surface orientation.
The synthesis descriptions are followed by a detailed characterisation of the obtained structures: fingerprints of MoS2 monolayer formation; MoS2 monolayer symmetry and its relation to the substrate below; characterisation of MoS2 monolayer coverage, domain distribution, sizes and shapes, and moire structures.
In chapter~4, we start our discussion with MoS2/Au(111) electronic and spin structure. Combining density functional theory computations (DFT) and spin-resolved photoemission studies, we demonstrate that the MoS2 monolayer band structure features an in-plane Rashba spin splitting. This confirms the possibility of MoS2 monolayer spin structure manipulation via a substrate.
Then we investigate the influence of a magnetic proximity in the MoS2/graphene/Co system on the MoS2 monolayer spin structure.
We focus our investigation on MoS2 high symmetry points: G and K.
First, using spin-resolved measurements, we confirm that electronic states are spin-split at the G point via a magnetic proximity effect. Second, combining spin-resolved measurements and DFT computations for MoS2 monolayer in the K point region, we demonstrate the appearance of a small in-plane spin polarisation in the valence band top and predict a full in-plane spin polarisation for the conduction band bottom.
We move forward discussing how these findings are related to the MoS2 monolayer optical properties, in particular the possibility of dark exciton observation. Additionally, we speculate on the control of the MoS2 valley energy via magnetic proximity from cobalt.
As graphene is spatially buffering the MoS2 monolayer from the Co thin film, we speculate on the role of graphene in the magnetic proximity transfer by replacing graphene with vacuum and other 2D materials in our computations.
We finish our discussion by investigating the K-doped MoS2/graphene/Co system and the influence of this doping on the electronic and spin structure as well as on the magnetic proximity effect.
In summary, using a scalable MBE approach we synthesised
MoS2/Au(111) and MoS2/graphene/Co systems. We found a Rashba effect taking place in MoS2/Au(111) which proves that the MoS2 monolayer in-plane spin structure can be modified. In MoS2/graphene/Co the in-plane magnetic proximity effect indeed takes place which rises the possibility of fine tuning the MoS2 optical properties via manipulation of the the substrate magnetisation.
In two-dimensional reaction-diffusion systems, local curvature perturbations on traveling waves are typically damped out and vanish. However, if the inhibitor diffuses much faster than the activator, transversal instabilities can arise, leading from flat to folded, spatio-temporally modulated waves and to spreading spiral turbulence. Here, we propose a scheme to induce or inhibit these instabilities via a spatio-temporal feedback loop. In a piecewise-linear version of the FitzHugh-Nagumo model, transversal instabilities and spiral turbulence in the uncontrolled system are shown to be suppressed in the presence of control, thereby stabilizing plane wave propagation. Conversely, in numerical simulations with the modified Oregonator model for the photosensitive Belousov-Zhabotinsky reaction, which does not exhibit transversal instabilities on its own, we demonstrate the feasibility of inducing transversal instabilities and study the emerging wave patterns in a well-controlled manner.
The oxidation and spin state of a metal-organic molecule determine its chemical reactivity and magnetic properties. Here, we demonstrate the reversible control of the oxidation and spin state in a single Fe porphyrin molecule in the force field of the tip of a scanning electron tunneling microscope. Within the regimes of half-integer and integer spin state, we can further track the evolution of the magnetocrystalline anisotropy. Our experimental results are corroborated by density functional theory and wave function theory. This combined analysis allows us to draw a complete picture of the molecular states over a large range of intramolecular deformations.
We demonstrate that a multiple delayed feedback is a powerful tool to control coherence properties of autonomous self-sustained oscillators. We derive the equation for the phase dynamics in presence of noise and delay, and analyze it analytically. In Gaussian approximation a closed set of equations for the frequency and the diffusion constant is obtained. Solutions of these equations are in good agreement with direct numerical simulations.
Arctic Amplification of climate warming is caused by various feedback processes in the atmosphere-ocean-ice system and yields the strongest temperature increase during winter in the Arctic North Atlantic region. In our study, we attempt to quantify the advective contribution to the observed atmospheric warming in the Svalbard area. Based on radiosonde measurements from Ny-Ålesund, a strong dependence of the tropospheric temperature on the synoptic flow direction is revealed. Using FLEXTRA backward trajectories, an increase of advection from the lower latitude Atlantic region towards Ny-Ålesund is found that is attributed to a change in atmospheric circulation patterns. We find that about one-quarter (0.45 K per decade) of the observed atmospheric winter near surface warming trend in the North Atlantic region of the Arctic (2 K per decade) is due to increased advection of warm and moist air from the lower latitude Atlantic region, affecting the entire troposphere.
We investigate the effects of Markovian resetting events on continuous time random walks where the waiting times and the jump lengths are random variables distributed according to power-law probability density functions.
We prove the existence of a nonequilibrium stationary state and finite mean first arrival time.
However, the existence of an optimum reset rate is conditioned to a specific relationship between the exponents of both power-law tails.
We also investigate the search efficiency by finding the optimal random walk which minimizes the mean first arrival time in terms of the reset rate, the distance of the initial position to the target, and the characteristic transport exponents.
We consider the emerging dynamics of a separable continuous time random walk (CTRW) in the case when the random walker is biased by a velocity field in a uniformly growing domain. Concrete examples for such domains include growing biological cells or lipid vesicles, biofilms and tissues, but also macroscopic systems such as expanding aquifers during rainy periods, or the expanding Universe. The CTRW in this study can be subdiffusive, normal diffusive or superdiffusive, including the particular case of a Lévy flight. We first consider the case when the velocity field is absent. In the subdiffusive case, we reveal an interesting time dependence of the kurtosis of the particle probability density function. In particular, for a suitable parameter choice, we find that the propagator, which is fat tailed at short times, may cross over to a Gaussian-like propagator. We subsequently incorporate the effect of the velocity field and derive a bi-fractional diffusion-advection equation encoding the time evolution of the particle distribution. We apply this equation to study the mixing kinetics of two diffusing pulses, whose peaks move towards each other under the action of velocity fields acting in opposite directions. This deterministic motion of the peaks, together with the diffusive spreading of each pulse, tends to increase particle mixing, thereby counteracting the peak separation induced by the domain growth. As a result of this competition, different regimes of mixing arise. In the case of Lévy flights, apart from the non-mixing regime, one has two different mixing regimes in the long-time limit, depending on the exact parameter choice: in one of these regimes, mixing is mainly driven by diffusive spreading, while in the other mixing is controlled by the velocity fields acting on each pulse. Possible implications for encounter–controlled reactions in real systems are discussed.
We consider the emerging dynamics of a separable continuous time random walk (CTRW) in the case when the random walker is biased by a velocity field in a uniformly growing domain. Concrete examples for such domains include growing biological cells or lipid vesicles, biofilms and tissues, but also macroscopic systems such as expanding aquifers during rainy periods, or the expanding Universe. The CTRW in this study can be subdiffusive, normal diffusive or superdiffusive, including the particular case of a Lévy flight. We first consider the case when the velocity field is absent. In the subdiffusive case, we reveal an interesting time dependence of the kurtosis of the particle probability density function. In particular, for a suitable parameter choice, we find that the propagator, which is fat tailed at short times, may cross over to a Gaussian-like propagator. We subsequently incorporate the effect of the velocity field and derive a bi-fractional diffusion-advection equation encoding the time evolution of the particle distribution. We apply this equation to study the mixing kinetics of two diffusing pulses, whose peaks move towards each other under the action of velocity fields acting in opposite directions. This deterministic motion of the peaks, together with the diffusive spreading of each pulse, tends to increase particle mixing, thereby counteracting the peak separation induced by the domain growth. As a result of this competition, different regimes of mixing arise. In the case of Lévy flights, apart from the non-mixing regime, one has two different mixing regimes in the long-time limit, depending on the exact parameter choice: in one of these regimes, mixing is mainly driven by diffusive spreading, while in the other mixing is controlled by the velocity fields acting on each pulse. Possible implications for encounter–controlled reactions in real systems are discussed.
We discuss the notion of symmetries in non-local field theories characterized by integro-differential equations of motion, from a geometric perspective. We then focus on group field theory (GFT) models of quantum gravity and provide a general analysis of their continuous point symmetry transformations, including the generalized conservation laws following from them.
Although it is theoretically expected that all organic semiconductors support ambipolar charge transport, most organic transistors either transport holes or electrons effectively. Single-layer ambipolar organic field-effect transistors enable the investigation of different mechanisms in hole and electron transport in a single device since the device architecture provides a controllable planar pn-junction within the transistor channel. However, a direct comparison of the injection barriers and of the channel conductivities between electrons and holes within the same device cannot be measured by standard electrical characterization. This article introduces a novel approach for determining threshold gate voltages for the onset of the ambipolar regime from the position of the pn-junction observed by photoluminescence electromodulation (PLEM) microscopy. Indeed, the threshold gate voltage in the ambipolar bias regime considers a vanishing channel length, thus correlating the contact resistance. PLEM microscopy is a valuable tool to directly compare the contact and channel resistances for both carrier types in the same device. The reported results demonstrate that designing the metal/organic semiconductor interfaces by aligning the bulk metal Fermi levels to the highest occupied molecular orbital or lowest unoccupied molecular orbital levels of the organic semiconductors is a too simplistic approach for optimizing the charge injection process in organic field-effect devices.
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.
Quasiuniversal relations between the tidal deformability and the quadrupole moment of neutron stars are predicted by theoretical computations, but have not been measured experimentally. We simulate 120 binary neutron star sources and find that Advanced LIGO and Advanced Virgo at design sensitivity could find possible deviations from predicted relations if the neutron stars are highly spinning. A network of envisaged third generation detectors will even allow extracting such relations, providing new tests of general relativity and nuclear physics predictions.
The flat spectrum radio quasar 3C 279 is known to exhibit pronounced variability in the high-energy (100MeV < E < 100 GeV) gamma-ray band, which is continuously monitored with Fermi-LAT. During two periods of high activity in April 2014 and June 2015 target-of-opportunity observations were undertaken with the High Energy Stereoscopic System (H.E.S.S.) in the very-high-energy (VHE, E > 100 GeV) gamma-ray domain. While the observation in 2014 provides an upper limit, the observation in 2015 results in a signal with 8 : 7 sigma significance above an energy threshold of 66 GeV. No VHE variability was detected during the 2015 observations. The VHE photon spectrum is soft and described by a power-law index of 4.2 +/- 0.3. The H.E.S.S. data along with a detailed and contemporaneous multiwavelength data set provide constraints on the physical parameters of the emission region. The minimum distance of the emission region from the central black hole was estimated using two plausible geometries of the broad-line region and three potential intrinsic spectra. The emission region is confidently placed at r greater than or similar to 1 : 7 X 1017 cm from the black hole, that is beyond the assumed distance of the broad-line region. Time-dependent leptonic and lepto-hadronic one-zone models were used to describe the evolution of the 2015 flare. Neither model can fully reproduce the observations, despite testing various parameter sets. Furthermore, the H.E.S.S. data were used to derive constraints on Lorentz invariance violation given the large redshift of 3C 279.
Uncertainty about the sensitivity of the climate system to changes in the Earth’s radiative balance constitutes a primary source of uncertainty for climate projections. Given the continuous increase in atmospheric greenhouse gas concentrations, constraining the uncertainty range in such type of sensitivity is of vital importance. A common measure for expressing this key characteristic for climate models is the climate sensitivity, defined as the simulated change in global-mean equilibrium temperature resulting from a doubling of atmospheric CO2 concentration. The broad range of climate sensitivity estimates (1.5-4.5°C as given in the last Assessment Report of the Intergovernmental Panel on Climate Change, 2001), inferred from comprehensive climate models, illustrates that the strength of simulated feedback mechanisms varies strongly among different models. The central goal of this thesis is to constrain uncertainty in climate sensitivity. For this objective we first generate a large ensemble of model simulations, covering different feedback strengths, and then request their consistency with present-day observational data and proxy-data from the Last Glacial Maximum (LGM). Our analyses are based on an ensemble of fully-coupled simulations, that were realized with a climate model of intermediate complexity (CLIMBER-2). These model versions cover a broad range of different climate sensitivities, ranging from 1.3 to 5.5°C, and have been generated by simultaneously perturbing a set of 11 model parameters. The analysis of the simulated model feedbacks reveals that the spread in climate sensitivity results from different realizations of the feedback strengths in water vapour, clouds, lapse rate and albedo. The calculated spread in the sum of all feedbacks spans almost the entire plausible range inferred from a sampling of more complex models. We show that the requirement for consistency between simulated pre-industrial climate and a set of seven global-mean data constraints represents a comparatively weak test for model sensitivity (the data constrain climate sensitivity to 1.3-4.9°C). Analyses of the simulated latitudinal profile and of the seasonal cycle suggest that additional present-day data constraints, based on these characteristics, do not further constrain uncertainty in climate sensitivity. The novel approach presented in this thesis consists in systematically combining a large set of LGM simulations with data information from reconstructed regional glacial cooling. Irrespective of uncertainties in model parameters and feedback strengths, the set of our model versions reveals a close link between the simulated warming due to a doubling of CO2, and the cooling obtained for the LGM. Based on this close relationship between past and future temperature evolution, we define a method (based on linear regression) that allows us to estimate robust 5-95% quantiles for climate sensitivity. We thus constrain the range of climate sensitivity to 1.3-3.5°C using proxy-data from the LGM at low and high latitudes. Uncertainties in glacial radiative forcing enlarge this estimate to 1.2-4.3°C, whereas the assumption of large structural uncertainties may increase the upper limit by an additional degree. Using proxy-based data constraints for tropical and Antarctic cooling we show that very different absolute temperature changes in high and low latitudes all yield very similar estimates of climate sensitivity. On the whole, this thesis highlights that LGM proxy-data information can offer an effective means of constraining the uncertainty range in climate sensitivity and thus underlines the potential of paleo-climatic data to reduce uncertainty in future climate projections.
The maximum entropy method is used to predict flows on water distribution networks. This analysis extends the water distribution network formulation of Waldrip et al. (2016) Journal of Hydraulic Engineering (ASCE), by the use of a continuous relative entropy defined on a reduced parameter set. This reduction in the parameters that the entropy is defined over ensures consistency between different representations of the same network. The performance of the proposed reduced parameter method is demonstrated with a one-loop network case study.
Levy walks are continuous time random walks with spatio-temporal coupling of jump lengths and waiting times, often used to model superdiffusive spreading processes such as animals searching for food, tracer motion in weakly chaotic systems, or even the dynamics in quantum systems such as cold atoms. In the simplest version Levy walks move with a finite speed. Here, we present an extension of the Levy walk scenario for the case when external force fields influence the motion. The resulting motion is a combination of the response to the deterministic force acting on the particle, changing its velocity according to the principle of total energy conservation, and random velocity reversals governed by the distribution of waiting times. For the fact that the motion stays conservative, that is, on a constant energy surface, our scenario is fundamentally different from thermal motion in the same external potentials. In particular, we present results for the velocity and position distributions for single well potentials of different steepness. The observed dynamics with its continuous velocity changes enriches the theory of Levy walk processes and will be of use in a variety of systems, for which the particles are externally confined.