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)
The optical signatures of molecular-doping induced polarons in poly(3-hexylthiophene-2,5-diyl)
(2020)
Optical absorption spectroscopy is a key method to investigate doped conjugated polymers and to characterize the doping-induced charge carriers, i.e., polarons. For prototypical poly(3-hexylthiophene-2,5-diyl) (P3HT), the absorption intensity of molecular dopant induced polarons is widely used to estimate the carrier density and the doping efficiency, i.e., the number of polarons formed per dopant molecule. However, the dependence of the polaron-related absorption features on the structure of doped P3HT, being either aggregates or separated individual chains, is not comprehensively understood in contrast to the optical absorption features of neutral P3HT. In this work, we unambiguously differentiate the optical signatures of polarons on individual P3HT chains and aggregates in solution, notably the latter exhibiting the same shape as aggregates in solid thin films. This is enabled by employing tris(pentafluorophenyl)borane (BCF) as dopant, as this dopant forms only ion pairs with P3HT and no charge transfer complexes, and BCF and its anion have no absorption in the spectral region of P3HT polarons. Polarons on individual chains exhibit absorption peaks at 1.5 eV and 0.6 eV, whereas in aggregates the high-energy peak is split into a doublet 1.3 eV and 1.65 eV, and the low-energy peak is shifted below 0.5 eV. The dependence of the fraction of solvated individual chains versus aggregates on absolute solution concentration, dopant concentration, and temperature is elucidated, and we find that aggregates predominate in solution under commonly used processing conditions. Aggregates in BCF-doped P3HT solution can be effectively removed upon simple filtering. From varying the filter pore size (down to 200 nm) and thin film morphology characterization with scanning force microscopy we reveal the aggregates' size dependence on solution absolute concentration and dopant concentration. Furthermore, X-ray photoelectron spectroscopy shows that the dopant loading in aggregates is higher than for individual P3HT chains. The results of this study help understanding the impact of solution pre-aggregation on thin film properties of molecularly doped P3HT, and highlight the importance of considering such aggregation for other doped conjugated polymers in general.
In their comment on our paper (Caesar et al 2020 Environ. Res. Lett. 15 024003), Chen and Tung (hereafter C&T) argue that our analysis, showing that over the last decades Atlantic meridional overturning circulation (AMOC) strength and global mean surface temperature (GMST) were positively correlated, is incorrect. Their claim is mainly based on two arguments, neither of which is justified: first, C&T claim that our analysis is based on 'established evidence' that was only true for preindustrial conditions-this is not the case. Using data from the modern period (1947-2012), we show that the established understanding (i.e. deep-water formation in the North Atlantic cools the deep ocean and warms the surface) is correct, but our analysis is not based on this fact. Secondly, C&T claim that our results are based on a statistical analysis of only one cycle of data which was furthermore incorrectly detrended. This, too, is not true. Our conclusion that a weaker AMOC delays the current surface warming rather than enhances it, is based on several independent lines of evidence. The data we show to support this covers more than one cycle and the detrending (which was performed to avoid spurious correlations due to a common trend) does not affect our conclusion: the correlation between AMOC strength and GMST is positive. We do not claim that this is strong evidence that the two time series are in phase, but rather that this means that the two time series are not anti-correlated.
Based on micromagnetic simulations and experimental observations of the magnetization and lattice dynamics after the direct optical excitation of the magnetic insulator Bi : YIG or indirect excitation via an optically opaque Pt/Cu double layer, we disentangle the dynamical effects of magnetic anisotropy and magneto-elastic coupling. The strain and temperature of the lattice are quantified via modeling ultrafast x-ray diffraction data. Measurements of the time-resolved magneto-optical Kerr effect agree well with the magnetization dynamics simulated according to the excitation via two mechanisms: the magneto-elastic coupling to the experimentally verified strain dynamics and the ultrafast temperature-induced transient change in the magnetic anisotropy. The numerical modeling proves that, for direct excitation, both mechanisms drive the fundamental mode with opposite phase. The relative ratio of standing spin wave amplitudes of higher-order modes indicates that both mechanisms are substantially active.
The remarkable progress of metal halide perovskites in photovoltaics has led to the power conversion efficiency approaching 26%. However, practical applications of perovskite-based solar cells are challenged by the stability issues, of which the most critical one is photo-induced degradation. Bare CH3NH3PbI3 perovskite films are known to decompose rapidly, with methylammonium and iodine as volatile species and residual solid PbI2 and metallic Pb, under vacuum under white light illumination, on the timescale of minutes. We find, in agreement with previous work, that the degradation is non-uniform and proceeds predominantly from the surface, and that illumination under N-2 and ambient air (relative humidity 20%) does not induce substantial degradation even after several hours. Yet, in all cases the release of iodine from the perovskite surface is directly identified by X-ray photoelectron spectroscopy. This goes in hand with a loss of organic cations and the formation of metallic Pb. When CH3NH3PbI3 films are covered with a few nm thick organic capping layer, either charge selective or non-selective, the rapid photodecomposition process under ultrahigh vacuum is reduced by more than one order of magnitude, and becomes similar in timescale to that under N-2 or air. We conclude that the light-induced decomposition reaction of CH3NH3PbI3, leading to volatile methylammonium and iodine, is largely reversible as long as these products are restrained from leaving the surface. This is readily achieved by ambient atmospheric pressure, as well as a thin organic capping layer even under ultrahigh vacuum. In addition to explaining the impact of gas pressure on the stability of this perovskite, our results indicate that covalently "locking" the position of perovskite components at the surface or an interface should enhance the overall photostability.
Organic solar cells with large insensitivity to donor polymer molar mass across all acceptor classes
(2020)
Donor polymer number-average molar mass (M-n) has long been known to influence organic photovoltaic (OPV) performance via changes in both the polymer properties and the resulting bulk heterojunction morphology. The exact nature of these M-n effects varies from system to system, although there is generally some intermediate M-n that results in optimal performance. Interestingly, our earlier work with the difluorobenzotriazole (FTAZ)-based donor polymer, paired with either N2200 (polymer acceptor) or PC61BM (fullerene acceptor), PcBm demonstrated <10% variation in power conversion efficiency and a consistent morphology over a large span of M-n (30 kg/mol to over 100 kg/mol). Would such insensitivity to polymer M-n still hold true when prevailing small molecular acceptors were used with FTAZ? To answer this question, we explored the impact of FTAZ on OPVs with ITIC, a high-performance small-molecule fused-ring electron acceptor (FREA). By probing the photovoltaic characteristics of the resulting OPVs, we show that a similar FTAZ mn insensitivity is also found in the FTAZ:ITIC system. This study highlights a single-donor polymer which, when paired with an archetypal fullerene, polymer, and FREA, results in systems that are largely insensitive to donor M. Our results may have implications in polymer batch-to-batch reproducibility, in particular, relaxing the need for tight M-n control during synthesis.
Context.
The supergiant ionized shell SMC-SGS 1 (DEM 167), which is located in the outer Wing of the Small Magellanic Cloud (SMC), resembles structures that originate from an energetic star-formation event and later stimulate star formation as they expand into the ambient medium. However, stellar populations within and surrounding SMC-SGS 1 tell a different story. Aims. We present a photometric study of the stellar population encompassed by SMC-SGS 1 in order to trace the history of such a large structure and its potential influence on star formation within the low-density, low-metallicity environment of the SMC.
Methods.
For a stellar population that is physically associated with SMC-SGS 1, we combined near-ultraviolet (NUV) photometry from the Galaxy Evolution Explorer with archival optical (V-band) photometry from the ESO Danish 1.54 m Telescope. Given their colors and luminosities, we estimated stellar ages and masses by matching observed photometry to theoretical stellar isochrone models. Results. We find that the investigated region supports an active, extended star-formation event spanning similar to 25-40 Myr ago, as well as continued star formation into the present. Using a standard initial mass function, we infer a lower bound on the stellar mass from this period of similar to 3 x 10(4) M-circle dot, corresponding to a star-formation intensity of similar to 6 x 10(-3) M-circle dot kpc(-2) yr(-1).
Conclusions.
The spatial and temporal distributions of young stars encompassed by SMC-SGS 1 imply a slow, consistent progression of star formation over millions of years. Ongoing star formation, both along the edge and interior to SMC-SGS 1, suggests a combined stimulated and stochastic mode of star formation within the SMC Wing. We note that a slow expansion of the shell within this low-density environment may preserve molecular clouds within the volume of the shell, leaving them to form stars even after nearby stellar feedback expels local gas and dust.
The DNA interaction with cis-isomers of photosensitive azobenzene-containing surfactants was studied by both experimental methods and computer simulation. It was shown that before the organization of micelles, such surfactants in the cis-conformation form associates of only a single type with a disordered orientation of molecules. In contrast, for trans-isomers, there exist two types of associates with head-to-head or head-to-tail orientations of molecules in dependence on salt concentration in a solution. The comparison of cis- and trans-isomer binding to DNA and the influence of salt concentration on the formation of their complexes with DNA were studied. It was shown that cis-isomers interact with phosphate groups of DNA and that their molecules were also located along the minor groove of DNA.
It is demonstrated for the case of photo-excited ferrocyanide how time-resolved soft X-ray absorption spectroscopy in transmission geometry at the ligand K-edge and metal L-3-edge provides quantitatively equivalent valence electronic structure information, where signatures of photo-oxidation are assessed locally at the metal as well as the ligand. This allows for a direct and independent quantification of the number of photo-oxidized molecules at two soft X-ray absorption edges highlighting the sensitivity of X-ray absorption spectroscopy to the valence orbital occupation of 3d transition metal complexes throughout the soft X-ray range.
Seasonal forecasts are of great interest in many areas. Knowing the amount of precipitation for the upcoming season in regions of water scarcity would facilitate a better water management. If farmers knew the weather conditions of the upcoming summer at sowing time, they could select those cereal species that are best adapted to these conditions. This would allow farmers to improve the harvest and potentially even reduce the amount of pesticides used. However, the undoubted advantages of seasonal forecasts are often opposed by their high degree of uncertainty. The great challenge of generating seasonal forecasts with lead times of several months mainly originates from the chaotic nature of the earth system. In a chaotic system, even tiny differences in the initial conditions can lead to strong deviations in the system’s state in the long run.
In this dissertation we propose an emergent machine learning approach for seasonal forecasting, called the AnlgModel. The AnlgModel combines the analogue method with myopic feature selection and bootstrapping. To benchmark the abilities of the AnlgModel we apply it to seasonal cyclone activity forecasts in the North Atlantic and Northwest Pacific. The AnlgModel demonstrates competitive hindcast skills with two operational forecasts and even outperforms these for long lead times.
In the second chapter we comprehend the forecasting strategy of the Anlg-Model. We thereby analyse the analogue selection process for the 2017 North Atlantic and the 2018 Northwest Pacific seasonal cyclone activity. The analysis shows that those climate indices which are known to influence the seasonal cyclone activity, such as the Niño 3.4 SST, are correctly represented among the selected analogues. Furthermore the selected analogues reflect large-scale climate patterns that were identified by expert reports as being determinative for these particular seasons.
In the third chapter we analyse the features that are used by the AnlgModel for its predictions. We therefore inspect the feature relevance (FR). The FR patterns learned by the AnlgModel show a high congruence with the predictor regions used by the operational forecasts. However, the AnlgModel also discovered new features, such as the SST anomaly in the Gulf of Guinea during November. This SST pattern exhibits a remarkably high predictive potential for the upcoming Atlantic hurricane activity.
In the final chapter we investigate potential mechanisms, that link two of these regions with high feature relevance to the Atlantic hurricane activity. We mainly focus on ocean surface transport. The ocean surface flow paths are calculated using Lagrangian particle analysis. We demonstrate that the FR patterns in the region of the Canary islands do not correspond with ocean surface transport. It is instead likely that these FR patterns fingerprint a wind transport of latent heat. The second region to be studied is situated in the Gulf of Guinea. Our analysis shows that the FR patterns seen there do fingerprint ocean surface transport. However, our simulations also show that at least one other mechanism is involved in linking the Gulf of Guinea SST anomaly in November to the hurricane activity of the upcoming season.
In this work the AnlgModel does not only demonstrate its outstanding forecast skills but also shows its capabilities as research tool for detecting oceanic and atmospheric mechanisms.
We analyze historical data of stock-market prices for multiple financial indices using the concept of delay-time averaging for the financial time series (FTS). The region of validity of our recent theoretical predictions [Cherstvy A G et al 2017 New J. Phys. 19 063045] for the standard and delayed time-averaged mean-squared 'displacements' (TAMSDs) of the historical FTS is extended to all lag times. As the first novel element, we perform extensive computer simulations of the stochastic differential equation describing geometric Brownian motion (GBM) which demonstrate a quantitative agreement with the analytical long-term price-evolution predictions in terms of the delayed TAMSD (for all stock-market indices in crisis-free times). Secondly, we present a robust procedure of determination of the model parameters of GBM via fitting the features of the price-evolution dynamics in the FTS for stocks and cryptocurrencies. The employed concept of single-trajectory-based time averaging can serve as a predictive tool (proxy) for a mathematically based assessment and rationalization of probabilistic trends in the evolution of stock-market prices.
We report a comparison of two photonic techniques for single-molecule sensing: fluorescence nanoscopy and optoplasmonic sensing. As the test system, oligonucleotides with and without fluorescent labels are transiently hybridized to complementary "docking" strands attached to gold nanorods. Comparing the measured single-molecule kinetics helps to examine the influence of the fluorescent labels as well as factors arising from different sensing geometries. Our results demonstrate that DNA dissociation is not significantly altered by the fluorescent labels and that DNA association is affected by geometric factors in the two techniques. These findings open the door to exploiting plasmonic sensing and fluorescence nanoscopy in a complementary fashion, which will aid in building more powerful sensors and uncovering the intricate effects that influence the behavior of single molecules.
Master equations are a vital tool to model heat flow through nanoscale thermodynamic systems. Most practical devices are made up of interacting subsystems and are often modelled using either local master equations (LMEs) or global master equations (GMEs). While the limiting cases in which either the LME or the GME breaks down are well understood, there exists a 'grey area' in which both equations capture steady-state heat currents reliably but predict very different transient heat flows. In such cases, which one should we trust? Here we show that, when it comes to dynamics, the local approach can be more reliable than the global one for weakly interacting open quantum systems. This is due to the fact that the secular approximation, which underpins the GME, can destroy key dynamical features. To illustrate this, we consider a minimal transport setup and show that its LME displays exceptional points (EPs). These singularities have been observed in a superconducting-circuit realisation of the model [1]. However, in stark contrast to experimental evidence, no EPs appear within the global approach. We then show that the EPs are a feature built into the Redfield equation, which is more accurate than the LME and the GME. Finally, we show that the local approach emerges as the weak-interaction limit of the Redfield equation, and that it entirely avoids the secular approximation.
We study the diffusive motion of a particle in a subharmonic potential of the form U(x) = |x|( c ) (0 < c < 2) driven by long-range correlated, stationary fractional Gaussian noise xi ( alpha )(t) with 0 < alpha <= 2. In the absence of the potential the particle exhibits free fractional Brownian motion with anomalous diffusion exponent alpha. While for an harmonic external potential the dynamics converges to a Gaussian stationary state, from extensive numerical analysis we here demonstrate that stationary states for shallower than harmonic potentials exist only as long as the relation c > 2(1 - 1/alpha) holds. We analyse the motion in terms of the mean squared displacement and (when it exists) the stationary probability density function. Moreover we discuss analogies of non-stationarity of Levy flights in shallow external potentials.
We introduce non-Markovian SIR epidemic spreading model inspired by the characteristics of the COVID-19, by considering discrete-and continuous-time versions. The distributions of infection intensity and recovery period may take an arbitrary form. By taking corresponding choice of these functions, it is shown that the model reduces to the classical Markovian case. The epidemic threshold is analytically determined for arbitrary functions of infectivity and recovery and verified numerically. The relevance of the model is shown by modeling the first wave of the epidemic in Italy, Spain and the UK, in the spring, 2020.
Glacial-cycle simulations of the Antarctic Ice Sheet with the Parallel Ice Sheet Model (PISM)
(2020)
The Parallel Ice Sheet Model (PISM) is applied to the Antarctic Ice Sheet over the last two glacial cycles (approximate to 210 000 years) with a resolution of 16 km. An ensemble of 256 model runs is analyzed in which four relevant model parameters have been systematically varied using full-factorial parameter sampling. Parameters and plausible parameter ranges have been identified in a companion paper (Albrecht et al., 2020) and are associated with ice dynamics, climatic forcing, basal sliding and bed deformation and represent distinct classes of model uncertainties. The model is scored against both modern and geologic data, including reconstructed grounding-line locations, elevation-age data, ice thickness, surface velocities and uplift rates. An aggregated score is computed for each ensemble member that measures the overall model-data misfit, including measurement uncertainty in terms of a Gaussian error model (Briggs and Tarasov, 2013). The statistical method used to analyze the ensemble simulation results follows closely the simple averaging method described in Pollard et al. (2016).
This analysis reveals clusters of best-fit parameter combinations, and hence a likely range of relevant model and boundary parameters, rather than individual best-fit parameters. The ensemble of reconstructed histories of Antarctic Ice Sheet volumes provides a score-weighted likely range of sea-level contributions since the Last Glacial Maximum (LGM) of 9.4 +/- 4.1m (or 6.5 +/- 2.0 x 10(6) km(3)), which is at the upper range of most previous studies. The last deglaciation occurs in all ensemble simulations after around 12 000 years before present and hence after the meltwater pulse 1A (MWP1a). Our ensemble analysis also provides an estimate of parametric uncertainty bounds for the present-day state that can be used for PISM projections of future sea-level contributions from the Antarctic Ice Sheet.
Transition path dynamics have been widely studied in chemical, physical, and technological systems. Mostly, the transition path dynamics is obtained for smooth barrier potentials, for instance, generic inverse-parabolic shapes. We here present analytical results for the mean transition path time, the distribution of transition path times, the mean transition path velocity, and the mean transition path shape in a rough inverted parabolic potential function under the driving of Gaussian white noise. These are validated against extensive simulations using the forward flux sampling scheme in parallel computations. We observe how precisely the potential roughness, the barrier height, and the noise intensity contribute to the particle transition in the rough inverted barrier potential.
The PM6:Y6 bulk-heterojunction (BHJ) blend system achieves high short-circuit current (J(SC)) values in thick photovoltaic junctions. Here we analyse these solar cells to understand the observed independence of the short-circuit current upon photoactive layer thickness. We employ a range of optoelectronic measurements and analyses, including Mott-Schottky analysis, CELIV, photoinduced absorption spectroscopy, mobility measurements and simulations, to conclude that, the invariant photocurrent for the devices with different active layer thicknesses is associated with the Y6's diffusion length exceeding 300 nm in case of a 300 nm thick cell. This is despite unintentional doping that occurs in PM6 and the associated space-charge effect, which is expected to be even more profound upon photogeneration. This extraordinarily long diffusion length - which is an order of magnitude larger than typical values for organics - dominates transport in the flat-band region of thick junctions. Our work suggests that the performance of the doped PM6:Y6 organic solar cells resembles that of inorganic devices with diffusion transport playing a pivotal role. Ultimately, this is expected to be a key requirement for the fabrication of efficient, high-photocurrent, thick organic solar cells.
Neutrophil granulocytes are essential for the first host defense. After leaving the blood circulation they migrate efficiently towards sites of inflammation. They are guided by chemoattractants released from cells within the inflammatory foci. On a cellular level, directional migration is a consequence of cellular front-rear asymmetry which is induced by the concentration gradient of the chemoattractants. The generation and maintenance of this asymmetry, however, is not yet fully understood. Here we analyzed the paths of chemotacting neutrophils with different stochastic models to gain further insight into the underlying mechanisms. Wildtype chemotacting neutrophils show an anomalous superdiffusive behavior. CXCR2 blockade and TRPC6-knockout cause the tempering of temporal correlations and a reduction of chemotaxis. Importantly, such tempering is found both in vitro and in vivo. These findings indicate that the maintenance of anomalous dynamics is crucial for chemotactic behavior and the search efficiency of neutrophils.
The motility of neutrophils and their ability to sense and to react to chemoattractants in their environment are of central importance for the innate immunity. Neutrophils are guided towards sites of inflammation following the activation of G-protein coupled chemoattractant receptors such as CXCR2 whose signaling strongly depends on the activity of Ca2+ permeable TRPC6 channels. It is the aim of this study to analyze data sets obtained in vitro (murine neutrophils) and in vivo (zebrafish neutrophils) with a stochastic mathematical model to gain deeper insight into the underlying mechanisms. The model is based on the analysis of trajectories of individual neutrophils. Bayesian data analysis, including the covariances of positions for fractional Brownian motion as well as for exponentially and power-law tempered model variants, allows the estimation of parameters and model selection. Our model-based analysis reveals that wildtype neutrophils show pure superdiffusive fractional Brownian motion. This so-called anomalous dynamics is characterized by temporal long-range correlations for the movement into the direction of the chemotactic CXCL1 gradient. Pure superdiffusion is absent vertically to this gradient. This points to an asymmetric 'memory' of the migratory machinery, which is found both in vitro and in vivo. CXCR2 blockade and TRPC6-knockout cause tempering of temporal correlations in the chemotactic gradient. This can be interpreted as a progressive loss of memory, which leads to a marked reduction of chemotaxis and search efficiency of neutrophils. In summary, our findings indicate that spatially differential regulation of anomalous dynamics appears to play a central role in guiding efficient chemotactic behavior.
SwSt 1 (PN G001.5-06.7) is a bright and compact planetary nebula containing a late [WC]-type central star. Previous studies suggested that the nebular and stellar lines are slowly changing with time. We studied new and archival optical and ultraviolet spectra of the object. The [O III] 4959 and 5007 angstrom to H beta line flux ratios decreased between about 1976 and 1997/2015. The stellar spectrum also shows changes between these epochs. We modelled the stellar and nebular spectra observed at different epochs. The analyses indicate a drop of the stellar temperature from about 42 kK to 40.5 kK between 1976 and 1993. We do not detect significant changes between 1993 and 2015. The observations show that the star performed a loop in the H-R diagram. This is possible when a shell source is activated during its post-AGB evolution. We infer that a late thermal pulse (LTP) experienced by a massive post-AGB star can explain the evolution of the central star. Such a star does not expand significantly as the result of the LTP and does not became a born-again red giant. However, the released energy can remove the tiny H envelope of the star.
The third observing run of the LIGO-Virgo Collaboration has resulted in many gravitational wave detections, including the binary neutron star merger GW190425. However, none of these events have been accompanied with an electromagnetic transient found during extensive follow-up searches. In this article, we perform new numerical-relativity simulations of binary neutron star and black hole-neutron star systems that have a chirp mass consistent with GW190425. Assuming that the GW190425's sky location was covered with sufficient accuracy during the electromagnetic follow-up searches, we investigate whether the nondetection of the kilonova is compatible with the source parameters estimated through the gravitational -wave analysis and how one can use this information to place constraints on the properties of the system. Our simulations suggest that GW190425 is incompatible with an unequal mass binary neutron star merger with a mass ratio q < 0.8 when considering stiff or moderately stiff equations of state if the binary was face on and covered by the observation. Our analysis shows that a detailed observational result for kilonovae will be useful to constrain the mass ratio of binary neutron stars in future events.
Perovskite solar cells represent one of the recent success stories in photovoltaics. The device efficiency has been steadily increasing over the past years, but further work is needed to enhance the performance, for example, through the reduction of defects to prevent carrier recombination. SCAPS-1D simulations were performed to assess efficiency limits and identify approaches to decrease the impact of defects, through the selection of an optimal hole-transport material and a hole-collecting electrode. Particular attention was given to evaluation of the influence of bulk defects within light-absorbing CH3NH3SnI3 layers. In addition, the study demonstrates the influence of interface defects at the TiO2/CH3NH3SnI3 (IL1) and CH3NH3SnI3/HTL (IL2) interfaces across the similar range of defect densities. Finally, the optimal device architecture TiO2/CH3NH3SnI3/Cu2O is proposed for the given absorber layer using the readily available Cu2O hole-transporting material with PCE = 27.95%, FF = 84.05%, V-OC = 1.02 V and J(SC) = 32.60 mA/cm(2), providing optimal performance and enhanced resistance to defects.
Chelating agents are an integral part of transition metal complex chemistry with broad biological and industrial relevance. The hexadentate chelating agent ethylenediaminetetraacetic acid (EDTA) has the capability to bind to metal ions at its two nitrogen and four of its carboxylate oxygen sites. We use resonant inelastic X-ray scattering at the 1s absorption edge of the aforementioned elements in EDTA and the iron(III)-EDTA complex to investigate the impact of the metal-ligand bond formation on the electronic structure of EDTA. Frontier orbital distortions, occupation changes, and energy shifts through metal- ligand bond formation are probed through distinct spectroscopic signatures.
In crystalline and amorphous semiconductors, the temperature-dependent Urbach energy can be determined from the inverse slope of the logarithm of the absorption spectrum and reflects the static and dynamic energetic disorder. Using recent advances in the sensitivity of photocurrent spectroscopy methods, we elucidate the temperature-dependent Urbach energy in lead halide perovskites containing different numbers of cation components. We find Urbach energies at room temperature to be 13.0 +/- 1.0, 13.2 +/- 1.0, and 13.5 +/- 1.0 meV for single, double, and triple cation perovskite. Static, temperature-independent contributions to the Urbach energy are found to be as low as 5.1 ?+/- 0.5, 4.7 +/- 0.3, and 3.3 +/- 0.9 meV for the same systems. Our results suggest that, at a low temperature, the dominant static disorder in perovskites is derived from zero-point phonon energy rather than structural disorder. This is unusual for solution-processed semiconductors but broadens the potential application of perovskites further to quantum electronics and devices.
The manufacturability of metallic alloys using laser-based additive manufacturing methods such as laser powder bed fusion has substantially improved within the last decade. However, local melting and solidification cause hierarchically structured and crystallographically textured microstructures possessing large residual stress. Such microstructures are not only the origin of mechanical anisotropy but also pose metrological challenges for the diffraction-based residual stress determination. Here we demonstrate the influence of the build orientation and the texture on the microstructure and consequently the mechanical anisotropy of as-built Inconel 718. For this purpose, we manufactured specimens with [001]/[011]-, [001]- and [011]/[11 (1) over bar]-type textures along their loading direction. In addition to changes in the Young's moduli, the differences in the crystallographic textures result in variations of the yield and ultimate tensile strengths. With this in mind, we studied the anisotropy on the micromechanical scale by subjecting the specimens to tensile loads along the different texture directions during in situ neutron diffraction experiments. In this context, the response of multiple lattice planes up to a tensile strain of 10% displayed differences in the load partitioning and the residual strain accumulation for the specimen with [011]/[(1) over bar 11]-type texture. However, the relative behavior of the specimens possessing an [001] /[011]- and [001]-type texture remained qualitatively similar. The consequences on the metrology of residual stress determination methods are discussed.
The electronic and magnetic excitations of bulk NiO have been determined using the 3A2g to 3T2g crystal-field transition at the Ni M2,3 edges with resonant inelastic x-ray scattering at 66.3- and 67.9-eV photon energies and 33-meV spectral resolution. Unambiguous assignment of the high-energy side of this state to a spin-flip satellite is achieved. We extract an effective exchange field of 89±4 meV in the 3T2g excited final state from empirical two-peak spin-flip model. The experimental data is found consistent with crystal-field model calculations using exchange fields of 60–100 meV. Full agreement with crystal-field multiplet calculations is achieved for the incident photon energy dependence of line shapes. The lower exchange parameter in the excited state as compared to the ground-state value of 120 meV is discussed in terms of the modification of the orbital occupancy (electronic effects) and of the structural dynamics: (A) With pure electronic effects, the lower exchange energy is attributed to the reduction in effective hopping integral. (B) With no electronic effects, we use the S = 1 Heisenberg model of antiferromagnetism to derive a second-nearest-neighbor exchange constant J2 = 14.8±0.6 meV. Based on the linear correlation between J2 and the lattice parameter from pressure-dependent experiments, an upper limit of 2% local Ni-O bond elongation during the femtosecond scattering duration is derived.
Perovskite semiconductors differ from most inorganic and organic semiconductors due to the presence of mobile ions in the material. Although the phenomenon is intensively investigated, important questions such as the exact impact of the mobile ions on the steady-state power conversion efficiency (PCE) and stability remain. Herein, a simple method is proposed to estimate the efficiency loss due to mobile ions via "fast-hysteresis" measurements by preventing the perturbation of mobile ions out of their equilibrium position at fast scan speeds (approximate to 1000 V s(-1)). The "ion-free" PCE is between 1% and 3% higher than the steady-state PCE, demonstrating the importance of ion-induced losses, even in cells with low levels of hysteresis at typical scan speeds (approximate to 100mv s(-1)). The hysteresis over many orders of magnitude in scan speed provides important information on the effective ion diffusion constant from the peak hysteresis position. The fast-hysteresis measurements are corroborated by transient charge extraction and capacitance measurements and numerical simulations, which confirm the experimental findings and provide important insights into the charge carrier dynamics. The proposed method to quantify PCE losses due to field screening induced by mobile ions clarifies several important experimental observations and opens up a large range of future experiments.
Focusing on transient chaos
(2022)
Recent advances in the field of complex, transiently chaotic dynamics are reviewed, based on the results published in the focus issue of J. Phys. Complex. on this topic. One group of achievements concerns network dynamics where transient features are intimately related to the degree and stability of synchronization, as well as to the network topology. A plethora of various applications of transient chaos are described, ranging from the collective motion of active particles, through the operation of power grids, cardiac arrhythmias, and magnetohydrodynamical dynamos, to the use of machine learning to predict time evolutions. Nontraditional forms of transient chaos are also explored, such as the temporal change of the chaoticity in the transients (called doubly transient chaos), as well as transients in systems subjected to parameter drift, the paradigm of which is climate change.
The electron-phonon scattering is one of the main microscopic mechanisms responsible for the spin-flip in the transient state of ultrafast demagnetization. Here, we present an experimental determination of the temperature-dependent electron-phonon scattering rate in Gd. Using a static x-ray emission spectroscopy method, where the reduction of the decay peak intensities when increasing the temperature is quantified, we measure independently the electron-phonon scattering rate for the 5d and the 4f electrons. We deduce the temperature dependence of scattering for the 5d electrons, while no effect on the phonon population is observed for the 4f electrons. Our results suggest that the ultrafast magnetization dynamics in Gd is triggered by the spin-flip in the 5d electrons. We also evidence the existence of a temperature threshold, above which spin-flip scattering of the 5d electrons takes place. We deduce that during the transient state of ultrafast demagnetization, the exchange energy between 5d electrons has to be overcome before the microscopic electron-phonon scattering process can occur.
Anomalous diffusion with a power-law time dependence vertical bar R vertical bar(2)(t) similar or equal to t(alpha i) of the mean squared displacement occurs quite ubiquitously in numerous complex systems. Often, this anomalous diffusion is characterised by crossovers between regimes with different anomalous diffusion exponents alpha(i). Here we consider the case when such a crossover occurs from a first regime with alpha(1) to a second regime with alpha(2) such that alpha(2) > alpha(1), i.e., accelerating anomalous diffusion. A widely used framework to describe such crossovers in a one-dimensional setting is the bi-fractional diffusion equation of the so-called modified type, involving two time-fractional derivatives defined in the Riemann-Liouville sense. We here generalise this bi-fractional diffusion equation to higher dimensions and derive its multidimensional propagator (Green's function) for the general case when also a space fractional derivative is present, taking into consideration long-ranged jumps (Levy flights). We derive the asymptotic behaviours for this propagator in both the short- and long-time as well the short- and long-distance regimes. Finally, we also calculate the mean squared displacement, skewness and kurtosis in all dimensions, demonstrating that in the general case the non-Gaussian shape of the probability density function changes.
In recent years, gravitational-wave astronomy has motivated increasingly accurate perturbative studies of gravitational dynamics in compact binaries. This in turn has enabled more detailed analyses of the dynamical black holes in these systems. For example, Pound et al. [Phys. Rev. Lett. 124, 021101 (2020)] recently computed the surface area of a Schwarzschild black hole's apparent horizon, perturbed by an orbiting body, to second order in the binary's mass ratio. In this paper, we take that as the starting point for a comprehensive study of a perturbed Schwarzschild black hole's apparent and event horizon at second perturbative order, deriving generic formulas for the first- and second-order corrections to the horizons' radial profiles, surface areas, Hawking masses, and intrinsic curvatures. We find that the two horizons are remarkably similar, and that any teleological behavior of the event horizon is suppressed in several ways. Critically, we establish that at all orders, the perturbed event horizon in a small-mass-ratio binary is effectively localized in time. Even more pointedly, the event horizon is identical to the apparent horizon at linear order regardless of the source of perturbation, implying that the seemingly teleological "tidal lead," previously observed in linearly perturbed event horizons, is not genuinely teleological in origin. The two horizons do generically differ at second order, but their Hawking masses remain identical, implying that the event horizon obeys the same energy-flux balance law as the apparent horizon. At least in the case of a binary system, the difference between their surface areas remains extremely small even in the late stages of inspiral. In the course of our analysis, we also numerically illustrate puzzling behavior in the black hole's motion around the binary's center of mass.
The stratosphere is one of the main potential sources for subseasonal to seasonal predictability in midlatitudes in winter. The ability of an atmospheric model to realistically simulate the stratospheric dynamics is essential in order to move forward in the field of seasonal predictions in midlatitudes. Earlier studies with the ICOsahedral Nonhydrostatic atmospheric model (ICON) point out that stratospheric westerlies in ICON are underestimated. This is the first extensive study on the evaluation of Northern Hemisphere stratospheric winter circulation with ICON in numerical weather prediction (NWP) mode. Seasonal experiments with the default setup are able to reproduce the basic climatology of the stratospheric polar vortex. However, westerlies are too weak and major stratospheric warmings too frequent in ICON. Both a reduction of the nonorographic, and a reduction of the orographic gravity wave and wake drag lead to a strengthening of the stratospheric vortex and a bias reduction, in particular in January. However, the effect of the nonorographic gravity wave drag scheme on the stratosphere is stronger. Stratosphere-troposphere coupling is intensified and more realistic due to a reduced gravity wave drag. Furthermore, an adjustment of the subgrid-scale orographic drag parameterization leads to a significant error reduction in the mean sea level pressure. As a result of these findings, we present our current suggested improved setup for seasonal experiments with ICON-NWP. <br /> Plain Language Summary Although seasonal forecasts for midlatitudes have the potential to be highly beneficial to the public sector, they are still characterized by a large amount of uncertainty. Exact simulations of the circulation in the stratosphere can help to improve tropospheric predictability on seasonal time scales. For this reason, we investigate how well the new German atmospheric model is able to simulate the stratospheric circulation. The model reproduces the basic behavior of the Northern Hemisphere stratospheric polar vortex, but the westerly circulation in winter is underestimated. The stratospheric circulation is influenced by gravity waves that exert drag on the flow. These processes are only partly physically represented in the model, but are very important and are hence parameterized. By adjusting the parameterizations for the gravity wave drag, the stratospheric polar vortex is strengthened, thereby yielding a more realistic stratospheric circulation. In addition, the altered parameterizations improve the simulated surface pressure pattern. Based upon this, we present our current suggested improved model setup for seasonal experiments.
The Dirac point of a topological surface state (TSS) is protected against gapping by time-reversal symmetry. Conventional wisdom stipulates, therefore, that only through magnetisation may a TSS become gapped. However, non-magnetic gaps have now been demonstrated in Bi2Se3 systems doped with Mn or In, explained by hybridisation of the Dirac cone with induced impurity resonances. Recent photoemission experiments suggest that an analogous mechanism applies even when Bi2Se3 is surface dosed with Au. Here, we perform a systematic spin- and angle-resolved photoemission study of Au-dosed Bi2Se3. Although there are experimental conditions wherein the TSS appears gapped due to unfavourable photoemission matrix elements, our photon-energy-dependent spectra unambiguously demonstrate the robustness of the Dirac cone against high Au coverage. We further show how the spin textures of the TSS and its accompanying surface resonances remain qualitatively unchanged following Au deposition, and discuss the mechanism underlying the suppression of the spectral weight.
Tautomerism is one of the most important forms of isomerism, owing to the facile interconversion between species and the large differences in chemical properties introduced by the proton transfer connecting the tautomers. Spectroscopic techniques are often used for the characterization of tautomers. In this context, separating the overlapping spectral response of coexisting tautomers is a long-standing challenge in chemistry. Here, we demonstrate that by using resonant inelastic X-ray scattering tuned to the core excited states at the site of proton exchange between tautomers one is able to experimentally disentangle the manifold of valence excited states of each tautomer in a mixture. The technique is applied to the prototypical keto-enol equilibrium of 3-hydroxypyridine in aqueous solution. We detect transitions from the occupied orbitals into the LUMO for each tautomer in solution, which report on intrinsic and hydrogen-bond-induced orbital polarization within the pi and sigma manifolds at the proton-transfer site.
As the use of free electron laser (FEL) sources increases, so do the findings mentioning non-linear phenomena occurring at these experiments, such as saturable absorption, induced transparency and scattering breakdowns. These are well known among the laser community, but are still rarely understood and expected among the X-ray community and to date lack tools and theories to accurately predict the respective experimental parameters and results. We present a simple theoretical framework to access short X-ray pulse induced light- matter interactions which occur at intense short X-ray pulses as available at FEL sources. Our approach allows to investigate effects such as saturable absorption, induced transparency and scattering suppression, stimulated emission, and transmission spectra, while including the density of state influence relevant to soft X-ray spectroscopy in, for example, transition metal complexes or functional materials. This computationally efficient rate model based approach is intuitively adaptable to most solid state sample systems in the soft X-ray spectrum with the potential to be extended for liquid and gas sample systems as well. The feasibility of the model to estimate the named effects and the influence of the density of state is demonstrated using the example of CoPd transition metal systems at the Co edge. We believe this work is an important contribution for the preparation, performance, and understanding of FEL based high intensity and short pulse experiments, especially on functional materials in the soft X-ray spectrum.
Suppression of the TeV Pair-beam-Plasma Instability by a Tangled Weak Intergalactic Magnetic Field
(2022)
We study the effect of a tangled sub-fG level intergalactic magnetic field (IGMF) on the electrostatic instability of a blazar-induced pair beam. Sufficiently strong IGMF may significantly deflect the TeV pair beams, which would reduce the flux of secondary cascade emission below the observational limits. A similar flux reduction may result from the electrostatic beam-plasma instability, which operates the best in the absence of IGMF. Considering IGMF with correlation lengths smaller than a kiloparsec, we find that weak magnetic fields increase the transverse momentum of the pair-beam particles, which dramatically reduces the linear growth rate of the electrostatic instability and hence the energy-loss rate of the pair beam. We show that the beam-plasma instability is eliminated as an effective energy-loss agent at a field strength three orders of magnitude below that needed to suppress the secondary cascade emission by magnetic deflection. For intermediate-strength IGMF, we do not know a viable process to explain the observed absence of GeV-scale cascade emission.
Nanostructured silicon and silicon-aluminum compounds are synthesized by a novel synthesis strategy based on spark plasma sintering (SPS) of silicon nanopowder, mesoporous silicon (pSi), and aluminum nanopowder. The interplay of metal-assisted crystallization and inherent porosity is exploited to largely suppress thermal conductivity. Morphology and temperature-dependent thermal conductivity studies allow us to elucidate the impact of porosity and nanostructure on the macroscopic heat transport. Analytic electron microscopy along with quantitative image analysis is applied to characterize the sample morphology in terms of domain size and interpore distance distributions. We demonstrate that nanostructured domains and high porosity can be maintained in densified mesoporous silicon samples. In contrast, strong grain growth is observed for sintered nanopowders under similar sintering conditions. We observe that aluminum agglomerations induce local grain growth, while aluminum diffusion is observed in porous silicon and dispersed nanoparticles. A detailed analysis of the measured thermal conductivity between 300 and 773 K allows us to distinguish the effect of reduced thermal conductivity caused by porosity from the reduction induced by phonon scattering at nanosized domains. With a modified Landauer/Lundstrom approach the relative thermal conductivity and the scattering length are extracted. The relative thermal conductivity confirms the applicability of Kirkpatrick's effective medium theory. The extracted scattering lengths are in excellent agreement with the harmonic mean of log-normal distributed domain sizes and the interpore distances combined by Matthiessen's rule.
Properties of Arctic aerosol in the transition between Arctic haze to summer season derived by lidar
(2023)
During the Arctic haze period, the Arctic troposphere consists of larger, yet fewer, aerosol particles than during the summer (Tunved et al., 2013; Quinn et al., 2007). Interannual variability (Graßl and Ritter, 2019; Rinke et al., 2004), as well as unknown origins (Stock et al., 2014) and properties of aerosol complicate modeling these annual aerosol cycles. This thesis investigates the modification of the microphysical properties of Arctic aerosols in the transition from Arctic haze to the summer season. Therefore, lidar measurements of Ny-Ålesund from April 2021 to the end of July 2021 are evaluated based on the aerosols’ optical properties. An overview of those properties will be provided. Furthermore, parallel radiosonde data is considered for indication of hygroscopic growth.
The annual aerosol cycle in 2021 differs from expectations based on previous studies from Tunved et al. (2013) and Quinn et al. (2007). Developments of backscatter, extinction, aerosol depolarisation, lidar ratio and color ratio show a return of the Arctic haze in May. The haze had already reduced in April, but regrew afterwards.
The average Arctic aerosol displays hygroscopic behaviour, meaning growth due to water uptake. To determine such a behaviour is generally laborious because various meteorological circumstances need to be considered. Two case studies provide further information on these possible events. In particular, a day with a rare ice cloud and with highly variable water cloud layers is observed.
Supernova remnants are considered to be the primary sources of galactic cosmic rays. These cosmic rays are assumed to be accelerated by the diffusive shock acceleration mechanism, specifically at shocks in the remnants. Particularly in the core-collapse scenario, these supernova remnant shocks expand inside the wind-blown bubbles structured by massive progenitors during their lifetime. Therefore, the complex environment of wind bubbles can influence the particle acceleration and radiation from the remnants. Further, the evolution of massive stars depends on their Zero Age Main Sequence mass, rotation, and metallicity. Consequently, the structures of the wind bubbles generated during the lifetime of massive stars should be considerably different. Hence, the particle acceleration in the core-collapse supernova remnants should vary, not only from the remnants evolving in the uniform environment but also from one another, depending on their progenitor stars.
A core-collapse supernova remnant with a very massive 60 𝑀 ⊙ progenitor star has been considered to study the particle acceleration at the shock considering Bohm-like diffusion. This dissertation demonstrates the modification in particle acceleration and radiation while the remnant propagates through different regions of the wind bubble by impacts from the profiles of gas density, the temperature of the bubble and the magnetic field structure. Subsequently, in this thesis, I discuss the impacts of the non-identical ambient environment of core-collapse supernova remnants on particle spectra and the non-thermal emissions, considering 20 𝑀 ⊙ and 60 𝑀⊙ massive progenitors having different evolutionary tracks. Additionally, I also analyse the effect of cosmic ray streaming instabilities on particle spectra.
To model the particle acceleration in the remnants, I have performed simulations in one-dimensional spherical symmetry using RATPaC code. The transport equation for cosmic rays and magnetic turbulence in test-particle approximation, along with the induction equation for the evolution of the large-scale magnetic field, have been solved simultaneously with the hydrodynamic equations for the expansion of remnants inside the pre-supernova circumstellar medium.
The results from simulations describe that the spectra of accelerated particles in supernova remnants are regulated by density fluctuations, temperature variations, the large-scale magnetic field configuration and scattering turbulence. Although the diffusive shock acceleration mechanism at supernova remnant shock predicts the spectral index of 2 for the accelerated non-thermal particles, I have obtained the particle spectra that deviate from this prediction, in the core-collapse scenario. I have found that the particle spectral index reaches 2.5 for the supernova remnant with 60 𝑀 ⊙ progenitor when the remnant resides inside the shocked wind region of the wind bubble, and this softness persists at later evolutionary stages even with Bohm-like diffusion for accelerated particles. However, the supernova remnant with 20 𝑀 ⊙ progenitor does not demonstrate persistent softness in particle spectra from the influence of the hydrodynamics of the corresponding wind bubble. At later stages of evolution, the particle spectra illustrate softness at higher energies for both remnants as the consequence of the escape of high-energy particles from the remnants while considering the cosmic ray streaming instabilities. Finally, I have probed the emission morphology of remnants that varies depending on the progenitors, particularly in earlier evolutionary stages. This dissertation provides insight into different core-collapse remnants expanding inside wind bubbles, for instance, the calculated gamma-ray spectral index from the supernova remnant with 60 𝑀 ⊙ progenitor at later evolutionary stages is consistent with that of the observed supernova remnants expanding in dense molecular clouds.
In this work, it is revealed how the photoinduced deformation of azobenzene containing polymers relates to the local direction of optomechanical stresses generated during irradiation with interference patterns (IPs). It can be substantiated by the modeling approach proposed by Saphiannikova et al., which describes the directional photodeformations in glassy side-chain azobenzene polymers, and proves that these deformations arise from the reorientation of rigid backbone segments along the light polarization direction. In experiments and modeling, surface relief gratings in pre-elongated photosensitive colloids of few micrometers length are inscribed using different IPs such as SS, PP, +/- 45, SP, RL, and LR. The deformation of colloidal particles is studied in situ, whereby the local variation of polymer topography is assigned to the local distribution of the electrical field vector for all IPs. Experimentally observed shapes are reproduced exactly with modeling azopolymer samples as visco-plastic bodies in the finite element software ANSYS. Orientation approach correctly predicts local variations of the main axis of light-induced stress in each interference pattern for both initially isotropic and highly oriented materials. With this work, it is suggested that the orientation approach implements a self-sufficient and convincing mechanism to describe photoinduced deformation in azopolymer films that in principle does not require auxiliary assumptions.
In this work, the fabrication and characterization of a simple, inexpensive, and effective microfluidic paper analytic device (mu PAD) for monitoring DNA samples is reported. The glass microfiber-based chip has been fabricated by a new wax-based transfer-printing technique and an electrode printing process. It is capable of moving DNA effectively in a time-dependent fashion. The nucleic acid sample is not damaged by this process and is accumulated in front of the anode, but not directly on the electrode. Thus, further DNA processing is feasible. The system allows the DNA to be purified by separating it from other components in sample mixtures such as proteins. Furthermore, it is demonstrated that DNA can be moved through several layers of the glass fiber material. This proof of concept will provide the basis for the development of rapid test systems, e.g., for the detection of pathogens in water samples.
The increase in the performance of organic solar cells observed over the past few years has reinvigorated the search for a deeper understanding of the loss and extraction processes in this class of device. A detailed knowledge of the density of free charge carriers under different operating conditions and illumination intensities is a prerequisite to quantify the recombination and extraction dynamics. Differential charging techniques are a promising approach to experimentally obtain the charge carrier density under the aforementioned conditions. In particular, the combination of transient photovoltage and photocurrent as well as impedance and capacitance spectroscopy have been successfully used in past studies to determine the charge carrier density of organic solar cells. In this Tutorial, these experimental techniques will be discussed in detail, highlighting fundamental principles, practical considerations, necessary corrections, advantages, drawbacks, and ultimately their limitations. Relevant references introducing more advanced concepts will be provided as well. Therefore, the present Tutorial might act as an introduction and guideline aimed at new prospective users of these techniques as well as a point of reference for more experienced researchers. Published under an exclusive license by AIP Publishing.
Cr(CO)(6) was investigated by X-ray absorption spectroscopy. The spectral signature at the metal edge provides information about the back-bonding of the metal in this class of complexes. Among the processes it participates in is ligand substitution in which a carbonyl ligand is ejected through excitation to a metal to ligand charge transfer (MLCT) band. The unsaturated carbonyl Cr(CO)(5) is stabilized by solution media in square pyramidal geometry and further reacts with the solvent. Multi-site-specific probing after photoexcitation was used to investigate the ligand substitution photoreaction process which is a common first step in catalytic processes involving metal carbonyls. The data were analysed with the aid of TD-DFT computations for different models of photoproducts and signatures for ligand rearrangement after substitution were found. The rearrangement was found to occur in about 790 ps in agreement with former studies of the photoreaction.
How does a systematic time-dependence of the diffusion coefficient D(t) affect the ergodic and statistical characteristics of fractional Brownian motion (FBM)? Here, we answer this question via studying the characteristics of a set of standard statistical quantifiers relevant to single-particle-tracking (SPT) experiments. We examine, for instance, how the behavior of the ensemble- and time-averaged mean-squared displacements-denoted as the standard MSD < x(2)(Delta)> and TAMSD <<(delta(2)(Delta))over bar>> quantifiers-of FBM featuring < x(2) (Delta >> = <<(delta(2)(Delta >)over bar>> proportional to Delta(2H) (where H is the Hurst exponent and Delta is the [lag] time) changes in the presence of a power-law deterministically varying diffusivity D-proportional to(t) proportional to t(alpha-1) -germane to the process of scaled Brownian motion (SBM)-determining the strength of fractional Gaussian noise. The resulting compound "scaled-fractional" Brownian motion or FBM-SBM is found to be nonergodic, with < x(2)(Delta >> proportional to Delta(alpha+)(2H)(-1) and <(delta 2(Delta >) over bar > proportional to Delta(2H). We also detect a stalling behavior of the MSDs for very subdiffusive SBM and FBM, when alpha + 2H - 1 < 0. The distribution of particle displacements for FBM-SBM remains Gaussian, as that for the parent processes of FBM and SBM, in the entire region of scaling exponents (0 < alpha < 2 and 0 < H < 1). The FBM-SBM process is aging in a manner similar to SBM. The velocity autocorrelation function (ACF) of particle increments of FBM-SBM exhibits a dip when the parent FBM process is subdiffusive. Both for sub- and superdiffusive FBM contributions to the FBM-SBM process, the SBM exponent affects the long-time decay exponent of the ACF. Applications of the FBM-SBM-amalgamated process to the analysis of SPT data are discussed. A comparative tabulated overview of recent experimental (mainly SPT) and computational datasets amenable for interpretation in terms of FBM-, SBM-, and FBM-SBM-like models of diffusion culminates the presentation. The statistical aspects of the dynamics of a wide range of biological systems is compared in the table, from nanosized beads in living cells, to chromosomal loci, to water diffusion in the brain, and, finally, to patterns of animal movements.
A panoply of new tools for tracking single particles and molecules has led to an explosion of experimental data, leading to novel insights into physical properties of living matter governing cellular development and function, health and disease. In this Perspective, we present tools to investigate the dynamics and mechanics of living systems from the molecular to cellular scale via single-particle techniques. In particular, we focus on methods to measure, interpret, and analyse complex data sets that are associated with forces, materials properties, transport, and emergent organisation phenomena within biological and soft-matter systems. Current approaches, challenges, and existing solutions in the associated fields are outlined in order to support the growing community of researchers at the interface of physics and the life sciences. Each section focuses not only on the general physical principles and the potential for understanding living matter, but also on details of practical data extraction and analysis, discussing limitations, interpretation, and comparison across different experimental realisations and theoretical frameworks. Particularly relevant results are introduced as examples. While this Perspective describes living matter from a physical perspective, highlighting experimental and theoretical physics techniques relevant for such systems, it is also meant to serve as a solid starting point for researchers in the life sciences interested in the implementation of biophysical methods.
A symmetry-breaking mechanism is investigated that creates bistability between fully and partially synchronized states in oscillator networks. Two populations of oscillators with unimodal frequency distribution and different amplitudes, in the presence of weak global coupling, are shown to simplify to a modular network with asymmetrical coupling. With increasing the coupling strength, a synchronization transition is observed with an isolated fully synchronized state. The results are interpreted theoretically in the thermodynamic limit and confirmed in experiments with chemical oscillators.
The effects of thermal processing on the micro- and nanostructural features and thus also on the relaxor-ferroelectric properties of a P(VDF-TrFE-CFE) terpolymer were investigated in detail by means of dielectric experiments, such as dielectric relaxation spectroscopy (DRS), dielectric hysteresis loops, and thermally stimulated depolarization currents (TSDCs). The results were correlated with those obtained from differential scanning calorimetry (DSC), wide-angle X-ray diffraction (WAXD), and Fourier-transform infrared spectroscopy (FTIR). The results from DRS and DSC show that annealing reduces the Curie transition temperature of the terpolymer, whereas the results from WAXD scans and FTIR spectra help to understand the shift in the Curie transition temperatures as a result of reducing the ferroelectric phase fraction, which by default exists even in terpolymers with relatively high CFE contents. In addition, the TSDC traces reveal that annealing has a similar effect on the midtemperature transition by altering the fraction of constrained amorphous phase at the interphase between the crystalline and the amorphous regions. Changes in the transition temperatures are in turn related to the behavior of the hysteresis curves on differently heat-treated samples. During heating, evolution of the hysteresis curves from ferroelectric to relaxor-ferroelectric, first exhibiting single hysteresis loops and then double hysteresis loops near the Curie transition of the sample, is observed. When comparing the dielectric-hysteresis loops obtained at various temperatures, we find that annealed terpolymer films show higher electric-displacement values and lower coercive fields than the nonannealed sample, irrespective of the measurement temperature, and also exhibit ideal relaxor- ferroelectric behavior at ambient temperatures, which makes them excellent candidates for applications at or near room temperature. By tailoring the annealing conditions, it has been shown that the application temperature could be increased by fine tuning the induced micro- and nanostructures.
We consider a system of two spins under a scanning tunneling microscope bias and derive its master equation. We find that the tunneling elements to the electronic contacts (tip and substrate) generate an exchange interaction between the spins as well as a Dzyaloshinskii-Moriya interaction in the presence of spin-orbit coupling. The tunnel current spectrum then shows additional lines compared to conventional spin-resonance experiments. When the spins have degenerate Larmor frequencies and equal tunneling amplitudes (without spin orbit), there is a dark state with a vanishing decay rate. The coupling to the electronic environment generates significant spin-spin entanglement via the dark state, even if the initial state is nonentangled.
Excitable solitons
(2020)
Excitable pulses are among the most widespread dynamical patterns that occur in many different systems, ranging from biological cells to chemical reactions and ecological populations. Traditionally, the mutual annihilation of two colliding pulses is regarded as their prototypical signature. Here we show that colliding excitable pulses may exhibit solitonlike crossover and pulse nucleation if the system obeys a mass conservation constraint. In contrast to previous observations in systems without mass conservation, these alternative collision scenarios are robustly observed over a wide range of parameters. We demonstrate our findings using a model of intracellular actin waves since, on time scales of wave propagations over the cell scale, cells obey conservation of actin monomers. The results provide a key concept to understand the ubiquitous occurrence of actin waves in cells, suggesting why they are so common, and why their dynamics is robust and long-lived.
How different microscopic mechanisms of ultrafast spin dynamics coexist and interplay is not only relevant for the development of spintronics but also for the thorough description of physical systems out-of-equilibrium. In pure crystalline ferromagnets, one of the main microscopic mechanism of spin relaxation is the electron-phonon (el-ph) driven spin-flip, or Elliott-Yafet, scattering. Unexpectedly, recent experiments with ferro- and ferrimagnetic alloys have shown different dynamics for the different sublattices. These distinct sublattice dynamics are contradictory to the Elliott-Yafet scenario. In order to rationalize this discrepancy, it has been proposed that the intra- and intersublattice exchange interaction energies must be considered in the microscopic demagnetization mechanism, too. Here, using a temperature-dependent x-ray emission spectroscopy (XES) method, we address experimentally the element specific el-ph angular momentum transfer rates, responsible for the spin-flips in the respective (sub)lattices of Fe20Ni80, Fe50Ni50 and pure nickel single crystals. We establish how the deduced rate evolution with the temperature is linked to the exchange coupling constants reported for different alloy stoichiometries and how sublattice exchange energies threshold the related el-ph spin-flip channels. Thus, these results evidence that the Elliott-Yafet spin-flip scattering, thresholded by sublattice exchange energies, is the relevant microscopic process to describe sublattice dynamics in alloys and elemental magnetic systems.
Multi-messenger observations of compact binary mergers provide a new way to constrain the nature of dark matter that may accumulate in and around neutron stars. In this article, we extend the infrastructure of our numerical-relativity code BAM to enable the simulation of neutron stars that contain an additional mirror dark matter component. We perform single star tests to verify our code and the first binary neutron star simulations of this kind. We find that the presence of dark matter reduces the lifetime of the merger remnant and favors a prompt collapse to a black hole. Furthermore, we find differences in the merger time for systems with the same total mass and mass ratio, but different amounts of dark matter. Finally, we find that electromagnetic signals produced by the merger of binary neutron stars admixed with dark matter are very unlikely to be as bright as their dark matter-free counterparts. Given the increased sensitivity of multi-messenger facilities, our analysis gives a new perspective on how to probe the presence of dark matter.