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A stellar census in globular clusters with MUSE: A spectral catalogue of emission-line sources
(2019)
Aims. Globular clusters produce many exotic stars due to a much higher frequency of dynamical interactions in their dense stellar environments. Some of these objects were observed together with several hundred thousand other stars in our MUSE survey of 26 Galactic globular clusters. Assuming that at least a few exotic stars have exotic spectra (i.e. spectra that contain emission lines), we can use this large spectroscopic data set of over a million stellar spectra as a blind survey to detect stellar exotica in globular clusters. Methods. To detect emission lines in each spectrum, we modelled the expected shape of an emission line as a Gaussian curve. This template was used for matched filtering on the di fferences between each observed 1D spectrum and its fitted spectral model. The spectra with the most significant detections of H alpha emission are checked visually and cross-matched with published catalogues. Results. We find 156 stars with H alpha emission, including several known cataclysmic variables (CV) and two new CVs, pulsating variable stars, eclipsing binary stars, the optical counterpart of a known black hole, several probable sub-subgiants and red stragglers, and 21 background emission-line galaxies. We find possible optical counterparts to 39 X-ray sources, as we detected H alpha emission in several spectra of stars that are close to known positions of Chandra X-ray sources. This spectral catalogue can be used to supplement existing or future X-ray or radio observations with spectra of potential optical counterparts to classify the sources.
Lévy flights are paradigmatic generalised random walk processes, in which the independent stationary increments—the 'jump lengths'—are drawn from an -stable jump length distribution with long-tailed, power-law asymptote. As a result, the variance of Lévy flights diverges and the trajectory is characterised by occasional extremely long jumps. Such long jumps significantly decrease the probability to revisit previous points of visitation, rendering Lévy flights efficient search processes in one and two dimensions. To further quantify their precise property as random search strategies we here study the first-passage time properties of Lévy flights in one-dimensional semi-infinite and bounded domains for symmetric and asymmetric jump length distributions. To obtain the full probability density function of first-passage times for these cases we employ two complementary methods. One approach is based on the space-fractional diffusion equation for the probability density function, from which the survival probability is obtained for different values of the stable index and the skewness (asymmetry) parameter . The other approach is based on the stochastic Langevin equation with -stable driving noise. Both methods have their advantages and disadvantages for explicit calculations and numerical evaluation, and the complementary approach involving both methods will be profitable for concrete applications. We also make use of the Skorokhod theorem for processes with independent increments and demonstrate that the numerical results are in good agreement with the analytical expressions for the probability density function of the first-passage times.
Precipitation patterns and extremes are significantly influenced by various climatic factors and large-scale atmospheric circulation patterns. This study uses wavelet coherence analysis to detect significant interannual and interdecadal oscillations in monthly precipitation extremes across India and their teleconnections to three prominent climate indices, namely, Nino 3.4, Pacific Decadal Oscillation, and Indian Ocean Dipole (IOD). Further, partial wavelet coherence analysis is used to estimate the standalone relationship between the climate indices and precipitation after removing the effect of interdependency. The wavelet analysis of monthly precipitation extremes at 30 different locations across India reveals that (a) interannual (2-8 years) and interdecadal (8-32 years) oscillations are statistically significant, and (b) the oscillations vary in both time and space. The results from the partial wavelet coherence analysis reveal that Nino 3.4 and IOD are the significant drivers of Indian precipitation at interannual and interdecadal scales. Intriguingly, the study also confirms that the strength of influence of large-scale atmospheric circulation patterns on Indian precipitation extremes varies with spatial physiography of the region.
Understanding and disentangling photophysical properties of long-lived photoexcitations in bulk heterojunction (BHJ) solar cells, which contribute mostly to photocurrent, provide essential guidelines to their improvement. However, to construct improved physical models, their rational design relies on reliable measurement techniques for charge recombination. Here, we combine photocurrent and photoinduced absorption spectroscopy (PCPIA) to directly probe the free carrier concentration and investigate loss mechanisms of long-lived excitations in nearly 10% efficient PPDT2FBT/PC70BM BHJ solar cells under steady-state operational conditions. From the PCPIA data obtained under open- circuit and short-circuit conditions, the absorption cross section and the concentration of photoexcitations are obtained. This material system exhibits an exceptionally low bimolecular recombination rate, about 300 times smaller than the diffusion-controlled electron and hole encounter rate. Furthermore, we observe that the fill factor is limited by losses originating from long-lived photoexcitations undergoing dispersive bimolecular recombination.
We predict the recoil-induced molecular dissociation in hard-x-ray photoionization. The recoil effect is caused by electronic and photon momentum exchange with the molecule. We show the strong role of relativistic effects for the studied molecular fragmentation. The recoil-induced fragmentation of the molecule is caused by elongation of the bond due to the vibrational recoil effect and because of the centrifugal force caused by the rotational recoil. The calculations of the x-ray photoelectron spectra of the H-2 and NO molecules show that the predicted effects can be observed in high-energy synchrotrons like SOLEIL, SPring-8, PETRA, and XFEL SACLA. The relativistic effect enhances the recoil momentum transfer and makes it strongly sensitive to the direction of ejection of the fast photoelectron with respect to the photon momentum.
Both climate-change damages and climate-change mitigation will incur economic costs. While the risk of severe damages increases with the level of global warming (Dell et al., 2014; IPCC, 2014b, 2018; Lenton et al., 2008), mitigating costs increase steeply with more stringent warming limits (IPCC, 2014a; Luderer et al., 2013; Rogelj et al., 2015). Here, we show that the global warming limit that minimizes this century's total economic costs of climate change lies between 1.9 and 2 ∘C, if temperature changes continue to impact national economic growth rates as observed in the past and if instantaneous growth effects are neither compensated nor amplified by additional growth effects in the following years. The result is robust across a wide range of normative assumptions on the valuation of future welfare and inequality aversion. We combine estimates of climate-change impacts on economic growth for 186 countries (applying an empirical damage function from Burke et al., 2015) with mitigation costs derived from a state-of-the-art energy–economy–climate model with a wide range of highly resolved mitigation options (Kriegler et al., 2017; Luderer et al., 2013, 2015). Our purely economic assessment, even though it omits non-market damages, provides support for the international Paris Agreement on climate change. The political goal of limiting global warming to “well below 2 degrees” is thus also an economically optimal goal given above assumptions on adaptation and damage persistence.
In this paper, we explore the time-energy domain quantum-classical transition comparing a classical pump-probe experiment on a diatomic molecule to its quantum enhanced counterpart, where the pump and probe pulses are substituted by the signal and idler beams of a spontaneous parametric down conversion (SPDC) source. Absorption of biphotons generated with SPDC exploits quantum time-energy entanglement to enhance the overall yield and selectivity of the process, when compared with a classical pump-probe setup, while maintaining femtosecond time resolution. We systematically study the effects of correlation strength on process efficiency and selectivity, comparing the results to classical pump-probe spectra. An excitation scheme to improve the yield based on spectral narrowing of biphotons is shown. The results indicate that the quantum improvements in yield are caused by a more efficient use of the total power available for the process.
In this Letter, we propose that the x-ray and the TeV observations in the vicinity of Geminga can be understood in the framework of anisotropic diffusion of injected electrons or positrons. This interpretation only requires the turbulence in the vicinity of Geminga to be sub-Alfvenic with the local mean magnetic field direction approximately aligned with our line of sight towards Geminga, without invoking extreme conditions for the environment, such as an extremely small diffusion coefficient and a weak magnetic field of submicrogauss as suggested in previous literature.
Charge extraction methods are popular for measuring the charge carrier density in thin film organic solar cells and to draw conclusions about the order and coefficient of nongeminate charge recombination. However, results from such studies may be falsified by inhomogeneous steady state carrier profiles or surface recombination. Here, we present a detailed drift-diffusion study of two charge extraction methods, bias-assisted charge extraction (BACE) and time-delayed collection field (TDCF). Simulations are performed over a wide range of the relevant parameters. Our simulations reveal that both charge extraction methods provide reliable information about the recombination order and coefficient if the measurements are performed under appropriate conditions. However, results from BACE measurements may be easily affected by surface recombination, in particular for small active layer thicknesses and low illumination densities. TDCF, on the other hand, is more robust against surface recombination due to its transient nature but also because it allows for a homogeneous high carrier density to be inserted into the active layer. Therefore, TDCF is capable to provide meaningful information on the order and coefficient of recombination even if the model conditions are not exactly fulfilled. We demonstrate this for an only 100 nm thick layer of a highly efficient nonfullerene acceptor (NFA) blend, comprising the donor polymer PM6 and the NFA Y6. TDCF measurements were performed as a function of delay time for different laser fluences and bias conditions. The full set of data could be consistently fitted by a strict second order recombination process, with a bias- and fluence-independent bimolecular recombination coefficient k(2) = 1.7 x 10(-17)m(3) s(-1). BACE measurements performed on the very same layer yielded the identical result, despite the very different excitation conditions. This proves that recombination in this blend is mostly through processes in the bulk and that surface recombination is of minor importance despite the small active layer thickness. Published under license by AIP Publishing.
Near ambient pressure - x-ray photoelectron spectroscopy (NAP-XPS) is a less traditional form of XPS that allows samples to be analyzed at relatively high pressures, i.e., at 2500Pa or higher. With NAP-XPS, one can analyze moderately volatile liquids, biological samples, porous materials, and/or polymeric materials that outgas significantly. In this submission we show C 1s, O 1s, and survey NAP-XPS spectra from poly(L-lactic acid). The C 1s and O 1s envelopes were fit with three and two Gaussian-Lorentzian sum functions, respectively. Water vapor (800Pa) was used as the residual gas for charge compensation, which was confirmed by the sharp peak at 535.0 eV in the O 1s narrow scan. The uniqueness plot corresponding to the C 1s fit shows that the fit parameters had statistical significance. C 1s and O 1s spectra of PLLA damaged by exposure to x-rays for ca. 1 hour are also included. Published by the AVS.
We propose an efficient method for demodulation of phase modulated signals via iterated Hilbert transform embeddings. We show that while a usual approach based on one application of the Hilbert transform provides only an approximation to a proper phase, with iterations the accuracy is essentially improved, up to precision limited mainly by discretization effects. We demonstrate that the method is applicable to arbitrarily complex waveforms, and to modulations fast compared to the basic frequency. Furthermore, we develop a perturbative theory applicable to a simple cosine waveform, showing convergence of the technique.
Dielectric Relaxation Spectroscopy (DRS) and Thermally Stimulated Depolarization Current (TSDC) measurements were employed to study dielectric-relaxation processes, structural transitions and electric-polarization phenomena in poly(vinylidenefluoride-trifluoroethylene-chlorofluoroethylene) (P(VDF-TrFE-CFE)) terpolymer films. Results from DRS confirm the existence of two separate dispersion regions related to a para-to-ferroelectric phase transition and to the glass transition. The dipolar TSDC peak correlates with the loss peak of the ? relaxation that represents the glass transition. The electric polarization calculated from the dipolar TSDC peak (glass transition) shows a non-linear electric-field dependence and saturates at high electric poling fields. As the observed behaviour is essentially the same as that of the electric polarization obtained from direct polarization-versus-electric-field hysteresis measurements, TSDC experiments are also suitable for studying the polarization in relaxor-ferroelectric polymers. A saturation polarization of 44 mC m(?2) was found for an electric field of 190 MV m(?1).
The stability of conducting Taylor-Couette flows under the presence of toroidal magnetic background fields is considered. For strong enough magnetic amplitudes such magnetohydrodynamic flows are unstable against non-axisymmetric perturbations which may also transport angular momentum. In accordance with the often used diffusion approximation, one expects the angular momentum transport to be vanishing for rigid rotation. In the sense of a non-diffusive Lambda effect, however, even for rigidly rotating z-pinches, an axisymmetric angular momentum flux appears which is directed outward (inward) for large (small) magnetic Mach numbers. The internal rotation in a magnetized rotating tank can thus never be uniform. Those particular rotation laws are used to estimate the value of the instability-induced eddy viscosity for which the non-diffusive Lambda effect and the diffusive shear-induced transport compensate each other. The results provide the Shakura & Sunyaev viscosity ansatz leading to numerical values linearly growing with the applied magnetic field.
X-ray free-electron lasers have, over the past decade, opened up the possibility of understanding the ultrafast response of matter to intense X-ray pulses. In earlier research on atoms and small molecules, new aspects of this response were uncovered, such as rapid sequences of inner-shell photoionization and Auger ionization. Here, we studied a larger molecule, buckminsterfullerene (C-60), exposed to 640 eV X-rays, and examined the role of chemical effects, such as chemical bonds and charge transfer, on the fragmentation following multiple ionization of the molecule. To provide time resolution, we performed femtosecond-resolved X-ray pump/X-ray probe measurements, which were accompanied by advanced simulations. The simulations and experiment reveal that despite substantial ionization induced by the ultrashort (20 fs) X-ray pump pulse, the fragmentation of C-60 is considerably delayed. This work uncovers the persistence of the molecular structure of C-60, which hinders fragmentation over a timescale of hundreds of femtoseconds. Furthermore, we demonstrate that a substantial fraction of the ejected fragments are neutral carbon atoms. These findings provide insights into X-ray free-electron laser-induced radiation damage in large molecules, including biomolecules.
Optimizing the photoluminescence (PL) yield of a solar cell has long been recognized as a key principle to maximize the power conversion efficiency. While PL measurements are routinely applied to perovskite films and solar cells under open circuit conditions (V-OC), it remains unclear how the emission depends on the applied voltage. Here, we performed PL(V) measurements on perovskite cells with different hole transport layer thicknesses and doping concentrations, resulting in remarkably different fill factors (FFs). The results reveal that PL(V) mirrors the current-voltage (JV) characteristics in the power-generating regime, which highlights an interesting correlation between radiative and nonradiative recombination losses. In particular, high FF devices show a rapid quenching of PL(V) from open-circuit to the maximum power point. We conclude that, while the PL has to be maximized at V-OC at lower biases < V-OC the PL must be rapidly quenched as charges need to be extracted prior to recombination.
We present results from our on-going MusE GAs FLOw and Wind (MEGAFLOW) survey, which consists of 22 quasar lines of sight, each observed with the integral field unit MUSE and the UVES spectrograph at the ESO Very Large Telescopes (VLT). The goals of this survey are to study the properties of the circumgalactic medium around z similar to 1 star-forming galaxies. The absorption-line selected survey consists of 79 strong MgII absorbers (with rest-frame equivalent width greater than or similar to 0.3 angstrom) and, currently, 86 associated galaxies within 100 projected kpc of the quasar with stellar masses (M-star) from 109 to 1011 M-circle dot. We find that the cool halo gas traced by MgII is not isotropically distributed around these galaxies from the strong bi-modal distribution in the azimuthal angle of the apparent location of the quasar with respect to the galaxy major axis. This supports a scenario in which outflows are bi-conical in nature and co-exist with a co-planar gaseous structure extending at least up to 60-80 kpc. Assuming that absorbers near the minor axis probe outflows, the current MEGAFLOW sample allowed us to select 26 galaxy-quasar pairs suitable for studying winds. From this sample, using a simple geometrical model, we find that the outflow velocity only exceeds the escape velocity when M-star less than or similar to 4 x 10(9) M-circle dot, implying the cool material is likely to fall back except in the smallest haloes. Finally, we find that the mass loading factor., the ratio between the ejected mass rate and the star formation rate, appears to be roughly constant with respect to the galaxy mass.
Stochastic models based on random diffusivities, such as the diffusing-diffusivity approach, are popular concepts for the description of non-Gaussian diffusion in heterogeneous media. Studies of these models typically focus on the moments and the displacement probability density function. Here we develop the complementary power spectral description for a broad class of random-diffusivity processes. In our approach we cater for typical single particle tracking data in which a small number of trajectories with finite duration are garnered. Apart from the diffusing-diffusivity model we study a range of previously unconsidered random-diffusivity processes, for which we obtain exact forms of the probability density function. These new processes are different versions of jump processes as well as functionals of Brownian motion. The resulting behaviour subtly depends on the specific model details. Thus, the central part of the probability density function may be Gaussian or non-Gaussian, and the tails may assume Gaussian, exponential, log-normal, or even power-law forms. For all these models we derive analytically the moment-generating function for the single-trajectory power spectral density. We establish the generic 1/f²-scaling of the power spectral density as function of frequency in all cases. Moreover, we establish the probability density for the amplitudes of the random power spectral density of individual trajectories. The latter functions reflect the very specific properties of the different random-diffusivity models considered here. Our exact results are in excellent agreement with extensive numerical simulations.
Near-ambient pressure x-ray photoelectron spectroscopy (NAP-XPS) is a less traditional form of XPS that allows samples to be analyzed at relatively high pressures, i. e., at greater than 2500 Pa. In this study, poly(.- benzyl L- glutamate) (PBLG) with a molar mass of 11.3 kg/mol was analyzed by NAP-XPS; here, we show the survey, C 1s, N 1s, and O 1s narrow scans of PBLG. The C 1s peak envelope was fitted in three different ways, to five, six, or seven synthetic peaks. In each fit, there was also a shake-up signal. The O 1s narrow scan was well fit with three peaks: CZO and CvO in a 1:2 ratio from the polymer, and a higher energy signal from water vapor. Hartree-Fock orbital energies of a model monomer served as a guide to an additional fit of the C 1s envelope.
Germanium oxide is a prototype network-forming oxide with pressure-induced structural changes similar to those found in crystals and amorphous silicate oxides at high pressure. Studying density and coordination changes in amorphous GeO2 allows for insight into structural changes in silicate oxides at very high pressure, with implications for the properties of planetary magmas. Here, we report the density of germanium oxide glass up to 133 GPa using the x-ray absorption technique, with very good agreement with previous experimental data at pressure below 40 GPa and recent calculation up to 140 GPa. Our data highlight four distinct compressibility domains, corresponding to changes of the local structure of GeO2. Above 80 GPa, our density data show a compressibility and bulk modulus similar to the counterpart crystal phase, and we propose that a compact distorted sixfold coordination, similar to the structural motif of the pyritelike crystalline GeO2 polymorph, is likely to be stable in that pressure range. Our density data point to a smooth continuous evolution of the average coordination for pressure above 20 GPa with persistent sixfold coordination, without sharp density or density slope discontinuities. These observations are in very good agreement with theoretical calculations and spectroscopic measurements, and our results indicate that glasses and melts may behave similarly to their high-pressure solid counterparts with comparable densities, compressibility, and possibly average coordination.
Border effect corrections for diagonal line based recurrence quantification analysis measures
(2019)
Recurrence Quantification Analysis (RQA) defines a number of quantifiers, which base upon diagonal line structures in the recurrence plot (RP). Due to the finite size of an RP, these lines can be cut by the borders of the RP and, thus, bias the length distribution of diagonal lines and, consequently, the line based RQA measures. In this letter we investigate the impact of the mentioned border effects and of the thickening of diagonal lines in an RP (caused by tangential motion) on the estimation of the diagonal line length distribution, quantified by its entropy. Although a relation to the Lyapunov spectrum is theoretically expected, the mentioned entropy yields contradictory results in many studies. Here we summarize correction schemes for both, the border effects and the tangential motion and systematically compare them to methods from the literature. We show that these corrections lead to the expected behavior of the diagonal line length entropy, in particular meaning zero values in case of a regular motion and positive values for chaotic motion. Moreover, we test these methods under noisy conditions, in order to supply practical tools for applied statistical research.
We investigate the ultrafast magnetization dynamics of FePt in the L1(0) phase after an optical heating pulse, as used in heat-assisted magnetic recording. We compare continuous and nano-granular thin films and emphasize the impact of the finite size on the remagnetization dynamics. The remagnetization speeds up significantly with increasing external magnetic field only for the continuous film, where domain-wall motion governs the dynamics. The ultrafast remagnetization dynamics in the continuous film are only dominated by heat transport in the regime of high magnetic fields, whereas the timescale required for cooling is prevalent in the granular film for all magnetic field strengths. These findings highlight the necessary conditions for studying the intrinsic heat transport properties in magnetic materials.
In this paper we investigate the magneto-optical (MO) and magnetic properties of bismuth iron garnet Bi3Fe5O12 thin films over a wide range of photon energies (1.6-3.5 eV) and temperatures (5-740 K). Depending on the photon energy range, the Faraday rotation (Theta(F)) and ellipticity (epsilon(F)) vary nonmonotonously with temperature. This behavior cannot be explained by a magnetization variation that can only decrease with increasing temperature. Theta(F) and epsilon(F) spectra have therefore been analyzed using a model based on two optical transitions of a diamagnetic nature, representing the tetrahedral and octahedral iron sites. Thus, the contribution of each magnetic sublattice has been extracted from the global macroscopic MO response and investigated as a function of temperature. The magnetic properties of octahedral and tetrahedral sublattices depend differently on temperature, suggesting a different anisotropy due to oxygen coordination. We have demonstrated that this relatively simple macroscopic measurement with a subsequent analysis can grant access to the information on the properties at a microscopic level. These results can advance the fundamental understanding of MO properties in multisublattice magnetic materials.
Phase reduction is a general tool widely used to describe forced and interacting self-sustained oscillators. Here, we explore the phase coupling functions beyond the usual first-order approximation in the strength of the force. Taking the periodically forced Stuart-Landau oscillator as the paradigmatic model, we determine and numerically analyse the coupling functions up to the fourth order in the force strength. We show that the found nonlinear phase coupling functions can be used for predicting synchronization regions of the forced oscillator.
We introduce a versatile mechanism of light-driven self-propelled motion applied to porous Janus-type particles. The mechanism is based on the generation of local light-driven diffusio-osmotic (l-LDDO) flow around each single porous particle subjected to suitable irradiation conditions. The photosensitivity is introduced by a cationic azobenzene containing surfactant, which undergoes a photoisomerization reaction from a more hydrophobic trans-state to a rather hydrophilic cis-state under illumination with light. The negatively charged porous silica particles are dispersed in a corresponding aqueous solution and absorb molecules in their trans-state but expel them in their cis-state. During illumination with blue light triggering both trans-cis and cis-trans isomerization at the same time, the colloids start to move due to the generation of a steady-state diffusive flow of cis-isomers out of and trans-isomers into the particle. This is because a hemi-spherical metal cap partially sealing the colloid breaks the symmetry of the otherwise radially directed local flow around the particle, leading to self-propelled motion. Janus particles exhibit superdiffusive motion with a velocity of similar to 0.5 mu m/s and a persistence length of ca. 50 mu m, confined to microchannels the direction can be maintained up to 300 mu m before rotational diffusion reverts it. Particles forming dimers of different shapes can be made to travel along circular trajectories. The unique feature of this mechanism is that the strength of self-propulsion can be tuned by convenient external optical stimuli (intensity and irradiation wavelength) such that a broad variety of experimental situations can be realized in a spatiotemporal way and in situ.
In July 2004 the Cassini–Huygens mission reached the Saturnian system and started its orbital tour. A total of 75 orbits will be carried out during the primary mission until August 2008. In these four years Cassini crosses the ring plane 150 times and spends approx. 400 h within Titan's orbit. The Cosmic Dust Analyser (CDA) onboard Cassini characterises the dust environment with its extended E ring and embedded moons. Here, we focus on the CDA results of the first year and we present the Dust Analyser (DA) data within Titan's orbit. This paper does investigate High Rate Detector data and dust composition measurements. The authors focus on the analysis of impact rates, which were strongly variable primarily due to changes of the spacecraft pointing. An overview is given about the ring plane crossings and the DA counter measurements. The DA dust impact rates are compared with the DA boresight configuration around all ring plane crossings between June 2004 and July 2005. Dust impacts were registered at altitudes as high as 100 000 km above the ring plane at distances from Saturn between 4 and 10 Saturn radii. In those regions the dust density of particles bigger than 0.5 can reach values of 0.001m-3.
In this study, we detect high percentile rainfall events in the eastern central Andes, based on Tropical Rainfall Measuring Mission (TRMM) with a spatial resolution of 0.25 × 0.25°, a temporal resolution of 3 h, and for the duration from 2001 to 2018. We identify three areas with high mean accumulated rainfall and analyze their atmospheric behaviour and rainfall characteristics with specific focus on extreme events. Extreme events are defined by events above the 95th percentile of their daily mean accumulated rainfall. Austral summer (DJF) is the period of the year presenting the most frequent extreme events over these three regions. Daily statistics show that the spatial maxima, as well as their associated extreme events, are produced during the night. For the considered period, ERA-Interim reanalysis data, provided by the European Centre for Medium-Range Weather Forecasts (ECMWF) with 0.75° x0.75° spatial and 6-hourly temporal resolutions, were used for the analysis of the meso- and synoptic-scale atmospheric patterns. Night- and day-time differences indicate a nocturnal overload of northerly and northeasterly low-level humidity flows arriving from tropical South America. Under these conditions, cooling descending air from the mountains may find unstable air at the surface, giving place to the development of strong local convection. Another possible mechanism is presented here: a forced ascent of the low-level flow due to the mountains, disrupting the atmospheric stratification and generating vertical displacement of air trajectories. A Principal Component Analysis (PCA) in T-mode is applied to day- and night-time data during the maximum and extreme events. The results show strong correlation areas over each subregion under study during night-time, whereas during day-time no defined patterns are found. This confirms the observed nocturnal behavior of rainfall within these three hotspots.
Solar wind observations show that geomagnetic storms are mainly driven by interplanetary coronal mass ejections (ICMEs) and corotating or stream interaction regions (C/SIRs). We present a binary classifier that assigns one of these drivers to 7,546 storms between 1930 and 2015 using ground‐based geomagnetic field observations only. The input data consists of the long‐term stable Hourly Magnetospheric Currents index alongside the corresponding midlatitude geomagnetic observatory time series. This data set provides comprehensive information on the global storm time magnetic disturbance field, particularly its spatial variability, over eight solar cycles. For the first time, we use this information statistically with regard to an automated storm driver identification. Our supervised classification model significantly outperforms unskilled baseline models (78% accuracy with 26[19]% misidentified interplanetary coronal mass ejections [corotating or stream interaction regions]) and delivers plausible driver occurrences with regard to storm intensity and solar cycle phase. Our results can readily be used to advance related studies fundamental to space weather research, for example, studies connecting galactic cosmic ray modulation and geomagnetic disturbances. They are fully reproducible by means of the underlying open‐source software (Pick, 2019, http://doi.org/10.5880/GFZ.2.3.2019.003)
The Ornstein–Uhlenbeck process is a stationary and ergodic Gaussian process, that is fully determined by its covariance function and mean. We show here that the generic definitions of the ensemble- and time-averaged mean squared displacements fail to capture these properties consistently, leading to a spurious ergodicity breaking. We propose to remedy this failure by redefining the mean squared displacements such that they reflect unambiguously the statistical properties of any stochastic process. In particular we study the effect of the initial condition in the Ornstein–Uhlenbeck process and its fractional extension. For the fractional Ornstein–Uhlenbeck process representing typical experimental situations in crowded environments such as living biological cells, we show that the stationarity of the process delicately depends on the initial condition.
This work focuses on the dynamics of particles in a confined geometry with position-dependent diffusivity, where the confinement is modelled by a periodic channel consisting of unit cells connected by narrow passage ways. We consider three functional forms for the diffusivity, corresponding to the scenarios of a constant (D ₀), as well as a low (D ₘ) and a high (D d) mobility diffusion in cell centre of the longitudinally symmetric cells. Due to the interaction among the diffusivity, channel shape and external force, the system exhibits complex and interesting phenomena. By calculating the probability density function, mean velocity and mean first exit time with the Itô calculus form, we find that in the absence of external forces the diffusivity D d will redistribute particles near the channel wall, while the diffusivity D ₘ will trap them near the cell centre. The superposition of external forces will break their static distributions. Besides, our results demonstrate that for the diffusivity D d, a high dependence on the x coordinate (parallel with the central channel line) will improve the mean velocity of the particles. In contrast, for the diffusivity D ₘ, a weak dependence on the x coordinate will dramatically accelerate the moving speed. In addition, it shows that a large external force can weaken the influences of different diffusivities; inversely, for a small external force, the types of diffusivity affect significantly the particle dynamics. In practice, one can apply these results to achieve a prominent enhancement of the particle transport in two- or three-dimensional channels by modulating the local tracer diffusivity via an engineered gel of varying porosity or by adding a cold tube to cool down the diffusivity along the central line, which may be a relevant effect in engineering applications. Effects of different stochastic calculi in the evaluation of the underlying multiplicative stochastic equation for different physical scenarios are discussed.
We develop a model of stochastic radiation pressure for rotating non-spherical particles and apply the model to circumplanetary dynamics of dust grains. The stochastic properties of the radiation pressure are related to the ensemble-averaged characteristics of the rotating particles, which are given in terms of the rotational time-correlation function of a grain. We investigate the model analytically and show that an ensemble of particle trajectories demonstrates a diffusion-like behaviour. The analytical results are compared with numerical simulations, performed for the motion of the dusty ejecta from Deimos in orbit around Mars. We find that the theoretical predictions are in a good agreement with the simulation results. The agreement however deteriorates at later time, when the impact of non-linear terms, neglected in the analytic approach, becomes significant. Our results indicate that the stochastic modulation of the radiation pressure can play an important role in the circumplanetary dynamics of dust and may in case of some dusty systems noticeably alter an optical depth. (c) 2006 Elsevier Ltd. All rights reserved.
Recurrence plot analyses suggest a novel reference system involved in newborn spontaneous movements
(2006)
The movements of newborns have been thoroughly studied in terms of reflexes, muscle synergies, leg coordination, and target-directed arm/hand movements. Since these approaches have concentrated mainly on separate accomplishments, there has remained a clear need for more integrated investigations. Here, we report an inquiry in which we explicitly concentrated on taking such a perspective and, additionally, were guided by the methodological concept of home base behavior, which Ilan Golard developed for studies of exploratory behavior in animals. Methods from nonlinear dynamics, such as symbolic dynamics and recurrence plot analyses of kinematic data received from audiovisual newborn recordings, yielded new insights into the spatial and temporal organization of limb movements. In the framework of home base behavior, our approach uncovered a novel reference system of spontaneous newborn movements.
Nous évaluons la force de Casimir entre deux surfaces planes métalliques constituées d'argent. Nous prenons, pour effectuer cette évaluation, des propriétés optiques de l'argent à différentes températures [1]. Nous montrons que cette dépendance en température modifie la force de Casimir (de 0.2%) y compris à des distances inférieures à la longueur d'onde thermique.
Experimental results show that the polymerization of pyrrole in the presence of beta-naphthalenesulfonic acid and different fluorosurfactants like perfluorooctanesulfonic acid, perfluorooctyldiethanolamide, and ammonium perfluorooctanoate leads to polypyrrole with special morphologies, such as rings or disks and rectangular frames or plates. The formation of these unusually shaped particles of polymer dispersions is explained by the chemical and colloidal peculiarities of the oxidative pyrrole polymerization with ammonium peroxodisulfate in aqueous medium.
Three methods for the determination of the surface tension of liquids based on force measurements namely, the vertical plate method of Wilhelmy, the frame method of Lenard and the ring method of du Nouy are compared and studied in respect of a common principle of correction. It is shown that these three most important force-based methods allow the determination of the surface tension under static conditions. The force components of the corresponding liquid column below the measuring wire obtained for the straight part of the withdrawal curve up to the transition in its curved part provides exact surface tension values. The experimentally accessible value of the force component describes the physical background of the measured value correction contrary to the approximate equations obtained by mathematical way. Usually the determination of surface tension of liquids is based merely at the vertical plate method on exact equations thermodynamically derived whereas in the case of the frame and ring methods correction factors in approximate equations are used. At usual application of the force-based methods under the non-static condition of the withdrawal of a liquid column, the force maximum measured at withdrawal of the measuring object (plate, frame, or ring) is the basis for the determination of surface tension. In these cases, the measured surface tension values are compensated by correction equations for the frame and ring methods which are based on an correction factor and correction tables empirically obtained. The surface tension values obtained in this usual way agree with those obtained by using the force component of the corresponding liquid column below the measuring wire for the straight part of the withdrawal curve up to the transition in its curved part. Problems arising at the force measurements with increasing thickness of the measuring wires inside and outside the rings are discussed.
Optical excitation of spin-ordered rare earth metals triggers a complex response of the crystal lattice since expansive stresses from electron and phonon excitations compete with a contractive stress induced by spin disorder. Using ultrafast x-ray diffraction experiments, we study the layer specific strain response of a dysprosium film within a metallic heterostructure upon femtosecond laser-excitation. The elastic and diffusive transport of energy to an adjacent, non-excited detection layer clearly separates the contributions of strain pulses and thermal excitations in the time domain. We find that energy transfer processes to magnetic excitations significantly modify the observed conventional bipolar strain wave into a unipolar pulse. By modeling the spin system as a saturable energy reservoir that generates substantial contractive stress on ultrafast timescales, we can reproduce the observed strain response and estimate the time- and space dependent magnetic stress. The saturation of the magnetic stress contribution yields a non-monotonous total stress within the nanolayer, which leads to unconventional picosecond strain pulses.
We employ Bayesian statistics using the nested-sampling algorithm to compare and rank multiple models of ergodic diffusion (including anomalous diffusion) as well as to assess their optimal parameters for in silico-generated and real time-series. We focus on the recently-introduced model of Brownian motion with "diffusing diffusivity'-giving rise to widely-observed non-Gaussian displacement statistics-and its comparison to Brownian and fractional Brownian motion, also for the time-series with some measurement noise. We conduct this model-assessment analysis using Bayesian statistics and the nested-sampling algorithm on the level of individual particle trajectories. We evaluate relative model probabilities and compute best-parameter sets for each diffusion model, comparing the estimated parameters to the true ones. We test the performance of the nested-sampling algorithm and its predictive power both for computer-generated (idealised) trajectories as well as for real single-particle-tracking trajectories. Our approach delivers new important insight into the objective selection of the most suitable stochastic model for a given time-series. We also present first model-ranking results in application to experimental data of tracer diffusion in polymer-based hydrogels.
The velocity distribution function of granular gases in the homogeneous cooling state as well as some heated granular gases decays for large velocities as f proportional to exp(-const x nu). That is, its high-energy tail is overpopulated as compared with the Maxwell distribution. At the present time, there is no theory to describe the influence of the tail on the kinetic characteristics of granular gases. We develop an approach to quantify the overpopulated tail and analyze its impact on granular gas properties, in particular on the cooling coefficient. We observe and explain anomalously slow relaxation of the velocity distribution function to its steady state.
This paper discusses translocation features of the 20S proteasome in order to explain typical proteasome length distributions. We assume that the protein transport depends significantly on the fragment length with some optimal length which is transported most efficiently. By means of a simple one-channel model, we show that this hypothesis can explain both the one- and the three-peak length distributions found in experiments. A possible mechanism of such translocation is provided by so-called fluctuation-driven transport.
Archival X-ray spectra of the four prominent single, non-magnetic O stars zeta Pup, zeta Ori, xi Per and zeta Oph, obtained in high resolution with Chandra HETGS/MEG have been studied. The resolved X-ray emission line profiles provide information about the shocked, hot gas which emits the X-radiation, and about the bulk of comparably cool stellar wind material which partly absorbs this radiation. In this paper, we synthesize X-ray line profiles with a model of a clumpy stellar wind. We find that the geometrical shape of the wind inhomogeneities is important: better agreement with the observations can be achieved with radially compressed clumps than with spherical clumps. The parameters of the model, i.e. chemical abundances, stellar radius, mass-loss rate and terminal wind velocity, are taken from existing analyses of UV and optical spectra of the programme stars. On this basis, we also calculate the continuum-absorption coefficient of the cool-wind material, using the Potsdam Wolf-Rayet (POWR) model atmosphere code. The radial location of X-ray emitting gas is restricted from analysing the FIR line ratios of helium-like ions. The only remaining free parameter of our model is the typical distance between the clumps; here, we assume that at any point in the wind there is one clump passing by per one dynamical time-scale of the wind. The total emission in a model line is scaled to the observation. There is a good agreement between synthetic and observed line profiles. We conclude that the X-ray emission line profiles in O stars can be explained by hot plasma embedded in a cool wind which is highly clumped in the form of radially compressed shell fragments.
Context. Very massive stars pass through the Wolf-Rayet (WR) stage before they finally explode. Details of their evolution have not yet been safely established, and their physics are not well understood. Their spectral analysis requires adequate model atmospheres, which have been developed step by step during the past decades and account in their recent version for line blanketing by the millions of lines from iron and iron-group elements. However, only very few WN stars have been re-analyzed by means of line-blanketed models yet. Aims. The quantitative spectral analysis of a large sample of Galactic WN stars with the most advanced generation of model atmospheres should provide an empirical basis for various studies about the origin, evolution, and physics of the Wolf-Rayet stars and their powerful winds. Methods. We analyze a large sample of Galactic WN stars by means of the Potsdam Wolf-Rayet (PoWR) model atmospheres, which account for iron line blanketing and clumping. The results are compared with a synthetic population, generated from the Geneva tracks for massive star evolution. Results. We obtain a homogeneous set of stellar and atmospheric parameters for the GalacticWN stars, partly revising earlier results. Conclusions. Comparing the results of our spectral analyses of the Galactic WN stars with the predictions of the Geneva evolutionary calculations, we conclude that there is rough qualitative agreement. However, the quantitative discrepancies are still severe, and there is no preference for the tracks that account for the effects of rotation. It seems that the evolution of massive stars is still not satisfactorily understood.
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.
It is shown that several polymers can form insoluble interfacial layers on a poly (ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) layer after annealing of the double-layer structure. The thickness of the interlayer is dependent on the characteristics of the underlying PEDOT.PSS and the molecular weight of the polymers. It is further shown that the electronic structures of the interlayer polymers have a significant effect on the properties of red-light-emitting polymer-based electrophosphorescent devices. Upon increasing the highest occupied molecular orbital and lowest unoccupied molecular orbital positions, a significant increase in current density and device efficiency is observed. This is attributed to efficient blocking of electrons in combination with direct injection of holes from the interlayer to the phosphorescent dye. Upon proper choice of the interlayer polymer, efficient red, polymer-based electrophosphorescent devices with a peak luminance efficiency of 5.5 cd A(-1) (external quantum efficiency = 6 %) and a maximum power-conversion efficiency of 5 Im W-1 can be realized.
If not oriented perfectly isotropically, the strong dipole moment of polar organic semiconductor materials such as tris-(8-hydroxyquinolate)aluminum (Alq3) will lead to the buildup of a giant surface potential (GSP) and thus to a macroscopic dielectric polarization of the organic film. Despite this having been a known fact for years, the implications of such high potentials within an organic layer stack have only been studied recently. In this work, the influence of the GSP on hole injection into organic layers is investigated. Therefore, we apply a concept called dipolar doping to devices consisting of the prototypical organic materials N,N′-Di(1-naphthyl)-N,N′-diphenyl-(1,1′-biphenyl)-4,4′-diamine (NPB) as nonpolar host and Alq3 as dipolar dopant with different mixing ratios to tune the GSP. The mixtures are investigated in single-layer monopolar devices as well as bilayer metal/insulator/semiconductor structures. Characterization is done electrically using current-voltage (I-V) characteristics, impedance spectroscopy, and charge extraction by linearly increasing voltage and time of flight, as well as with ultraviolet photoelectron spectroscopy. We find a maximum in device performance for moderate to low doping concentrations of the polar species in the host. The observed behavior can be described on the basis of the Schottky effect for image-force barrier lowering, if the changes in the interface dipole, the carrier mobility, and the GSP induced by dipolar doping are taken into account.
We investigate the effects of a time-delayed all-to-all coupling scheme in a large population of oscillators with natural frequencies following a bimodal distribution. The regions of parameter space corresponding to synchronized and incoherent solutions are obtained both numerically and analytically for particular frequency distributions. In particular, we find that bimodality introduces a new time scale that results in a quasiperiodic disposition of the regions of incoherence.
We present experimental results showing the diffuse reflection of a Bose Einstein condensate from a rough mirror, consisting of a dielectric substrate supporting a blue-detuned evanescent wave. The scattering is anisotropic, more pronounced in the direction of the surface propagation of the evanescent wave. These results agree very well with theoretical predictions.
We present experimental and numerical evidence of synchronization of burst events in two different modulated CO2 lasers. Bursts appear randomly in each laser as trains of large amplitude spikes intercalated by a small amplitude chaotic regime. Experimental data and model show the frequency locking of bursts in a suitable interval of coupling strength. We explain the mechanism of this phenomenon and demonstrate the inhibitory properties of the implemented coupling.
Recent research using the complex network approach has revealed a rich and complicated network topology in the cortical connectivity of mammalian brains. It is of importance to understand the implications of such complex network structures in the functional organization of the brain activities. Here we study this problem from the viewpoint of dynamical complex networks. We investigate synchronization dynamics on the corticocortical network of the cat by modeling each node (cortical area) of the network with a sub-network of interacting excitable neurons. We find that the network displays clustered synchronization behavior, and the dynamical clusters coincide with the topological community structures observed in the anatomical network. Our results provide insights into the relationship between the global organization and the functional specialization of the brain cortex.
New amphiphilic compounds 1-9 that feature a construction with dendronized hydrophilic and hydrophobic segment groups connected to a specific aromatic or aliphatic spacer unit have been synthesized, following a modular building block strategy. The hydrophilic dendrons are typically branched elements with peripheral carboxylic groups, unlike the hydrophobic dendrons that contain peripheral alkyl chains as part of respective amide functions. The hydrophilic dendrons are in different generations of branching, while the hydrophobic dendrons are all in the first generation of branching (three terminal branching), but differ in the length of the alkyl chains, thus giving rise to designed structure and amphiphilic properties in the new compounds. The resulting surfactants are capable of forming well-defined Langmuir films of remarkable stability when spread from a solution onto an aqueous subphase. Nevertheless, specific packing behaviour and orientation of the amphiphilic molecules were found, depending on the molecular structure, as determined using analysis of the surface pressure-area (pi-A) isotherms. Langmuir-Blodgett transfer of the first monolayer from a pure water subphase to a clean silicon wafer proved possible for the amphiphiles of peripheral alkyl chain length C-12, while the amphiphiles with the longer alkyl chains failed, possibly due to the more rigid monolayers they form, impeding the transfer.
Atrial natriuretic peptides (ANP) and brain natriuretic peptides (BNP) are powerful neurohormonal indicators of left-ventricular function and prognosis in heart failure (HF). Chagas disease (CD) caused by the protozoan Trypanosoma cruzi. remains a major cause of HF in Latin America. We assessed whether the plasma concentration of the third natriuretic peptide, C-type natnuretic peptide (CNP), also has diagnostic and prognostic properties in patients with CD or other dilated cardiomyopathies (DCM). Blood samples were obtained from 66 patients with CD, 50 patients with DCM from other causes, and 30 gender- and age-matched healthy subjects. Patients were subdivided according to the New York Heart Association (NYHA) class. The CNP concentration was determined by radioimmunoassay (Immundiagnostik, Bensheim, Germany). The main duration of follow-up was 31.4 months (range 13 to 54 months), 19 patients had died and 11 patients received a heart transplant. CNP concentrations were only significantly altered in patients with DCM or CD of the NYHA classes III and IV (P < 0.05). The Pearson correlation of echocardiographic data with CNP revealed an association only with the left-ventricular end systolic volume (P = 0.03) in patients with DCM. Furthermore, CNP did not predict mortality or the necessity for heart transplant. Our data are the first to demonstrate the raised levels of the third natriuretic peptide CNP in CD and other DCM Whereas ANP and BNP have a high predictive value for mortality in both diseases, CNP is without any predictive potency.
We investigate the bifurcation structures in a two-dimensional parameter space (PS) of a parametrically excited system with two degrees of freedom both analytically and numerically. By means of the Renyi entropy of second order K-2, which is estimated from recurrence plots, we uncover that regions of chaotic behavior are intermingled with many complex periodic windows, such as shrimp structures in the PS. A detailed numerical analysis shows that, the stable solutions lose stability either via period doubling, or via intermittency when the parameters leave these shrimps in different directions, indicating different bifurcation properties of the boundaries. The shrimps of different sizes offer promising ways to control the dynamics of such a complex system.
Fast, three-dimensional polarization mapping in piezoelectric sensor cables was performed by means of the novel thermal-pulse tomography (TPT) technique with a lateral resolution of 200 mum. The active piezoelectric cable material (a copolymer of polyvinylidene fluoride with trifluoroethylene) was electrically poled with a point-to-cable corona discharge. A focused laser was employed to heat the opaque outer electrode, and the short-circuit current generated by the thermal pulse was used to obtain 3D polarization maps via the scale transformation method. The article describes the TPT technique as a fast non-destructive option for studying cylindrical geometries.
We analytically describe the complex scenario of homoclinic bifurcations in the Chua’s circuit. We obtain a general scaling law that gives the ratio between bifurcation parameters of different nearby homoclinic orbits. As an application of this theoretical approach, we estimate the number of higher order subsidiary homoclinic orbits that appear between two consecutive lower order subsidiary orbits. Our analytical finds might be valid for a large class of dynamical systems and are numerically confirmed in the parameter space of the Chua’s circuit.
Shilnikov homoclinic orbits are trajectories that depart from a fixed saddle-focus point, with specific eigenvalues, and return to it after an infinite amount of time (that is also true to time reversal evolution). That results in an orbit that is unstable and has an infinite period. These two main characteristics contribute in the hardness for its observation in a dynamical system as well as in nature. However, its presence reveals fundamental characteristics of the system involved, as the existence of unstable periodic orbits embedded in a chaotic set. Once the unstable periodic orbits give invariants quantities of this set,1 the Shilnikov homoclinic orbits are also related to the characteristics of the chaotic set. Their connection with the fundamental dynamical properties is verified in a wide variety of systems. A series of numerical and experimental investigations reveal how Shilnikov homoclinic orbits, in the vicinity of a chaotic attractor, determine its dynamical and topological properties.4 Thus, the Shilnikov orbits are related to the returning time of the trajectory of a CO2 laser,5 also to the topology of a glow-discharge system.6 Moreover, some class of spiking neurons are modeled by chaos governed by such orbits,7,8 and their presence are connected to the intermittence present in rabbit arteries.9 These orbits are shown to be behind the mechanism of noise-induced phenomena,10 and they are also responsible for the dynamics of an electrochemical oscillator.11 In this work, we contribute to the understanding of how Shilnikov homoclinic orbits appear on the parameter space of systems as the ones above mentioned, by showing that these orbits are not only distributed following an universal rule but also exist for large parameter variations. We then confirm our previsions in the Chua’s circuit system
Crystal structures of four different di-aryl-1,3,4-oxadiazole compounds (aryl = 2-pyridyl-, 3-pyridyl-, 2-aminophenyl-, 3-aminophenyl-) are determined. Crystallization of di(2-pyridyl)-1,3,4-oxadiazole yielded monoclinic and triclinic polymorphs. The structures are characterized by the occurrence of pi-pi interactions. Additionally, in case of the aminophenyl compounds intra- as well as intermolecular hydrogen bonds are found that influence the packing motif as well. Since these molecules are often used as ligands in metal-organic complexes similarities and differences of the molecular conformation between the molecules in the pure crystals and that of the ligands in the complexes are discussed. (c) 2006 Elsevier B.V. All rights reserved.
Relaxation processes at the glass transition in polyamide 11: From rigidity to viscoelasticity
(2006)
Relaxation processes associated with the glass transition in nonferroelectric and ferroelectric polyamide (PA) 11 are investigated by means of differential scanning calorimetry, dynamic mechanical analysis, and dielectric relaxation spectroscopy (DRS) in order to obtain information about the molecular mobility within the amorphous phase. In particular, the effects of melt quenching, cold drawing, and annealing just below the melting region are studied with respect to potential possibilities and limitations for improving the piezoelectric and pyroelectric properties of PA 11. A relaxation map is obtained from DRS that shows especially the crossover region where the cooperative alpha relaxation and the local beta relaxation merge into a single high-temperature process. No fundamental difference between quenched, cold-drawn, and annealed films is found, though in the cold-drawn (ferroelectric) film the alpha relaxation is suppressed and slowed down, but it is at least partly recovered by subsequent annealing. It is concluded that there exists an amorphous phase in all structures, even in the cold-drawn film. The amorphous phase can be more rigid or more viscoelastic depending on preparation. Cold drawing not only leads to crystallization in a ferroelectric form but also to higher rigidity of the remaining amorphous phase. Annealing just below the melting region after cold drawing causes a stronger phase separation between the crystalline phase and a more viscoelastic amorphous phase.
How do diverse dynamical patterns arise from the topology of complex networks? We study synchronization dynamics in the cortical brain network of the cat, which displays a hierarchically clustered organization, by modeling each node (cortical area) with a subnetwork of interacting excitable neurons. We find that in the biologically plausible regime the dynamics exhibits a hierarchical modular organization, in particular, revealing functional clusters coinciding with the anatomical communities at different scales. Our results provide insights into the relationship between network topology and functional organization of complex brain networks.
Translational diffusion of fluorescent tracer molecules in azobenzene polymer layers is studied at different temperatures and under illumination using the method of fluorescence recovery after photobleaching. Diffusion is clearly observed in the dark above the glass transition temperature, while homogeneous illumination at 488 nm and 100 mW/cm(2) does not cause any detectable diffusion of the dye molecules within azobenzene layers. This implies that the viscosity of azobenzene layers remains nearly unchanged under illumination with visible light in the absence of internal or external forces. (c) 2006 American Institute of Physics.
We study the overdamped version of two coupled anharmonic oscillators under the influence of both low- and high-frequency forces respectively and a Gaussian noise term added to one of the two state variables of the system. The dynamics of the system is first studied in the presence of both forces separately without noise. In the presence of only one of the forces, no resonance behaviour is observed, however, hysteresis happens there. Then the influence of the high-frequency force in the presence of a low-frequency, i.e. biharmonic forcing, is studied. Vibrational resonance is found to occur when the amplitude of the high-frequency force is varied. The resonance curve resembles a stochastic resonance-like curve. It is maximum at the value of g at which the orbit lies in one well during one half of the drive cycle of the low-frequency force and in the other for the remaining half cycle. Vibrational resonance is characterized using the response amplitude and mean residence time. We show the occurrence of stochastic resonance behaviour in the overdamped system by replacing the high-frequency force by Gaussian noise. Similarities and differences between both types of resonance are presented. (c) 2006 Elsevier B.V. All rights reserved.
We demonstrate the existence of solitary waves of synchrony in one-dimensional arrays of oscillator populations with Laplacian coupling. Characterizing each community with its complex order parameter, we obtain lattice equations similar to those of the discrete nonlinear Schrodinger system. Close to full synchrony, we find solitary waves for the order parameter perturbatively, starting from the known phase compactons and kovatons; these solutions are extended numerically to the full domain of possible synchrony levels. For nonidentical oscillators, the existence of dissipative solitons is shown.
The possibility to manufacture perovskite solar cells (PSCs) at low temperatures paves the way to flexible and lightweight photovoltaic (PV) devices manufactured via high-throughput roll-to-roll processes. In order to achieve higher power conversion efficiencies, it is necessary to approach the radiative limit via suppression of non-radiative recombination losses. Herein, we performed a systematic voltage loss analysis for a typical low-temperature processed, flexible PSC in n-i-p configuration using vacuum deposited C-60 as electron transport layer (ETL) and two-step hybrid vacuum-solution deposition for CH3NH3PbI3 perovskite absorber. We identified the ETL/absorber interface as a bottleneck in relation to non-radiative recombination losses, the quasi-Fermi level splitting (QFLS) decreases from similar to 1.23 eV for the bare absorber, just similar to 90 meV below the radiative limit, to similar to 1.10 eV when C-60 is used as ETL. To effectively mitigate these voltage losses, we investigated different interfacial modifications via vacuum deposited interlayers (BCP, B4PyMPM, 3TPYMB, and LiF). An improvement in QFLS of similar to 30-40 meV is observed after interlayer deposition and confirmed by comparable improvements in the open-circuit voltage after implementation of these interfacial modifications in flexible PSCs. Further investigations on absorber/hole transport layer (HTL) interface point out the detrimental role of dopants in Spiro-OMeTAD film (widely employed HTL in the community) as recombination centers upon oxidation and light exposure. [GRAPHICS] .
Charge carrier recombination in organic disordered semiconductors is strongly influenced by the thermalization of charge carriers in the density of states (DOS). Measurements of recombination dynamics, conducted under transient or steady-state conditions, can easily be misinterpreted when a detailed understanding of the interplay of thermalization and recombination is missing. To enable adequate measurement analysis, we solve the multiple-trapping problem for recombining charge carriers and analyze it in the transient and steady excitation paradigm for different DOS distributions. We show that recombination rates measured after pulsed excitation are inherently time dependent since recombination gradually slows down as carriers relax in the DOS. When measuring the recombination order after pulsed excitation, this leads to an apparent high-order recombination at short times. As times goes on, the recombination order approaches an asymptotic value. For the Gaussian and the exponential DOS distributions, this asymptotic value equals the recombination order of the equilibrated system under steady excitation. For a more general DOS distribution, the recombination order can also depend on the carrier density, under both transient and steady-state conditions. We conclude that transient experiments can provide rich information about recombination in and out of equilibrium and the underlying DOS occupation provided that consistent modeling of the system is performed.
We present an X-ray-optical cross-correlator for the soft (> 150 eV) up to the hard X-ray regime based on a molybdenum-silicon superlattice. The cross-correlation is done by probing intensity and position changes of superlattice Bragg peaks caused by photoexcitation of coherent phonons. This approach is applicable for a wide range of X-ray photon energies as well as for a broad range of excitation wavelengths and requires no external fields or changes of temperature. Moreover, the cross-correlator can be employed on a 10 ps or 100 fs time scale featuring up to 50% total X-ray reflectivity and transient signal changes of more than 20%. (C) 2016 Author(s).
In the scenario of the narrow escape problem (NEP) a particle diffuses in a finite container and eventually leaves it through a small 'escape window' in the otherwise impermeable boundary, once it arrives to this window and crosses an entropic barrier at the entrance to it. This generic problem is mathematically identical to that of a diffusion-mediated reaction with a partially-reactive site on the container's boundary. Considerable knowledge is available on the dependence of the mean first-reaction time (FRT) on the pertinent parameters. We here go a distinct step further and derive the full FRT distribution for the NEP. We demonstrate that typical FRTs may be orders of magnitude shorter than the mean one, thus resulting in a strong defocusing of characteristic temporal scales. We unveil the geometry-control of the typical times, emphasising the role of the initial distance to the target as a decisive parameter. A crucial finding is the further FRT defocusing due to the barrier, necessitating repeated escape or reaction attempts interspersed with bulk excursions. These results add new perspectives and offer a broad comprehension of various features of the by-now classical NEP that are relevant for numerous biological and technological systems.
In nature as well as in the context of infection and medical applications, bacteria often have to move in highly complex environments such as soil or tissues. Previous studies have shown that bacteria strongly interact with their surroundings and are often guided by confinements. Here, we investigate theoretically how the dispersal of swimming bacteria can be augmented by microfluidic environments and validate our theoretical predictions experimentally. We consider a system of bacteria performing the prototypical run-and-tumble motion inside a labyrinth with square lattice geometry. Narrow channels between the square obstacles limit the possibility of bacteria to reorient during tumbling events to an area where channels cross. Thus, by varying the geometry of the lattice it might be possible to control the dispersal of cells. We present a theoretical model quantifying diffusive spreading of a run-and-tumble random walker in a square lattice. Numerical simulations validate our theoretical predictions for the dependence of the diffusion coefficient on the lattice geometry. We show that bacteria moving in square labyrinths exhibit enhanced dispersal as compared to unconfined cells. Importantly, confinement significantly extends the duration of the phase with strongly non-Gaussian diffusion, when the geometry of channels is imprinted in the density profiles of spreading cells. Finally, in good agreement with our theoretical findings, we observe the predicted behaviors in experiments with E. coli bacteria swimming in a square lattice labyrinth created in amicrofluidic device. Altogether, our comprehensive understanding of bacterial dispersal in a simple two-dimensional labyrinth makes the first step toward the analysis of more complex geometries relevant for real world applications.
For both Lévy flight and Lévy walk search processes we analyse the full distribution of first-passage and first-hitting (or first-arrival) times. These are, respectively, the times when the particle moves across a point at some given distance from its initial position for the first time, or when it lands at a given point for the first time. For Lévy motions with their propensity for long relocation events and thus the possibility to jump across a given point in space without actually hitting it ('leapovers'), these two definitions lead to significantly different results. We study the first-passage and first-hitting time distributions as functions of the Lévy stable index, highlighting the different behaviour for the cases when the first absolute moment of the jump length distribution is finite or infinite. In particular we examine the limits of short and long times. Our results will find their application in the mathematical modelling of random search processes as well as computer algorithms.
Many studies on biological and soft matter systems report the joint presence of a linear mean-squared displacement and a non-Gaussian probability density exhibiting, for instance, exponential or stretched-Gaussian tails. This phenomenon is ascribed to the heterogeneity of the medium and is captured by random parameter models such as ‘superstatistics’ or ‘diffusing diffusivity’. Independently, scientists working in the area of time series analysis and statistics have studied a class of discrete-time processes with similar properties, namely, random coefficient autoregressive models. In this work we try to reconcile these two approaches and thus provide a bridge between physical stochastic processes and autoregressive models.Westart from the basic Langevin equation of motion with time-varying damping or diffusion coefficients and establish the link to random coefficient autoregressive processes. By exploring that link we gain access to efficient statistical methods which can help to identify data exhibiting Brownian yet non-Gaussian diffusion.
Fractional Brownian motion (FBM) is a Gaussian stochastic process with stationary, long-time correlated increments and is frequently used to model anomalous diffusion processes. We study numerically FBM confined to a finite interval with reflecting boundary conditions. The probability density function of this reflected FBM at long times converges to a stationary distribution showing distinct deviations from the fully flat distribution of amplitude 1/L in an interval of length L found for reflected normal Brownian motion. While for superdiffusion, corresponding to a mean squared displacement (MSD) 〈X² (t)〉 ⋍ tᵅ with 1 < α < 2, the probability density function is lowered in the centre of the interval and rises towards the boundaries, for subdiffusion (0 < α < 1) this behaviour is reversed and the particle density is depleted close to the boundaries. The MSD in these cases at long times converges to a stationary value, which is, remarkably, monotonically increasing with the anomalous diffusion exponent α. Our a priori surprising results may have interesting consequences for the application of FBM for processes such as molecule or tracer diffusion in the confines of living biological cells or organelles, or other viscoelastic environments such as dense liquids in microfluidic chambers.
Astandard approach to study time-dependent stochastic processes is the power spectral density (PSD), an ensemble-averaged property defined as the Fourier transform of the autocorrelation function of the process in the asymptotic limit of long observation times, T → ∞. In many experimental situations one is able to garner only relatively few stochastic time series of finite T, such that practically neither an ensemble average nor the asymptotic limit T → ∞ can be achieved. To accommodate for a meaningful analysis of such finite-length data we here develop the framework of single-trajectory spectral analysis for one of the standard models of anomalous diffusion, scaled Brownian motion.Wedemonstrate that the frequency dependence of the single-trajectory PSD is exactly the same as for standard Brownian motion, which may lead one to the erroneous conclusion that the observed motion is normal-diffusive. However, a distinctive feature is shown to be provided by the explicit dependence on the measurement time T, and this ageing phenomenon can be used to deduce the anomalous diffusion exponent.Wealso compare our results to the single-trajectory PSD behaviour of another standard anomalous diffusion process, fractional Brownian motion, and work out the commonalities and differences. Our results represent an important step in establishing singletrajectory PSDs as an alternative (or complement) to analyses based on the time-averaged mean squared displacement.
We show that the codifference is a useful tool in studying the ergodicity breaking and non-Gaussianity properties of stochastic time series. While the codifference is a measure of dependence that was previously studied mainly in the context of stable processes, we here extend its range of applicability to random-parameter and diffusing-diffusivity models which are important in contemporary physics, biology and financial engineering. We prove that the codifference detects forms of dependence and ergodicity breaking which are not visible from analysing the covariance and correlation functions. We also discuss a related measure of dispersion, which is a nonlinear analogue of the mean squared displacement.
We combine ultrafast X-ray diffraction (UXRD) and time-resolved Magneto-Optical Kerr Effect (MOKE) measurements to monitor the strain pulses in laser-excited TbFe2/Nb heterostructures. Spatial separation of the Nb detection layer from the laser excitation region allows for a background-free characterization of the laser-generated strain pulses. We clearly observe symmetric bipolar strain pulses if the excited TbFe2 surface terminates the sample and a decomposition of the strain wavepacket into an asymmetric bipolar and a unipolar pulse, if a SiO2 glass capping layer covers the excited TbFe2 layer. The inverse magnetostriction of the temporally separated unipolar strain pulses in this sample leads to a MOKE signal that linearly depends on the strain pulse amplitude measured through UXRD. Linear chain model simulations accurately predict the timing and shape of UXRD and MOKE signals that are caused by the strain reflections from multiple interfaces in the heterostructure.
We measure valence-to-core x-ray emission spectra of compressed crystalline GeO₂ up to 56 GPa and of amorphous GeO₂ up to 100 GPa. In a novel approach, we extract the Ge coordination number and mean Ge-O distances from the emission energy and the intensity of the Kβ'' emission line. The spectra of high-pressure polymorphs are calculated using the Bethe-Salpeter equation. Trends observed in the experimental and calculated spectra are found to match only when utilizing an octahedral model. The results reveal persistent octahedral Ge coordination with increasing distortion, similar to the compaction mechanism in the sequence of octahedrally coordinated crystalline GeO₂ high-pressure polymorphs.
Abstract
The emerging diffusive dynamics in many complex systems show a characteristic crossover behaviour from anomalous to normal diffusion which is otherwise fitted by two independent power-laws. A prominent example for a subdiffusive–diffusive crossover are viscoelastic systems such as lipid bilayer membranes, while superdiffusive–diffusive crossovers occur in systems of actively moving biological cells. We here consider the general dynamics of a stochastic particle driven by so-called tempered fractional Gaussian noise, that is noise with Gaussian amplitude and power-law correlations, which are cut off at some mesoscopic time scale. Concretely we consider such noise with built-in exponential or power-law tempering, driving an overdamped Langevin equation (fractional Brownian motion) and fractional Langevin equation motion. We derive explicit expressions for the mean squared displacement and correlation functions, including different shapes of the crossover behaviour depending on the concrete tempering, and discuss the physical meaning of the tempering. In the case of power-law tempering we also find a crossover behaviour from faster to slower superdiffusion and slower to faster subdiffusion. As a direct application of our model we demonstrate that the obtained dynamics quantitatively describes the subdiffusion–diffusion and subdiffusion–subdiffusion crossover in lipid bilayer systems. We also show that a model of tempered fractional Brownian motion recently proposed by Sabzikar and Meerschaert leads to physically very different behaviour with a seemingly paradoxical ballistic long time scaling.
A considerable number of systems have recently been reported in which
Brownian yet non-Gaussian dynamics was observed. These are processes characterised by a linear growth in time of the mean squared displacement, yet the probability density function of the particle displacement is distinctly non-Gaussian, and often of exponential(Laplace) shape. This apparently ubiquitous behaviour observed in very different physical systems has been interpreted as resulting from diffusion in inhomogeneous environments and mathematically represented through a variable, stochastic diffusion coefficient. Indeed different models describing a fluctuating diffusivity have been studied. Here we present a new view of the stochastic basis describing time dependent random diffusivities within a broad spectrum of distributions. Concretely, our study is based on the very generic class of the generalised Gamma distribution. Two models for the particle spreading in such random diffusivity settings are studied. The first belongs to the class of generalised grey Brownian motion while the second follows from the idea of diffusing diffusivities. The two processes exhibit significant characteristics which reproduce experimental results from different biological and physical systems. We promote these two physical models for the description of stochastic particle motion in complex environments.
Recent advances in single particle tracking and supercomputing techniques demonstrate the emergence of normal or anomalous, viscoelastic diffusion in conjunction with non-Gaussian distributions in soft, biological, and active matter systems. We here formulate a stochastic model based on a generalised Langevin equation in which non-Gaussian shapes of the probability density function and normal or anomalous diffusion have a common origin, namely a random parametrisation of the stochastic force. We perform a detailed analysis demonstrating how various types of parameter distributions for the memory kernel result in exponential, power law, or power-log law tails of the memory functions. The studied system is also shown to exhibit a further unusual property: the velocity has a Gaussian one point probability density but non-Gaussian joint distributions. This behaviour is reflected in the relaxation from a Gaussian to a non-Gaussian distribution observed for the position variable. We show that our theoretical results are in excellent agreement with stochastic simulations.
Fixational eye movements show scaling behaviour of the positional mean-squared displacement with a characteristic transition from persistence to antipersistence for increasing time-lag. These statistical patterns were found to be mainly shaped by microsaccades (fast, small-amplitude movements). However, our re-analysis of fixational eye-movement data provides evidence that the slow component (physiological drift) of the eyes exhibits scaling behaviour of the mean-squared displacement that varies across human participants. These results suggest that drift is a correlated movement that interacts with microsaccades. Moreover, on the long time scale, the mean-squared displacement of the drift shows oscillations, which is also present in the displacement auto-correlation function. This finding lends support to the presence of time-delayed feedback in the control of drift movements. Based on an earlier non-linear delayed feedback model of fixational eye movements, we propose and discuss different versions of a new model that combines a self-avoiding walk with time delay. As a result, we identify a model that reproduces oscillatory correlation functions, the transition from persistence to antipersistence, and microsaccades.
Effects of the target aspect ratio and intrinsic reactivity onto diffusive search in bounded domains
(2017)
Westudy the mean first passage time (MFPT) to a reaction event on a specific site in a cylindrical geometry—characteristic, for instance, for bacterial cells, with a concentric inner cylinder representing the nuclear region of the bacterial cell. Asimilar problem emerges in the description of a diffusive search by a transcription factor protein for a specific binding region on a single strand of DNA.We develop a unified theoretical approach to study the underlying boundary value problem which is based on a self-consistent approximation of the mixed boundary condition. Our approach permits us to derive explicit, novel, closed-form expressions for the MFPT valid for a generic setting with an arbitrary relation between the system parameters.Weanalyse this general result in the asymptotic limits appropriate for the above-mentioned biophysical problems. Our investigation reveals the crucial role of the target aspect ratio and of the intrinsic reactivity of the binding region, which were disregarded in previous studies. Theoretical predictions are confirmed by numerical simulations.
Molecules often fragment after photoionization in the gas phase. Usually, this process can only be investigated spectroscopically as long as there exists electron correlation between the photofragments. Important parameters, like their kinetic energy after separation, cannot be investigated. We are reporting on a femtosecond time-resolved Auger electron spectroscopy study concerning the photofragmentation dynamics of thymine. We observe the appearance of clearly distinguishable signatures from thymine′s neutral photofragment isocyanic acid. Furthermore, we observe a time-dependent shift of its spectrum, which we can attribute to the influence of the charged fragment on the Auger electron. This allows us to map our time-dependent dataset onto the fragmentation coordinate. The time dependence of the shift supports efficient transformation of the excess energy gained from photoionization into kinetic energy of the fragments. Our method is broadly applicable to the investigation of photofragmentation processes.
We consider synchronization properties of arrays of spin-torque nano-oscillators coupled via an RC load. We show that while the fully synchronized state of identical oscillators may be locally stable in some parameter range, this synchrony is not globally attracting. Instead, regimes of different levels of compositional complexity are observed. These include chimera states (a part of the array forms a cluster while other units are desynchronized), clustered chimeras (several clusters plus desynchronized oscillators), cluster state (all oscillators form several clusters), and partial synchronization (no clusters but a nonvanishing mean field). Dynamically, these states are also complex, demonstrating irregular and close to quasiperiodic modulation. Remarkably, when heterogeneity of spin-torque oscillators is taken into account, dynamical complexity even increases: close to the onset of a macroscopic mean field, the dynamics of this field is rather irregular.
Passive coherent combination of several discrete low power laser diodes is a promising way to overcome the issue of degrading beam quality when scaling single emitters to > 10W output power. Such systems would be an efficient alternative to current high power sources, yet they suffer from fatal coherence loss when operated well above threshold. We present a new way to obtain detailed coherence information for laser diode arrays using a spatial light modulator to help identify the underlying decoherence processes. Reconstruction tests of the emitted far-field distribution are conducted to evaluate the performance of our setup.
Anomalous diffusion is being discovered in a fast growing number of systems. The exact nature of this anomalous diffusion provides important information on the physical laws governing the studied system. One of the central properties analysed for finite particle motion time series is the intrinsic variability of the apparent diffusivity, typically quantified by the ergodicity breaking parameter EB. Here we demonstrate that frequently EB is insufficient to provide a meaningful measure for the observed variability of the data. Instead, important additional information is provided by the higher order moments entering by the skewness and kurtosis. We analyse these quantities for three popular anomalous diffusion models. In particular, we find that even for the Gaussian fractional Brownian motion a significant skewness in the results of physical measurements occurs and needs to be taken into account. Interestingly, the kurtosis and skewness may also provide sensitive estimates of the anomalous diffusion exponent underlying the data. We also derive a new result for the EB parameter of fractional Brownian motion valid for the whole range of the anomalous diffusion parameter. Our results are important for the analysis of anomalous diffusion but also provide new insights into the theory of anomalous stochastic processes.
We introduce three strategies for the analysis of financial time series based on time averaged observables. These comprise the time averaged mean squared displacement (MSD) as well as the ageing and delay time methods for varying fractions of the financial time series. We explore these concepts via statistical analysis of historic time series for several Dow Jones Industrial indices for the period from the 1960s to 2015. Remarkably, we discover a simple universal law for the delay time averaged MSD. The observed features of the financial time series dynamics agree well with our analytical results for the time averaged measurables for geometric Brownian motion, underlying the famed Black–Scholes–Merton model. The concepts we promote here are shown to be useful for financial data analysis and enable one to unveil new universal features of stock market dynamics.
Complementarity in single photon interference – the role of the mode function and vacuum fields
(2017)
Background
In earlier experiments the role of the vacuum fields could be demonstrated as the source of complementarity with respect to the temporal properties (Heuer et al., Phys. Rev. Lett. 114:053601, 2015).
Methods
Single photon first order interferences of spatially separated regions from the cone structure of spontaneous parametric down conversion allow for analyzing the role of the mode function in quantum optics regarding the complementarity principle.
Results
Here the spatial coherence properties of these vacuum fields are demonstrated as the physical reason for complementarity in these single photon quantum optical experiments. These results are directly connected to the mode picture in classical optics.
Conclusion
The properties of the involved vacuum fields selected via the measurement process are the physical background of the complementarity principle in quantum optics.
The results of the theoretical consideration of stochastic resonance in overdamped bistable oscillators are given. These results are founded not on the model of two states as in [McNamara B, Wiesenfeld K. Theory of stochastic resonance. Phys Rev A 1989;39:4854-69], but on splitting of motion into regular and random and the rigorous solution of the Fokker-Planck equation for the random component. We show that this resonance is caused by a change, under the influence of noise, of the system's effective stiffness and damping factor contained in the equation for the regular component. For a certain value of the noise intensity the effective stiffness is minimal, and this fact causes non-monotonic change of the output signal amplitude as the noise intensity changes. It is important that the location of the minimum and its value depend essentially on the signal frequency.
Motivated by the successful Karlsruhe dynamo experiment, a relatively low-dimensional dynamo model is proposed. It is based on a strong truncation of the magnetohydrodynamic (MHD) equations with an external forcing of the Roberts type and the requirement that the model system satisfies the symmetries of the full MHD system, so that the first symmetry-breaking bifurcations can be captured. The backbone of the Roberts dynamo is formed by the Roberts flow, a helical mean magnetic field and another part of the magnetic field coupled to these two by triadic mode interactions. A minimum truncation model (MTM) containing only these energetically dominating primary mode triads is fully equivalent to the widely used first-order smoothing approximation. However, it is shown that this approach works only in the limit of small wave numbers of the excited magnetic field or small magnetic Reynolds numbers ($Rm ll 1$). To obtain dynamo action under more general conditions, secondary mode
Recent progress towards a quantum theory of laser-induced desorption and related phenomena is reviewed, for specific examples. These comprise the photodesorption of NO from Pt(111), the scanning tunnelling microscope and laser- induced desorption and switching of H at Si(100), and the electron stimulated desorption and dissociation of CO at Ru(0001). The theoretical methods used for nuclear dynamics range from open-system density matrix theory over nonadiabatically coupled multi-state models to electron-nuclear wavepackets. Also, aspects of time-dependent spectroscopy to probe ultrafast nonadiabatic processes at surfaces will be considered for the example of two-photon photoemission of solvated electrons in ice layers on Cu(111)
The title compounds, [(1R,3R,4R,5R,6S)-4,5-bis(acetyloxy)-7-oxo-2-oxabicyclo-
[4.2.0]octan-3-yl]methyl acetate, C14H18O8, (I), [(1S,4R,5S,6R)-5-acetyloxy-7-
hydroxyimino-2-oxobicyclo[4.2.0]octan-4-yl acetate, C11H15NO6, (II), and
[(3aR,5R,6R,7R,7aS)-6,7-bis(acetyloxy)-2-oxooctahydropyrano[3,2-b]pyrrol-5-
yl]methyl acetate, C14H19NO8, (III), are stable bicyclic carbohydrate derivatives.
They can easily be synthesized in a few steps from commercially available
glycals. As a result of the ring strain from the four-membered rings in (I) and
(II), the conformations of the carbohydrates deviate strongly from the ideal
chair form. Compound (II) occurs in the boat form. In the five-membered
lactam (III), on the other hand, the carbohydrate adopts an almost ideal chair
conformation. As a result of the distortion of the sugar rings, the configurations
of the three bicyclic carbohydrate derivatives could not be determined from
their NMR coupling constants. From our three crystal structure determinations,
we were able to establish for the first time the absolute configurations of all new
stereocenters of the carbohydrate rings.
The strong adhesion of sub-micron sized particles to surfaces is a nuisance, both for removing contaminating colloids from surfaces and for conscious manipulation of particles to create and test novel micro/nano-scale assemblies. The obvious idea of using detergents to ease these processes suffers from a lack of control: the action of any conventional surface-modifying agent is immediate and global. With photosensitive azobenzene containing surfactants we overcome these limitations. Such photo-soaps contain optical switches (azobenzene molecules), which upon illumination with light of appropriate wavelength undergo reversible trans-cis photo-isomerization resulting in a subsequent change of the physico-chemical molecular properties. In this work we show that when a spatial gradient in the composition of trans- and cis- isomers is created near a solid-liquid interface, a substantial hydrodynamic flow can be initiated, the spatial extent of which can be set, e.g., by the shape of a laser spot. We propose the concept of light induced diffusioosmosis driving the flow, which can remove, gather or pattern a particle assembly at a solid-liquid interface. In other words, in addition to providing a soap we implement selectivity: particles are mobilized and moved at the time of illumination, and only across the illuminated area.
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 present a temperature and fluence dependent Ultrafast X-Ray Diffraction study of a laser-heated antiferromagnetic dysprosium thin film. The loss of antiferromagnetic order is evidenced by a pronounced lattice contraction. We devise a method to determine the energy flow between the phonon and spin system from calibrated Bragg peak positions in thermal equilibrium. Reestablishing the magnetic order is much slower than the cooling of the lattice, especially around the Néel temperature. Despite the pronounced magnetostriction, the transfer of energy from the spin system to the phonons in Dy is slow after the spin-order is lost.
It is quite generally assumed that the overdamped Langevin equation provides a quantitative description of the dynamics of a classical Brownian particle in the long time limit. We establish and investigate a paradigm anomalous diffusion process governed by an underdamped Langevin equation with an explicit time dependence of the system temperature and thus the diffusion and damping coefficients. We show that for this underdamped scaled Brownian motion (UDSBM) the overdamped limit fails to describe the long time behaviour of the system and may practically even not exist at all for a certain range of the parameter values. Thus persistent inertial effects play a non-negligible role even at significantly long times. From this study a general questions on the applicability of the overdamped limit to describe the long time motion of an anomalously diffusing particle arises, with profound consequences for the relevance of overdamped anomalous diffusion models. We elucidate our results in view of analytical and simulations results for the anomalous diffusion of particles in free cooling granular gases.
What are the physical laws of the mutual interactions of objects bound to cell membranes, such as various membrane proteins or elongated virus particles? To rationalise this, we here investigate by extensive computer simulations mutual interactions of rod-like particles adsorbed on the surface of responsive elastic two-dimensional sheets. Specifically, we quantify sheet deformations as a response to adhesion of such filamentous particles. We demonstrate that tip-to-tip contacts of rods are favoured for relatively soft sheets, while side-by-side contacts are preferred for stiffer elastic substrates. These attractive orientation-dependent substrate-mediated interactions between the rod-like particles on responsive sheets can drive their aggregation and self-assembly. The optimal orientation of the membrane-bound rods is established via responding to the elastic energy profiles created around the particles. We unveil the phase diagramme of attractive–repulsive rod–rod interactions in the plane of their separation and mutual orientation. Applications of our results to other systems featuring membrane-associated particles are also discussed.
The gravitational field of a laser pulse of finite lifetime, is investigated in the framework of linearized gravity. Although the effects are very small, they may be of fundamental physical interest. It is shown that the gravitational field of a linearly polarized light pulse is modulated as the norm of the corresponding electric field strength, while no modulations arise for circular polarization. In general, the gravitational field is independent of the polarization direction. It is shown that all physical effects are confined to spherical shells expanding with the speed of light, and that these shells are imprints of the spacetime events representing emission and absorption of the pulse. Nearby test particles at rest are attracted towards the pulse trajectory by the gravitational field due to the emission of the pulse, and they are repelled from the pulse trajectory by the gravitational field due to its absorption. Examples are given for the size of the attractive effect. It is recovered that massless test particles do not experience any physical effect if they are co-propagating with the pulse, and that the acceleration of massless test particles counter-propagating with respect to the pulse is four times stronger than for massive particles
at rest. The similarities between the gravitational effect of a laser pulse and Newtonian gravity in two dimensions are pointed out. The spacetime curvature close to the pulse is compared to that induced by gravitational waves from astronomical sources.
Many chemical reactions in biological cells occur at very low concentrations of constituent molecules. Thus, transcriptional gene-regulation is often controlled by poorly expressed transcription-factors, such as E.coli lac repressor with few tens of copies. Here we study the effects of inherent concentration fluctuations of substrate-molecules on the seminal Michaelis-Menten scheme of biochemical reactions. We present a universal correction to the Michaelis-Menten equation for the reaction-rates. The relevance and validity of this correction for enzymatic reactions and intracellular gene-regulation is demonstrated. Our analytical theory and simulation results confirm that the proposed variance-corrected Michaelis-Menten equation predicts the rate of reactions with remarkable accuracy even in the presence of large non-equilibrium concentration fluctuations. The major advantage of our approach is that it involves only the mean and variance of the substrate-molecule concentration. Our theory is therefore accessible to experiments and not specific to the exact source of the concentration fluctuations.
Temperature-memory polymers remember the temperature, where they were deformed recently, enabled by broad thermal transitions. In this study, we explored a series of crosslinked poly[ethylene-co-(vinyl acetate)] networks (cPEVAs) comprising crystallizable polyethylene (PE) controlling units exhibiting a pronounced temperature-memory effect (TME) between 16 and 99 °C related to a broad melting transition (∼100 °C). The nanostructural changes in such cPEVAs during programming and activation of the TME were analyzed via in situ X-ray scattering and specific annealing experiments. Different contributions to the mechanism of memorizing high or low deformation temperatures (Tdeform) were observed in cPEVA, which can be associated to the average PE crystal sizes. At high deformation temperatures (>50 °C), newly formed PE crystals, which are established during cooling when fixing the temporary shape, dominated the TME mechanism. In contrast, at low Tdeform (<50 °C), corresponding to a cold drawing scenario, the deformation led preferably to a disruption of existing large crystals into smaller ones, which then fix the temporary shape upon cooling. The observed mechanism of memorizing a deformation temperature might enable the prediction of the TME behavior and the knowledge based design of other TMPs with crystallizable controlling units.
Recent experiments show that transcription factors (TFs) indeed use the facilitated diffusion mechanism to locate their target sequences on DNA in living bacteria cells: TFs alternate between sliding motion along DNA and relocation events through the cytoplasm. From simulations and theoretical analysis we study the TF-sliding motion for a large section of the DNA-sequence of a common E. coli strain, based on the two-state TF-model with a fast-sliding search state and a recognition state enabling target detection. For the probability to detect the target before dissociating from DNA the TF-search times self-consistently depend heavily on whether or not an auxiliary operator (an accessible sequence similar to the main operator) is present in the genome section. Importantly, within our model the extent to which the interconversion rates between search and recognition states depend on the underlying nucleotide sequence is varied. A moderate dependence maximises the capability to distinguish between the main operator and similar sequences. Moreover, these auxiliary operators serve as starting points for DNA looping with the main operator, yielding a spectrum of target detection times spanning several orders of magnitude. Auxiliary operators are shown to act as funnels facilitating target detection by TFs.
We define and study in detail utraslow scaled Brownian motion (USBM) characterized by a time dependent diffusion coefficient of the form . For unconfined motion the mean squared displacement (MSD) of USBM exhibits an ultraslow, logarithmic growth as function of time, in contrast to the conventional scaled Brownian motion. In a harmonic potential the MSD of USBM does not saturate but asymptotically decays inverse-proportionally to time, reflecting the highly non-stationary character of the process. We show that the process is weakly non-ergodic in the sense that the time averaged MSD does not converge to the regular MSD even at long times, and for unconfined motion combines a linear lag time dependence with a logarithmic term. The weakly non-ergodic behaviour is quantified in terms of the ergodicity breaking parameter. The USBM process is also shown to be ageing: observables of the system depend on the time gap between initiation of the test particle and start of the measurement of its motion. Our analytical results are shown to agree excellently with extensive computer simulations.
Stochastic Wilson
(2015)
We consider a simple Markovian class of the stochastic Wilson–Cowan type models of neuronal network dynamics, which incorporates stochastic delay caused by the existence of a refractory period of neurons. From the point of view of the dynamics of the individual elements, we are dealing with a network of non-Markovian stochastic two-state oscillators with memory, which are coupled globally in a mean-field fashion. This interrelation of a higher-dimensional Markovian and lower-dimensional non-Markovian dynamics is discussed in its relevance to the general problem of the network dynamics of complex elements possessing memory. The simplest model of this class is provided by a three-state Markovian neuron with one refractory state, which causes firing delay with an exponentially decaying memory within the two-state reduced model. This basic model is used to study critical avalanche dynamics (the noise sustained criticality) in a balanced feedforward network consisting of the excitatory and inhibitory neurons. Such avalanches emerge due to the network size dependent noise (mesoscopic noise). Numerical simulations reveal an intermediate power law in the distribution of avalanche sizes with the critical exponent around −1.16. We show that this power law is robust upon a variation of the refractory time over several orders of magnitude. However, the avalanche time distribution is biexponential. It does not reflect any genuine power law dependence.
Molecular motors pulling cargos in the viscoelastic cytosol: how power strokes beat subdiffusion
(2014)
The discovery of anomalous diffusion of larger biopolymers and submicron tracers such as endogenous granules, organelles, or virus capsids in living cells, attributed to the viscoelastic nature of the cytoplasm, provokes the question whether this complex environment equally impacts the active intracellular transport of submicron cargos by molecular motors such as kinesins: does the passive anomalous diffusion of free cargo always imply its anomalously slow active transport by motors, the mean transport distance along microtubule growing sublinearly rather than linearly in time? Here we analyze this question within the widely used two-state Brownian ratchet model of kinesin motors based on the continuous-state diffusion along microtubules driven by a flashing binding potential, where the cargo particle is elastically attached to the motor. Depending on the cargo size, the loading force, the amplitude of the binding potential, the turnover frequency of the molecular motor enzyme, and the linker stiffness we demonstrate that the motor transport may turn out either normal or anomalous, as indeed measured experimentally. We show how a highly efficient normal active transport mediated by motors may emerge despite the passive anomalous diffusion of the cargo, and study the intricate effects of the elastic linker. Under different, well specified conditions the microtubule-based motor transport becomes anomalously slow and thus significantly less efficient.
Anomalous diffusion is frequently described by scaled Brownian motion (SBM){,} a Gaussian process with a power-law time dependent diffusion coefficient. Its mean squared displacement is ?x2(t)? [similar{,} equals] 2K(t)t with K(t) [similar{,} equals] t[small alpha]-1 for 0 < [small alpha] < 2. SBM may provide a seemingly adequate description in the case of unbounded diffusion{,} for which its probability density function coincides with that of fractional Brownian motion. Here we show that free SBM is weakly non-ergodic but does not exhibit a significant amplitude scatter of the time averaged mean squared displacement. More severely{,} we demonstrate that under confinement{,} the dynamics encoded by SBM is fundamentally different from both fractional Brownian motion and continuous time random walks. SBM is highly non-stationary and cannot provide a physical description for particles in a thermalised stationary system. Our findings have direct impact on the modelling of single particle tracking experiments{,} in particular{,} under confinement inside cellular compartments or when optical tweezers tracking methods are used.
Probably no other field of statistical physics at the borderline of soft matter and biological physics has caused such a flurry of papers as polymer translocation since the 1994 landmark paper by Bezrukov, Vodyanoy, and Parsegian and the study of Kasianowicz in 1996. Experiments, simulations, and theoretical approaches are still contributing novel insights to date, while no universal consensus on the statistical understanding of polymer translocation has been reached. We here collect the published results, in particular, the famous–infamous debate on the scaling exponents governing the translocation process. We put these results into perspective and discuss where the field is going. In particular, we argue that the phenomenon of polymer translocation is non-universal and highly sensitive to the exact specifications of the models and experiments used towards its analysis.