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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.
We consider the effect of global repulsive coupling on an ensemble of identical excitable elements. An increase of the coupling strength destabilizes the synchronous equilibrium and replaces it with many attracting oscillatory states, created in the transcritical heteroclinic bifurcation. The period of oscillations is inversely proportional to the distance from the critical parameter value. If the elements interact with the global field via the first Fourier harmonics of their phases, the stable equilibrium is in one step replaced by the attracting continuum of periodic motions.
We consider collective dynamics in the ensemble of serially connected spin-torque oscillators governed by the Landau-Lifshitz-Gilbert-Slonczewski magnetization equation. Proximity to homoclinicity hampers synchronization of spin-torque oscillators: when the synchronous ensemble experiences the homoclinic bifurcation, the growth rate per oscillation of small deviations from the ensemble mean diverges. Depending on the configuration of the contour, sufficiently strong common noise, exemplified by stochastic oscillations of the current through the circuit, may suppress precession of the magnetic field for all oscillators. We derive the explicit expression for the threshold amplitude of noise, enabling this suppression.
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.
Realization of all-optically controlled and efficient DNA compaction is the major motivation in the study of interactions between DNA and photosensitive surfactants. In this article, using recently published approach of phase diagram construction [Y. Zakrevskyy, P. Cywinski, M. Cywinska, J. Paasche, N. Lomadze, O. Reich, H.-G. Lohmannsroben, and S. Santer, J. Chem. Phys. 140, 044907 (2014)], a strategy for substantial reduction of compaction agent concentration and simultaneous maintaining the light-induced decompaction efficiency is proposed. The role of ionic strength (NaCl concentration), as a very important environmental parameter, and surfactant structure (spacer length) on the changes of positions of phase transitions is investigated. Increase of ionic strength leads to increase of the surfactant concentration needed to compact DNA molecule. However, elongation of the spacer results to substantial reduction of this concentration. DNA compaction by surfactants with longer tails starts to take place in diluted solutions at charge ratios Z < 1 and is driven by azobenzene-aggregation compaction mechanism, which is responsible for efficient decompaction. Comparison of phase diagrams for different DNA-photosensitive surfactant systems allowed explanation and proposal of a strategy to overcome previously reported limitations of the light-induced decompaction for complexes with increasing surfactant hydrophobicity. (C) 2014 AIP Publishing LLC.
Recently, photosensitive surfactants have re-attracted considerable attention. It has been shown that their association with oppositely charged biologically important polyelectrolytes, such as DNA or microgels, can be efficiently manipulated simply by light exposure. In this article, we investigate the self-assembly of photosensitive surfactants as well as their interactions with DNA by calorimetric and spectroscopic methods. Critical micelle concentration (CMC), standard micellization enthalpy, entropy, and Gibbs energy were determined in different conditions (ionic strengths and temperatures) for a series of cationic surfactants with an azobenzene group in their tail. It is shown, that aggregation forces of photosensitive units play an important role in the micellization giving the major contribution to the micellization enthalpy. The onset of the aggregation can be traced from shift of the absorption peak position in the UV-visible spectrum. Titration UV-visible spectroscopy is used as an alternative, simple, and sensitive approach to estimate CMC. The titration UV-visible spectroscopy was also employed to investigate interactions (CAC: critical aggregation concentration, precipitation, and colloidal stabilization) in the DNA-surfactant complex.
The light-induced reversible switching of the swelling of microgel particles triggered by photo-isomerization and binding/unbinding of a photosensitive azobenzene-containing surfactant is reported. The interactions between the microgel (N-isopropylacrylamide, co-monomer: allyl acetic acid, crosslinker: N,N'-methylenebisacrylamide) and the surfactant are studied by UV-Vis spectroscopy, dynamic and electrophoretic light scattering measurements. Addition of the surfactant above a critical concentration leads to contraction/collapse of the microgel. UV light irradiation results in trans-cis isomerization of the azobenzene unit incorporated into the surfactant tail and causes an unbinding of the more hydrophilic cis isomer from the microgel and its reversible swelling. The reversible contraction can be realized by blue light irradiation that transfers the surfactant back to the more hydrophobic trans conformation, in which it binds to the microgel. The phase diagram of the surfactant-microgel interaction and transitions (aggregation, contraction, and precipitation) is constructed and allows prediction of changes in the system when the concentration of one or both components is varied. Remote and reversible switching between different states can be realized by either UV or visible light irradiation.
We report on the interaction of cationic azobenzene-containing surfactant with DNA investigated by absorption and fluorescence spectroscopy, dynamic light scattering, and atomic force microscopy. The properties of the surfactant can be controlled with light by reversible switching of the azobenzene unit, incorporated into the surfactant tail, between a hydrophobic trans (visible irradiation) and a hydrophilic cis (UV irradiation) configuration. The influence of the trans-cis isomerization of the azobenzene on the compaction process of DNA molecules and the role of both isomers in the formation and colloidal stability of DNA-surfactant complexes is discussed. It is shown that the trans isomer plays a major role in the DNA compaction process. The influence of the cis isomer on the DNA coil configuration is rather small. The construction of a phase diagram of the DNA concentration versus surfactant/DNA charge ratio allows distancing between three major phases: colloidally stable and unstable compacted globules, and extended coil conformation. There is a critical concentration of DNA above which the compacted globules can be hindered from aggregation and precipitation by adding an appropriate amount of the surfactant in the trans configuration. This is because of the compensation of hydrophobicity of the globules with an increasing amount of the surfactant. Below the critical DNA concentration, the compacted globules are colloidally stable and can be reversibly transferred with light to an extended coil state.
Stochastic bifurcations and coherencelike resonance in a self-sustained bistable noisy oscillator
(2010)
We investigate the influence of additive Gaussian white noise on two different bistable self-sustained oscillators: Duffing-Van der Pol oscillator with hard excitation and a model of a synthetic genetic oscillator. In the deterministic case, both oscillators are characterized with a coexistence of a stable limit cycle and a stable equilibrium state. We find that under the influence of noise, their dynamics can be well characterized through the concept of stochastic bifurcation, consisting in a qualitative change of the stationary amplitude distribution. For the Duffing-Van der Pol oscillator analytical results, obtained for a quasiharmonic approach, are compared with the result of direct computer simulations. In particular, we show that the dynamics is different for isochronous and anisochronous systems. Moreover, we find that the increase of noise intensity in the isochronous regime leads to a narrowing of the spectral line. This effect is similar to coherence resonance. However, in the case of anisochronous systems, this effect breaks down and a new phenomenon, anisochronous-based stochastic bifurcation occurs.
The dynamical structure of genetic networks determines the occurrence of various biological mechanisms, such as cellular differentiation. However, the question of how cellular diversity evolves in relation to the inherent stochasticity and intercellular communication remains still to be understood. Here, we define a concept of stochastic bifurcations suitable to investigate the dynamical structure of genetic networks, and show that under stochastic influence, the expression of given proteins of interest is defined via the probability distribution of the phase variable, representing one of the genes constituting the system. Moreover, we show that under changing stochastic conditions, the probabilities of expressing certain concentration values are different, leading to different functionality of the cells, and thus to differentiation of the cells in the various types.
We propose a fibre-based approach for generation of optical frequency combs (OFCs) with the aim of calibration of astronomical spectrographs in the low and medium-resolution range. This approach includes two steps: in the first step, an appropriate state of optical pulses is generated and subsequently moulded in the second step delivering the desired OFC. More precisely, the first step is realised by injection of two continuous-wave (CW) lasers into a conventional single-mode fibre, whereas the second step generates a broad OFC by using the optical solitons generated in step one as initial condition. We investigate the conversion of a bichromatic input wave produced by two initial CW lasers into a train of optical solitons, which happens in the fibre used as step one. Especially, we are interested in the soliton content of the pulses created in this fibre. For that, we study different initial conditions (a single cosine-hump, an Akhmediev breather, and a deeply modulated bichromatic wave) by means of soliton radiation beat analysis and compare the results to draw conclusion about the soliton content of the state generated in the first step. In case of a deeply modulated bichromatic wave, we observed the formation of a collective soliton crystal for low input powers and the appearance of separated solitons for high input powers. An intermediate state showing the features of both, the soliton crystal and the separated solitons, turned out to be most suitable for the generation of OFC for the purpose of calibration of astronomical spectrographs.
We investigate the generation of optical frequency combs through a cascade of four-wave mixing processes in nonlinear fibres with optimised parameters. The initial optical field consists of two continuous-wave lasers with frequency separation larger than 40 GHz (312.7 pm at 1531 nm). It propagates through three nonlinear fibres. The first fibre serves to pulse shape the initial sinusoidal-square pulse, while a strong pulse compression down to sub-100 fs takes place in the second fibre which is an amplifying erbium-doped fibre. The last stage is a low-dispersion highly nonlinear fibre where the frequency comb bandwidth is increased and the line intensity is equalised. We model this system using the generalised nonlinear Schrodinger equation and investigate it in terms of fibre lengths, fibre dispersion, laser frequency separation and input powers with the aim to minimise the frequency comb noise. With the support of the numerical results, a frequency comb is experimentally generated, first in the near infra-red and then it is frequency-doubled into the visible spectral range. Using a MUSE-type spectrograph, we evaluate the comb performance for astronomical wavelength calibration in terms of equidistancy of the comb lines and their stability.
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.
We study several algorithms to simulate bone mass loss in two-dimensional and three-dimensional computed tomography bone images. The aim is to extrapolate and predict the bone loss, to provide test objects for newly developed structural measures, and to understand the physical mechanisms behind the bone alteration. Our bone model approach differs from those already reported in the literature by two features. First, we work with original bone images, obtained by computed tomography (CT); second, we use structural measures of complexity to evaluate bone resorption and to compare it with the data provided by CT. This gives us the possibility to test algorithms of bone resorption by comparing their results with experimentally found dependencies of structural measures of complexity, as well as to show efficiency of the complexity measures in the analysis of bone models. For two-dimensional images we suggest two algorithms, a threshold algorithm and a virtual slicing algorithm. The threshold algorithm simulates bone resorption on a boundary between bone and marrow, representing an activity of osteoclasts. The virtual slicing algorithm uses a distribution of the bone material between several virtually created slices to achieve statistically correct results, when the bone-marrow transition is not clearly defined. These algorithms have been tested for original CT 10 mm thick vertebral slices and for simulated 10 mm thick slices constructed from ten I mm thick slices. For three-dimensional data, we suggest a variation of the threshold algorithm and apply it to bone images. The results of modeling have been compared with CT images using structural measures of complexity in two- and three-dimensions. This comparison has confirmed credibility of a virtual slicing modeling algorithm for two-dimensional data and a threshold algorithm for three-dimensional data
We examine the influence of noise on the propagation of harmonic signals with two frequencies through discrete bistable media. We show that random fluctuations enhance propagation of this kind of signals for low coupling strengths, similarly to what happens with purely monochromatic signals. As a more relevant finding, we observe that the frequency being propagated with better efficiency can be selected by tuning the intensity of the noise, in such a way that for large noises the highest frequency is transmitted better than the lower one, whereas for small noises the reverse holds. Such a noise-induced frequency selection can be expected to exist for general multifrequency harmonic signals.
Control of noise-induced oscillations of a pendulum with a rondomly vibrating suspension axis
(1997)
We have recently reported the phenomenon of doubly stochastic resonance [Phys. Rev. Lett. 85, 227 (2000)], a synthesis of noise-induced transition and stochastic resonance. The essential feature of this phenomenon is that multiplicative noise induces a bimodality and additive noise causes stochastic resonance behavior in the induced structure. In the present paper we outline possible applications of this effect and design a simple lattice of electronic circuits for the experimental realization of doubly stochastic resonance.
We report on the effect of vibrational resonance in a spatially extended system of coupled noisy oscillators under the action of two periodic forces, a low-frequency one (signal) and a high-frequency one (carrier). Vibrational resonance manifests itself in the fact that for optimally selected values of high-frequency force amplitude, the response of the system to a low-frequency signal is optimal. This phenomenon is a synthesis of two effects, a noise- induced phase transition leading to bistability, and a conventional vibrational resonance, resulting in the optimization of signal processing. Numerical simulations, which demonstrate this effect for an extended system, can be understood by means of a zero-dimensional "effective" model. The behavior of this "effective" model is also confirmed by an experimental realization of an electronic circuit.
Doubly stochastic resonance
(2000)
We report the effect of doubly stochastic resonance which appears in nonlinear extended systems if the influence of noise is twofold: A multiplicative noise induces bimodality of the mean field of the coupled network and an independent additive noise governs the dynamic behavior in response to small periodic driving. For optimally selected values of the additive noise intensity stochastic resonance is observed, which is manifested by a maximal coherence between the dynamics of the mean field and the periodic input. Numerical simulations of the signal-to-noise ratio and theoretical results from an effective two state model are in good quantitative agreement.
We show that external fluctuations are able to induce propagation of harmonic signals through monostable media. This property is based on the phenomenon of doubly stochastic resonance, where the joint action of multiplicative noise and spatial coupling induces bistability in an otherwise monostable extended medium, and additive noise resonantly enhances the response of the system to a harmonic forcing. Under these conditions, propagation of the harmonic signal through the unforced medium i observed for optimal intensities of the two noises. This noise-induced propagation is studied and quantified in a simple model of coupled nonlinear electronic circuits.
The absorption of TeV gamma-ray photons produced in relativistic jets by surrounding soft photon fields is a long-standing problem of jet physics. In some cases, the most likely emission site close to the central black hole is ruled out because of the high opacity caused by strong optical and infrared photon sources, such as the broad-line region. Mostly neglected for jet modelling is the absorption of gamma-rays in the starlight photon field of the host galaxy. Analysing the absorption for arbitrary locations and observation angles of the gamma-ray emission site within the host galaxy, we find that the distance to the galaxy centre, the observation angle, and the distribution of starlight in the galaxy are crucial for the amount of absorption. We derive the absorption value for a sample of 20 TeV-detected blazars with a redshift z(r) < 0.2. The absorption value of the gamma-ray emission located in the galaxy centre may be as high as 20 per cent, with an average value of 6 per cent. This is important in order to determine the intrinsic blazar parameters. We see no significant trends in our sample between the degree of absorption and host properties, such as starlight emissivity, galactic size, half-light radius, and redshift. While the uncertainty of the spectral properties of the extragalactic background light exceeds the effect of absorption by stellar light from the host galaxy in distant objects, the latter is a dominant effect in nearby sources. It may also be revealed in a differential comparison of sources with similar redshifts.
We use the MusE GAs FLOw and Wind (MEGAFLOW) survey to study the kinematics of extended disc-like structures of cold gas around z approximate to 1 star-forming galaxies. The combination of VLT/MUSE and VLT/UVES observations allows us to connect the kinematics of the gas measured through MgII quasar absorption spectroscopy to the kinematics and orientation of the associated galaxies constrained through integral field spectroscopy. Confirming previous results, we find that the galaxy-absorber pairs of the MEGAFLOW survey follow a strong bimodal distribution, consistent with a picture of MgII absorption being predominantly present in outflow cones and extended disc-like structures. This allows us to select a bona-fide sample of galaxy-absorber pairs probing these discs for impact paramometers of 10-70 kpc. We test the hypothesis that the disc-like gas is co-rotating with the galaxy discs, and find that for seven out of nine pairs the absorption velocity shares the sign of the disc velocity, disfavouring random orbits. We further show that the data are roughly consistent with inflow velocities and angular momenta predicted by simulations, and that the corresponding mass accretion rates are sufficient to balance the star formation rates.
Organic solar cells (OSCs) have progressed rapidly in recent years through the development of novel organic photoactive materials, especially non-fullerene acceptors (NFAs). Consequently, OSCs based on state-of-the-art NFAs have reached significant milestones, such as similar to 19% power conversion efficiencies (PCEs) and small energy losses (less than 0.5 eV). Despite these significant advances, understanding of the interplay between molecular structure and optoelectronic properties lags significantly behind. For example, despite the theoretical framework for describing the energetic disorder being well developed for the case of inorganic semiconductors, the question of the applicability of classical semiconductor theories in analyzing organic semiconductors is still under debate. A general observation in the inorganic field is that inorganic photovoltaic materials possessing a polycrystalline microstructure exhibit suppressed disorder properties and better charge carrier transport compared to their amorphous analogs. Accordingly, this principle extends to the organic semiconductor field as many organic photovoltaic materials are synthesized to pursue polycrystalline-like features. Yet, there appears to be sporadic examples that exhibit an opposite trend. However, full studies decoupling energetic disorder from aggregation effects have largely been left out. Hence, the potential role of the energetic disorder in OSCs has received little attention. Interestingly, recently reported state-of-the-art NFA-based devices could achieve a small energetic disorder and high PCE at the same time; and interest in this investigation related to the disorder properties in OSCs was revived. In this contribution, progress in terms of the correlation between molecular design and energetic disorder is reviewed together with their effects on the optoelectronic mechanism and photovoltaic performance. Finally, the specific challenges and possible solutions in reducing the energetic disorder of OSCs from the viewpoint of materials and devices are proposed.
X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (10(20) W cm(-2)) of x-rays at wavelengths down to similar to 1 Angstrom, and HHG provides unprecedented time resolution (similar to 50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of similar to 280 eV (44 Angstroms) and the bond length in methane of similar to 1 Angstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Angstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Angstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.
We present deep optical observations of the gravitational lens system CLASS B0218 + 357, from which we derive an estimate for the Hubble constant (H-0). Extensive radio observations using the VLA, MERLIN, the VLBA and VLBI have reduced the degeneracies between H-0 and the mass model parameters in this lens to one involving only the position of the radio-quiet lensing galaxy with respect to the lensed images. B0218 + 357 has an image separation of only 334 mas, so optical observations have, up until now, been unable to resolve the lens galaxy from the bright lensed images. Using the new Advanced Camera for Surveys (ACS), installed on the Hubble Space Telescope in 2002, we have obtained deep optical images of the lens system and surrounding field. These observations have allowed us to determine the separation between the lens galaxy centre and the brightest image, and so estimate H-0. We find an optical galaxy position, and hence an H0 value, that varies depending on our approach to the spiral arms in B0218 + 357. If the most prominent spiral arms are left unmasked, we find H-0 = 70 +/- 5 km s(-1) Mpc(-1) (95 per cent confidence). If the spiral arms are masked out, we find H-0 = 61 +/- 7 km s(-1) Mpc(-1) (95 per cent confidence)
We investigate the effects of rotation on the behavior of the helium-burning shell source in accreting carbon- oxygen white dwarfs, in the context of the single degenerate Chandrasekhar mass progenitor scenario for type la supernovae (SNe Ia). We model the evolution of helium-accreting white dwarfs of initially 1 M-circle dot, assuming four different constant accretion rates (2, 3, 5 and 10 x 10(-7) M-circle dot/yr). In a one-dimensional approximation, we compute the mass accretion and subsequent nuclear fusion of helium into carbon and oxygen, as well as angular momentum accretion, angular momentum transport inside the white dwarf, and rotationally induced chemical mixing. Our models show two major effects of rotation: a) The helium-burning nuclear shell source in the rotating models is much more stable than in corresponding non-rotating models - which increases the likelihood that accreting white dwarfs reach the stage of central carbon ignition. This effect is mainly due to rotationally induced mixing at the CO/He interface which widens the shell source, and due to the centrifugal force lowering the density and degeneracy at the shell source location. b) The C/O-ratio in the layers which experience helium shell burning - which may affect the energy of an SN Ia explosion - is strongly decreased by the rotationally induced mixing of a-particles into the carbon-rich layers. We discuss implications of our results for the evolution of SNe la progenitors
Low-frequency fluctuations are pervasively observed in the solar wind. The present paper theoretically calculates the steady state spectra of low-frequency electromagnetic (EM) fluctuations of the Alfvenic type for thermal equilibrium plasma. The analysis is based upon a recently formulated theory of spontaneously emitted EM fluctuations in magnetized thermal plasmas. It is found that the fluctuations in the magnetosonic mode branch is constant, while the kinetic Alfvenic mode spectrum is dependent on a form factor that is a function of perpendicular wave number. Potential applicability of the present work in the wider context of heliospheric research is also discussed.
Self-organized patterns in the actin cytoskeleton are essential for eukaryotic cellular life. They are the building blocks of many functional structures that often operate simultaneously to facilitate, for example, nutrient uptake and movement of cells. However, identifying how qualitatively distinct actin patterns can coexist remains a challenge.
Using bifurcation theory of a mass conserved activator-inhibitor system, we uncover a generic mechanism of how different actin waves-traveling waves and excitable pulses- organize and simultaneously emerge.
Live-cell imaging experiments indeed reveal that narrow, planar, and fast-moving excitable pulses may coexist with ring-shaped macropinocytic actin waves in the cortex of motile amoeboid cells.
Excitable solitons
(2020)
Excitable pulses are among the most widespread dynamical patterns that occur in many different systems, ranging from biological cells to chemical reactions and ecological populations. Traditionally, the mutual annihilation of two colliding pulses is regarded as their prototypical signature. Here we show that colliding excitable pulses may exhibit solitonlike crossover and pulse nucleation if the system obeys a mass conservation constraint. In contrast to previous observations in systems without mass conservation, these alternative collision scenarios are robustly observed over a wide range of parameters. We demonstrate our findings using a model of intracellular actin waves since, on time scales of wave propagations over the cell scale, cells obey conservation of actin monomers. The results provide a key concept to understand the ubiquitous occurrence of actin waves in cells, suggesting why they are so common, and why their dynamics is robust and long-lived.
X-ray spectroscopy is a powerful tool to study the local charge distribution of chemical systems. Together with the liquid jet it becomes possible to probe chemical systems in their natural environment, the liquid phase. In this work, we present X-ray absorption (XA), X-ray emission (XE) and resonant inelastic X-ray scattering (RIXS) data of pure water and various salt solutions and show the possibilities these methods offer to elucidate the nature of ion-water interaction.
In the current work, X-ray emission spectra of aqueous solutions of different inorganic salts within the Hofmeister series are presented. The results reflect the direct interaction of the ions with the water molecules and therefore, reveal general properties of the salt-water interactions. Within the experimental precision a significant effect of the ions on the water structure has been observed but no ordering according to the structure maker/structure breaker concept could be mirrored in the results indicating that the Hofmeister effect if existent may be caused by more complex interactions.
Hydration shells around ions are crucial for many fundamental biological and chemical processes. Their local physicochemical properties are quite different from those of bulk water and hard to probe experimentally. We address this problem by combining soft X-ray spectroscopy using a liquid jet and molecular dynamics (MD) simulations together with ab initio electronic structure calculations to elucidate the water ion interaction in a MgCl2 solution at the molecular level. Our results reveal that salt ions mainly affect the electronic properties of water molecules in close vicinity and that the oxygen K-edge X-ray emission spectrum of water molecules in the first solvation shell differs significantly from that of bulk water. Ion-specific effects are identified by fingerprint features in the water X-ray emission spectra. While Mg2+ ions cause a bathochromic shift of the water lone pair orbital, the 3p orbital of the Cl- ions causes an additional peak in the water emission spectrum at around 528 eV.
This paper presents a study of the surface properties of two Ce/Zr mixed oxides with different reducibility, obtained by applying distinct thermal ageing treatments to an oxide with the composition Ce0.62Zr0.38O2. The surface composition was investigated by XPS. Chemical reactivity of the surface was studied by adsorption of the probe molecules CO2, D-2 and methanol. Nanostructural characterization was carried out by XRD, Raman and high-resolution Eu3+ spectroscopy (FLNS). The characterization showed only slight variations in surface composition and bulk Ce-Zr distribution, but hardy differences concerning the type and strength of acidic surface centres, as well as strong differences in the ability to dissociate hydrogen. Structural variations between both samples were identified by comparing the optical spectra of Eu3+ in surface doped samples.
We demonstrate the emergence of a complex state in a homogeneous ensemble of globally coupled identical oscillators, reminiscent of chimera states in nonlocally coupled oscillator lattices. In this regime some part of the ensemble forms a regularly evolving cluster, while all other units irregularly oscillate and remain asynchronous. We argue that the chimera emerges because of effective bistability, which dynamically appears in the originally monostable system due to internal delayed feedback in individual units. Additionally, we present two examples of chimeras in bistable systems with frequency-dependent phase shift in the global coupling.
Plain Language Summary Cassini flew through the gap between Saturn and its rings for 22 times before plunging into the atmosphere of Saturn, ending its 20-year mission. The radio and plasma waves instrument on board Cassini helped quantify the dust hazard in this previously unexplored region. The measured density of large dust particles was much lower than expected, allowing high-value science observations during the subsequent Grand Finale orbits.
During the Ring Grazing orbits near the end of Cassini mission, the spacecraft crossed the equatorial plane near the orbit of Janus/Epimetheus (similar to 2.5 Rs). This region is populated with dust particles that can be detected by the Radio and Plasma Wave Science (RPWS) instrument via an electric field antenna signal. Analysis of the voltage waveforms recorded on the RPWS antennas provides estimations of the density and size distribution of the dust particles. Measured RPWS profiles, fitted with Lorentzian functions, are shown to be mostly consistent with the Cosmic Dust Analyzer, the dedicated dust instrument on board Cassini. The thickness of the dusty ring varies between 600 and 1,000 km. The peak location shifts north and south within 100 km of the ring plane, likely a function of the precession phase of Janus orbit.
Inverted perovskite solar cells still suffer from significant non-radiative recombination losses at the perovskite surface and across the perovskite/C₆₀ interface, limiting the future development of perovskite-based single- and multi-junction photovoltaics. Therefore, more effective inter- or transport layers are urgently required. To tackle these recombination losses, we introduce ortho-carborane as an interlayer material that has a spherical molecular structure and a three-dimensional aromaticity. Based on a variety of experimental techniques, we show that ortho-carborane decorated with phenylamino groups effectively passivates the perovskite surface and essentially eliminates the non-radiative recombination loss across the perovskite/C₆₀ interface with high thermal stability. We further demonstrate the potential of carborane as an electron transport material, facilitating electron extraction while blocking holes from the interface. The resulting inverted perovskite solar cells deliver a power conversion efficiency of over 23% with a low non-radiative voltage loss of 110 mV, and retain >97% of the initial efficiency after 400 h of maximum power point tracking. Overall, the designed carborane based interlayer simultaneously enables passivation, electron-transport and hole-blocking and paves the way toward more efficient and stable perovskite solar cells.
Achieving the highest power conversion efficiencies in bulk heterojunction organic solar cells requires a morphology that delivers electron and hole percolation pathways for optimized transport, plus sufficient donor:acceptor contact area for near unity charge transfer state formation. This is a significant structural challenge, particularly in semiconducting polymer:fullerene systems. This balancing act in the model high efficiency PTB7:PC70BM blend is studied by tuning the donor:acceptor ratio, with a view to understanding the recombination loss mechanisms above and below the fullerene transport percolation threshold. The internal quantum efficiency is found to be strongly correlated to the slower carrier mobility in agreement with other recent studies. Furthermore, second-order recombination losses dominate the shape of the current density-voltage curve in efficient blend combinations, where the fullerene phase is percolated. However, below the charge transport percolation threshold, there is an electric-field dependence of first-order losses, which includes electric-field-dependent photogeneration. In the intermediate regime, the fill factor appears to be limited by both first- and second-order losses. These findings provide additional basic understanding of the interplay between the bulk heterojunction morphology and the order of recombination in organic solar cells. They also shed light on the limitations of widely used transport models below the percolation threshold.
Polymeric electrophosphorescent LEDs with internal quantum efficiencies approaching unity have been fabricated. Such performance levels are previously unknown for OLEDs. The key to this success is redox chemically doped oxetane- crosslinkable hole-transporting layers with multilayer capability (see figure). They improve hole injection and act as electron-blocking layers, without the need to include exciton-or hole-blocking layers
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.
Suppression of the keto-emission in polyfluorene light-emitting diodes : Experiments and models
(2004)
The spectral characteristics of polyfluorene (PF)-based light-emitting diodes (LEDs) containing a defined low concentration of either keto-defects or of the polymer poly(9.9-octylfuorene-co-benzothiadiazole) (F8BT) are preseneted. Both types of blend layers were tested in different device configurations with respect to the relative and absolute intensities of green blue emission components. It is shown that blending hole-transporting molecules into the emission layer at low concentration or incorporation of a suitable hole-transport layer reduces the green emission contribution in the electroluminescence (EL) spectrum of the PF:F8BT blend, which is similar to what is observed for the keto- containing PF layer. We conclude that the keto-defects in PF homopolymer layers mainly constitute weakly emissive electron traps, in agreement with the results of quantum-mechanical calculations
A commercially available Ir complex has been employed for the preparation of highly efficient (see Figure) single-layer phosphorescent polymer light,emitting diodes by use of appropriate thermal treatment and proper adjustment of the layer composition. These devices exhibit essentially no dependence of the driving field on the concentration of the Ir complex, suggesting that the build-up of space-charge in the layer is insignificant
We demonstrate efficient single-layer polymer phosphorescent light-emitting devices based on a green-emitting iridium complex and a polymer host co-doped with electron-transporting and hole-transporting molecules. These devices can be operated at relatively low voltages, resulting in a power conversion efficiency of up to 24 lm/W at luminous efficiencies exceeding 30 cd/A. The overall performances of these devices suggest that efficient electrophosphorescent devices with acceptable operating voltages can be achieved in very simple device structures fabricated by spin coating. (C) 2004 American Institute of Physics
We report that the performances of blue polymer electrophosphorescent devices are crucially depending on the choice of the electron transporting material incorporated into the emissive layer. Devices with 1,3-bis[(4-tert- butylphenyl)-1,3,4-oxidiazolyl]phenylene (OXD-7) doped at similar to 40 wt% into a poly(vinylcarbazole) matrix exhibited significantly higher efficiencies than those with 2-(4-biphenylyl)-5-(4-tert-butylphenyl)-1,3,4-oxadiazole (PBD), yielding maximum luminous and power efficiency values of 18.2 Cd/A and 8.8 lm/W, respectively. Time resolved photoluminescence measurements revealed a long lifetime phosphorescence component in layers with PBD, which we assign to significant triplet harvesting by this electron-transporting component. (c) 2006 American Institute of Physics
Imaging CF3I conical intersection and photodissociation dynamics with ultrafast electron diffraction
(2018)
Conical intersections play a critical role in excited-state dynamics of polyatomic molecules because they govern the reaction pathways of many nonadiabatic processes. However, ultrafast probes have lacked sufficient spatial resolution to image wave-packet trajectories through these intersections directly. Here, we present the simultaneous experimental characterization of one-photon and two-photon excitation channels in isolated CF3I molecules using ultrafast gas-phase electron diffraction. In the two-photon channel, we have mapped out the real-space trajectories of a coherent nuclear wave packet, which bifurcates onto two potential energy surfaces when passing through a conical intersection. In the one-photon channel, we have resolved excitation of both the umbrella and the breathing vibrational modes in the CF3 fragment in multiple nuclear dimensions. These findings benchmark and validate ab initio nonadiabatic dynamics calculations.
We present results on ultrafast gas electron diffraction (UGED) experiments with femtosecond resolution using the MeV electron gun at SLAC National Accelerator Laboratory. UGED is a promising method to investigate molecular dynamics in the gas phase because electron pulses can probe the structure with a high spatial resolution. Until recently, however, it was not possible for UGED to reach the relevant timescale for the motion of the nuclei during a molecular reaction. Using MeV electron pulses has allowed us to overcome the main challenges in reaching femtosecond resolution, namely delivering short electron pulses on a gas target, overcoming the effect of velocity mismatch between pump laser pulses and the probe electron pulses, and maintaining a low timing jitter. At electron kinetic energies above 3 MeV, the velocity mismatch between laser and electron pulses becomes negligible. The relativistic electrons are also less susceptible to temporal broadening due to the Coulomb force. One of the challenges of diffraction with relativistic electrons is that the small de Broglie wavelength results in very small diffraction angles. In this paper we describe the new setup and its characterization, including capturing static diffraction patterns of molecules in the gas phase, finding time-zero with sub-picosecond accuracy and first time-resolved diffraction experiments. The new device can achieve a temporal resolution of 100 fs root-mean-square, and sub-angstrom spatial resolution. The collimation of the beam is sufficient to measure the diffraction pattern, and the transverse coherence is on the order of 2 nm. Currently, the temporal resolution is limited both by the pulse duration of the electron pulse on target and by the timing jitter, while the spatial resolution is limited by the average electron beam current and the signal-to-noise ratio of the detection system. We also discuss plans for improving both the temporal resolution and the spatial resolution.
Imaging changes in molecular geometries on their natural femtosecond timescale with sub-Angstrom spatial precision is one of the critical challenges in the chemical sciences, as the nuclear geometry changes determine the molecular reactivity. For photoexcited molecules, the nuclear dynamics determine the photoenergy conversion path and efficiency. Here we report a gas-phase electron diffraction experiment using megaelectronvolt (MeV) electrons, where we captured the rotational wavepacket dynamics of nonadiabatically laser-aligned nitrogen molecules. We achieved a combination of 100 fs root-mean-squared temporal resolution and sub-Angstrom (0.76 angstrom) spatial resolution that makes it possible to resolve the position of the nuclei within the molecule. In addition, the diffraction patterns reveal the angular distribution of the molecules, which changes from prolate (aligned) to oblate (anti-aligned) in 300 fs. Our results demonstrate a significant and promising step towards making atomically resolved movies of molecular reactions.
Observing the motion of the nuclear wave packets during a molecular reaction, in both space and time, is crucial for understanding and controlling the outcome of photoinduced chemical reactions. We have imaged the motion of a vibrational wave packet in isolated iodine molecules using ultrafast electron diffraction with relativistic electrons. The time-varying interatomic distance was measured with a precision 0.07 angstrom and temporal resolution of 230 fs full width at half maximum. The method is not only sensitive to the position but also the shape of the nuclear wave packet.
Entanglement combing
(2009)
We show that all multipartite pure states can, under local operations, be transformed into bipartite pairwise entangled states in a "lossless fashion": An arbitrary distinguished party will keep pairwise entanglement with all other parties after the asymptotic protocol-decorrelating all other parties from each other-in a way that the degree of entanglement of this party with respect to the rest will remain entirely unchanged. The set of possible entanglement distributions of bipartite pairs is also classified. Finally, we point out several applications of this protocol as a useful primitive in quantum information theory.
It has been found in recent measurements that the singlet-to-triplet exciton ratio in organic light-emitting diodes (OLEDs) is larger than expected from spin degeneracy, and that singlet excitons form at a larger rate than triplets. We employed the technique of optically detected magnetic resonance to measure the spin-dependent exciton formation rates in films of a polymer and corresponding monomer, and explore the relation between the formation rates and the actual singlet-to-triplet ratio measured previously in OLEDs. We found that the spin-dependent exciton formation rates can indeed quantitatively explain the observed exciton yields, and that singlet formation rates and yields are significantly enhanced only in polymer OLEDs, but not in OLEDs made from the corresponding monomer
Magnetic reconnection is a multi-faceted process of energy conversion in astrophysical, space and laboratory plasmas that operates at microscopic scales but has macroscopic drivers and consequences.
Solar flares present a key laboratory for its study, leaving imprints of the microscopic physics in radiation spectra and allowing the macroscopic evolution to be imaged, yet a full observational characterization remains elusive.
Here we combine high resolution imaging and spectral observations of a confined solar flare at multiple wavelengths with data-constrained magnetohydrodynamic modeling to study the dynamics of the flare plasma from the current sheet to the plasmoid scale. The analysis suggests that the flare resulted from the interaction of a twisted magnetic flux rope surrounding a filament with nearby magnetic loops whose feet are anchored in chromospheric fibrils. Bright cusp-shaped structures represent the region around a reconnecting separator or quasi-separator (hyperbolic flux tube).
The fast reconnection, which is relevant for other astrophysical environments, revealed plasmoids in the current sheet and separatrices and associated unresolved turbulent motions.
Solar flares provide wide range of observational details about fundamental processes involved. Here, the authors show evidence for magnetic reconnection in a strong confined solar flare displaying all four reconnection flows with plasmoids in the current sheet and the separatrices.
In this paper, we propose a revised fractional Brownian motion run with a nonlinear clock (fBm-nlc) model and utilize it to illustrate the microscopic mechanism analysis of the fractal derivative diffusion model with variable coefficient (VC-FDM).
The power-law mean squared displacement (MSD) links the fBm-nlc model and the VC-FDM via the two-parameter power law clock and the Hurst exponent is 0.5.
The MSD is verified by using the experimental points of the chloride ions diffusion in concrete.
When compared to the linear Brownian motion, the results show that the power law MSD of the fBm-nlc is much better in fitting the experimental points of chloride ions in concrete.
The fBm-nlc clearly interprets the VC-FDM and provides a microscopic strategy in characterizing different types of non-Fickian diffusion processes with more different nonlinear functions.
The atmospheric lunar tide is one known source of ionospheric variability. The subject received renewed attention as recent studies found a link between stratospheric sudden warmings and amplified lunar tidal perturbations in the equatorial ionosphere. There is increasing evidence from ground observations that the lunar tidal influence on the ionosphere depends on longitude. We use magnetic field measurements from the CHAMP satellite during July 2000 to September 2010 and from the two Swarm satellites during November 2013 to February 2017 to determine, for the first time, the complete seasonal- longitudinal climatology of the semidiurnal lunar tidal variation in the equatorial electrojet intensity. Significant longitudinal variability is found in the amplitude of the lunar tidal variation, while the longitudinal variability in the phase is small. The amplitude peaks in the Peruvian sector (similar to 285 degrees E) during the Northern Hemisphere winter and equinoxes, and in the Brazilian sector (similar to 325 degrees E) during the Northern Hemisphere summer. There are also local amplitude maxima at similar to 55 degrees E and similar to 120 degrees E. The longitudinal variation is partly due to the modulation of ionospheric conductivities by the inhomogeneous geomagnetic field. Another possible cause of the longitudinal variability is neutral wind forcing by nonmigrating lunar tides. A tidal spectrum analysis of the semidiurnal lunar tidal variation in the equatorial electrojet reveals the dominance of the westward propagating mode with zonal wave number 2 (SW2), with secondary contributions by westward propagating modes with zonal wave numbers 3 (SW3) and 4 (SW4). Eastward propagating waves are largely absent from the tidal spectrum. Further study will be required for the relative importance of ionospheric conductivities and nonmigrating lunar tides.
The geomagnetic activity index Kp is widely used but is restricted by low time resolution (3-hourly) and an upper limit. To address this, new geomagnetic activity indices, Hpo, are introduced. Similar to Kp, Hpo expresses the level of planetary geomagnetic activity in units of thirds (0o, 0+, 1-, 1o, 1+, 2-, horizontal ellipsis ) based on the magnitude of geomagnetic disturbances observed at subauroral observatories. Hpo has a higher time resolution than Kp. 30-min (Hp30) and 60-min (Hp60) indices are produced. The frequency distribution of Hpo is designed to be similar to that of Kp so that Hpo may be used as a higher time-resolution alternative to Kp. Unlike Kp, which is capped at 9o, Hpo is an open-ended index and thus can characterize severe geomagnetic storms more accurately. Hp30, Hp60 and corresponding linearly scaled ap30 and ap60 are available, in near real time, at the GFZ website (https://www.gfz-potsdam.de/en/hpo-index).
In this paper, we report on differences in the response of photosensitive azobenzene containing films upon irradiation with the intensity or polarization interference patterns. Two materials are studied differing in the molecular weight: an azobenzene-containing polymer and a molecular glass formed from a much smaller molecule consisting of three connected azobenzene units. Topography changes occurring along with the changes in irradiation conditions are recorded using a homemade set-up combining an optical part for generation and shaping of interference patterns and an atomic force microscope for acquiring the kinetics of film deformation. In this way, we could reveal the unique behavior of photosensitive materials during the first few minutes of irradiation: the change in topography is initially driven by an increase in the azobenzene free volume along with the transcis isomerization, followed by the mass transport finally resulting in the surface relief grating. This study demonstrates the great potential of our setup to experimentally highlight puzzling processes governing the formation of surface relief gratings. (C) 2014 AIP Publishing LLC.
In this paper, we report on in-situ atomic force microscopy (AFM) studies of topographical changes in azobenzene-containing photosensitive polymer films that are irradiated with light interference patterns. We have developed an experimental setup consisting of an AFM combined with two-beam interferometry that permits us to switch between different polarization states of the two interfering beams while scanning the illuminated area of the polymer film, acquiring corresponding changes in topography in-situ. This way, we are able to analyze how the change in topography is related to the variation of the electrical field vector within the interference pattern. It is for the first time that with a rather simple experimental approach a rigorous assignment can be achieved. By performing in-situ measurements we found that for a certain polarization combination of two interfering beams [namely for the SP (a dagger center dot, a dagger") polarization pattern] the topography forms surface relief grating with only half the period of the interference patterns. Exploiting this phenomenon we are able to fabricate surface relief structures with characteristic features measuring only 140 nm, by using far field optics with a wavelength of 491 nm. We believe that this relatively simple method could be extremely valuable to, for instance, produce structural features below the diffraction limit at high-throughput, and this could significantly contribute to the search of new fabrication strategies in electronics and photonics industry.
When photosensitive azobenzene-containing polymer films are irradiated with light interference patterns, topographic variations in the film develop that follow the local distribution of the electric field vector. The exact correspondence of e.g., the vector orientation in relation to the presence of local topographic minima or maxima is in general difficult to determine. Here, we report on a systematic procedure how this can be accomplished. For this, we devise a new set-up combining an atomic force microscope and two-beam interferometry. With this set-up, it is possible to track the topography change in-situ, while at the same time changing polarization and phase of the impinging interference pattern. This is the first time that an absolute correspondence between the local distribution of electric field vectors and the local topography of the relief grating could be established exhaustively. Our setup does not require a complex mathematical post-processing and its simplicity renders it interesting for characterizing photosensitive polymer films in general.
In this paper two groups supporting different views on the mechanism of light induced polymer deformation argue about the respective underlying theoretical conceptions, in order to bring this interesting debate to the attention of the scientific community. The group of Prof. Nicolae Hurduc supports the model claiming that the cyclic isomerization of azobenzenes may cause an athermal transition of the glassy azobenzene containing polymer into a fluid state, the so-called photo-fluidization concept. This concept is quite convenient for an intuitive understanding of the deformation process as an anisotropic flow of the polymer material. The group of Prof. Svetlana Santer supports the re-orientational model where the mass-transport of the polymer material accomplished during polymer deformation is stated to be generated by the light-induced re-orientation of the azobenzene side chains and as a consequence of the polymer backbone that in turn results in local mechanical stress, which is enough to irreversibly deform an azobenzene containing material even in the glassy state. For the debate we chose three polymers differing in the glass transition temperature, 32 degrees C, 87 degrees C and 95 degrees C, representing extreme cases of flexible and rigid materials. Polymer film deformation occurring during irradiation with different interference patterns is recorded using a homemade set-up combining an optical part for the generation of interference patterns and an atomic force microscope for acquiring the kinetics of film deformation. We also demonstrated the unique behaviour of azobenzene containing polymeric films to switch the topography in situ and reversibly by changing the irradiation conditions. We discuss the results of reversible deformation of three polymers induced by irradiation with intensity (IIP) and polarization (PIP) interference patterns, and the light of homogeneous intensity in terms of two approaches: the re-orientational and the photo-fluidization concepts. Both agree in that the formation of opto-mechanically induced stresses is a necessary prerequisite for the process of deformation. Using this argument, the deformation process can be characterized either as a flow or mass transport.
The interface between thin films of metal and polymer materials play a significant role in modern flexible microelectronics viz., metal contacts on polymer substrates, printed electronics and prosthetic devices. The major emphasis in metal polymer interface is on studying how the externally applied stress in the polymer substrate leads to the deformation and cracks in metal film and vice versa. Usually, the deformation process involves strains varying over large lateral dimensions because of excessive stress at local imperfections. Here we show that the seemingly random phenomena at macroscopic scales can be rendered rather controllable at submicrometer length scales. Recently, we have created a metal polymer interface system with strains varying over periods of several hundred nanometers. This was achieved by exploiting the formation of surface relief grating (SRG) within the azobenzene containing photosensitive polymer film upon irradiation with light interference pattern. Up to a thickness of 60 nm, the adsorbed metal film adapts neatly to the forming relief, until it ultimately ruptures into an array of stripes by formation of highly regular and uniform cracks along the maxima and minima of the polymer topography. This surprising phenomenon has far-reaching implications. This is the first time a direct probe is available to estimate the forces emerging in SRG formation in glassy polymers. Furthermore, crack formation in thin metal films can be studied literally in slow motion, which could lead to substantial improvements in the design process of flexible electronics. Finally, cracks are produced uniformly and at high density, contrary to common sense. This could offer new strategies for precise nanofabrication procedures mechanical in character.
Here, we report on two photosensitive amorphous polymers showing opposite behavior upon exposure to illumination. The first polymer (PAZO) consists of linear backbone to which azobenzene-containing side chains are covalently attached, while in the second polymer (azo-PEI), the azobenzene side chains are attached ionically to a polyelectrolyte backbone. When irradiated through a mask, the PAZO goes away from the intensity maxima, leaving behind topography trenches, while the direction of the mass transport of the azo-PEI polymer points towards the intensity maxima. This kind of behavior has been reported only for certain liquid crystalline polymers that exhibit in-phase reaction on illumination, that is, topography maxima coincides with the intensity maxima. Furthermore, flat nanocrystals placed on top of azo-PEI film was found to be moved together with the mass transport of the underlying polymer film as visualized using in situ atomic force microscopy (AFM) measurements. It was also demonstrated that the two polymer films respond differently on irradiation with the polarization and intensity interference patterns (IPs). To record the kinetic of the surface relief grating formation within two polymers during irradiation with different IPs, we utilized a homemade setup combining the optical part for the generation of IP and AFM. A possible mechanism explaining different responses on the irradiation of amorphous polymers is discussed in the frame of a theoretical model proposed by Saphiannikova et al. (J. Phys. Chem. B 113, 5032-5045 (2009)).
Azo-modified photosensitive polymers offer the interesting possibility to reshape bulk polymers and thin films by UV-irradiation while being in the solid glassy state. The polymer undergoes considerable mass transport under irradiation with a light interference pattern resulting in the formation of surface relief grating (SRG). The forces inscribing this SRG pattern into a thin film are hard to assess experimentally directly. In the current study, we are proposing a method to probe opto-mechanical stresses within polymer films by characterizing the mechanical response of thin metal films (10 nm) deposited on the photosensitive polymer. During irradiation, the metal film not only deforms along with the SRG formation but ruptures in a regular and complex manner. The morphology of the cracks differs strongly depending on the electrical field distribution in the interference pattern, even when the magnitude and the kinetics of the strain are kept constant. This implies a complex local distribution of the opto-mechanical stress along the topography grating. In addition, the neutron reflectivity measurements of the metal/polymer interface indicate the penetration of a metal layer within the polymer, resulting in a formation of a bonding layer that confirms the transduction of light-induced stresses in the polymer layer to a metal film.
Magnetic reconnection is a fundamental process of topology change and energy release, taking place in plasmas on the Sun, in space, in astrophysical objects and in the laboratory. However, observational evidence has been relatively rare and typically only partial. Here we present evidence of fast reconnection in a solar filament eruption using high-resolution H-alpha images from the New Vacuum Solar Telescope, supplemented by extreme ultraviolet observations. The reconnection is seen to occur between a set of ambient chromospheric fibrils and the filament itself. This allows for the relaxation of magnetic tension in the filament by an untwisting motion, demonstrating a flux rope structure. The topology change and untwisting are also found through nonlinear force-free field modelling of the active region in combination with magnetohydrodynamic simulation. These results demonstrate a new role for reconnection in solar eruptions: the release of magnetic twist.
We study the requirement of the jet power in the conventional p-gamma models (photopion production and Bethe-Heitler pair production) for TeV BL Lac objects. We select a sample of TeV BL Lac objects whose spectral energy distributions are difficult to explain by the one-zone leptonic model. Based on the relation between the p-gamma interaction efficiency and the opacity of gamma gamma absorption, we find that the detection of TeV emission poses upper limits on the p-gamma interaction efficiencies in these sources and hence minimum jet powers can be derived accordingly. We find that the obtained minimum jet powers exceed the Eddington luminosity of the supermassive black holes (SMBHs). Implications for the accretion mode of the SMBHs in these BL Lac objects and the origin of their TeV emissions are discussed.
Heterogeneous diffusion processes (HDPs) with space-dependent diffusion coefficients D(x) are found in a number of real-world systems, such as for diffusion of macromolecules or submicron tracers in biological cells. Here, we examine HDPs in quenched-disorder systems with Gaussian colored noise (GCN) characterized by a diffusion coefficient with a power-law dependence on the particle position and with a spatially random scaling exponent. Typically, D(x) is considered to be centerd at the origin and the entire x axis is characterized by a single scaling exponent a. In this work we consider a spatially random scenario: in periodic intervals ("layers") in space D(x) is centerd to the midpoint of each interval. In each interval the scaling exponent alpha is randomly chosen from a Gaussian distribution. The effects of the variation of the scaling exponents, the periodicity of the domains ("layer thickness") of the diffusion coefficient in this stratified system, and the correlation time of the GCN are analyzed numerically in detail. We discuss the regimes of superdiffusion, subdiffusion, and normal diffusion realisable in this system. We observe and quantify the domains where nonergodic and non-Gaussian behaviors emerge in this system. Our results provide new insights into the understanding of weak ergodicity breaking for HDPs driven by colored noise, with potential applications in quenched layered systems, typical model systems for diffusion in biological cells and tissues, as well as for diffusion in geophysical systems.
We study the damping processes of both incompressible and compressible magnetohydrodynamic (MHD) turbulence in a partially ionized medium. We start from the linear analysis of MHD waves, applying both single-fluid and two-fluid treatments. The damping rates derived from the linear analysis are then used in determining the damping scales of MHD turbulence. The physical connection between the damping scale of MHD turbulence and the cutoff boundary of linear MHD waves is investigated. We find two branches of slow modes propagating in ions and neutrals, respectively, below the damping scale of slow MHD turbulence, and offer a thorough discussion of their propagation and dissipation behavior. Our analytical results are shown to be applicable in a variety of partially ionized interstellar medium (ISM) phases and the solar chromosphere. The importance of neutral viscosity in damping the Alfvenic turbulence in the interstellar warm neutral medium and the solar chromosphere is demonstrated. As a significant astrophysical utility, we introduce damping effects to the propagation of cosmic rays in partially ionized ISM. The important role of turbulence damping in both transit-time damping and gyroresonance is identified.
Levy walks (LWs) are spatiotemporally coupled random-walk processes describing superdiffusive heat conduction in solids, propagation of light in disordered optical materials, motion of molecular motors in living cells, or motion of animals, humans, robots, and viruses. We here investigate a key feature of LWs-their response to an external harmonic potential. In this generic setting for confined motion we demonstrate that LWs equilibrate exponentially and may assume a bimodal stationary distribution. We also show that the stationary distribution has a horizontal slope next to a reflecting boundary placed at the origin, in contrast to correlated superdiffusive processes. Our results generalize LWs to confining forces and settle some longstanding puzzles around LWs.
We introduce and study a Lévy walk (LW) model of particle spreading with a finite propagation speed combined with soft resets, stochastically occurring periods in which an harmonic external potential is switched on and forces the particle towards a specific position. Soft resets avoid instantaneous relocation of particles that in certain physical settings may be considered unphysical. Moreover, soft resets do not have a specific resetting point but lead the particle towards a resetting point by a restoring Hookean force. Depending on the exact choice for the LW waiting time density and the probability density of the periods when the harmonic potential is switched on, we demonstrate a rich emerging response behaviour including ballistic motion and superdiffusion. When the confinement periods of the soft-reset events are dominant, we observe a particle localisation with an associated non-equilibrium steady state. In this case the stationary particle probability density function turns out to acquire multimodal states. Our derivations are based on Markov chain ideas and LWs with multiple internal states, an approach that may be useful and flexible for the investigation of other generalised random walks with soft and hard resets. The spreading efficiency of soft-rest LWs is characterised by the first-passage time statistic.
Levy walks are continuous-time random-walk processes with a spatiotemporal coupling of jump lengths and waiting times. We here apply the Hermite polynomial method to study the behavior of LWs with power-law walking time density for four different cases. First we show that the known result for the infinite density of an unconfined, unbiased LW is consistently recovered. We then derive the asymptotic behavior of the probability density function (PDF) for LWs in a constant force field, and we obtain the corresponding qth-order moments. In a harmonic external potential we derive the relaxation dynamic of the LW. For the case of a Poissonian walking time an exponential relaxation behavior is shown to emerge. Conversely, a power-law decay is obtained when the mean walking time diverges. Finally, we consider the case of an unconfined, unbiased LW with decaying speed v(r ) = v0/./r. When the mean walking time is finite, a universal Gaussian law for the position-PDF of the walker is obtained explicitly.
To analyze stochastic processes, one often uses integral transform (Fourier and Laplace) methods. However, for the time-space coupled cases, e.g. the Levy walk, sometimes the integral transform method may fail. Here we provide a Hermite polynomial expansion approach, being complementary to the integral transform method, to the Levy walk. Two approaches are compared for some already known results. We also consider the generalized Levy walk with parameter dependent velocity. Namely, we consider the Levy walk with velocity which depends on the walking length or on the duration of each step. Some interesting features of the generalized Levy walk are observed, including the special shapes of the probability density function, the first passage time distributions, and various diffusive behaviors of the mean squared displacement.
Here, a new method for enhancing the photoelectrochemical properties of carbon nitride thin films by in situ supramolecular-driven preorganization of phenyl-contained monomers in molten sulfur is reported. A detailed analysis of the chemical and photophysical properties suggests that the molten sulfur can texture the growth and induce more effective integration of phenyl groups into the carbon nitride electrodes, resulting in extended light absorption alongside with improved conductivity and better charge transfer. Furthermore, photophysical measurements indicate the formation of sub-bands in the optical bandgap which is beneficial for exciton splitting. Moreover, the new bands can mediate hole transfer to the electrolyte, thus improving the photooxidation activity. The utilization of high temperature solvent as the polymerization medium opens new opportunities for the significant improvement of carbon nitride films toward an efficient photoactive material for various applications.
Herein, we report the use of upconversion agents to modify graphite carbon nitride (g-C3N4) by direct thermal condensation of a mixture of ErCl3 center dot 6H(2)O and the supramolecular precursor cyanuric acid-melamine. We show the enhancement of g-C3N4 photoactivity after Er3+ doping by monitoring the photodegradation of Rhodamine B dye under visible light. The contribution of the upconversion agent is demonstrated by measurements using only a red laser. The Er3+ doping alters both the electronic and the chemical properties of g-C3N4. The Er3+ doping reduces emission intensity and lifetime, indicating the formation of new, nonradiative deactivation pathways, probably involving charge-transfer processes.
Herein we report a general liquid-mediated pathway for the growth of continuous polymeric carbon nitride (C3N4) thin films. The deposition method consists of the use of supramolecular complexes that transform to the liquid state before direct thermal condensation into C3N4 solid films. The resulting films exhibit continuous porous C3N4 networks on various substrates. Moreover, the optical absorption can be easily tuned to cover the solar spectrum by the insertion of an additional molecule into the starting complex. The strength of the deposition method is demonstrated by the use of the C3N4 layer as the electron acceptor in a polymer solar cell that exhibits a remarkable open-circuit voltage exceeding 1 V. The easy, safe, and direct synthesis of carbon nitride in a continuous layered architecture on different functional substrates opens new possibilities for the fabrication of many energy-related devices.
The Role of Super-Atom Molecular Orbitals in Doped Fullerenes in a Femtosecond Intense Laser Field
(2017)
The interaction of gas phase endohedral fullerene Ho3N@C-80 with intense (0.1-5 x 10(14) W/cm(2)), short (30 fs), 800 nm laser pulses was investigated. The power law dependence of Ho3N@C-80(q+), q = 1-2, was found to be different from that of C-60. Time-dependent density functional theory computations revealed different light-induced ionization mechanisms. Unlike in C-60, in doped fullerenes, the breaking of the cage spherical symmetry makes super atomic molecular orbital (SAMO) states optically active. Theoretical calculations suggest that the fast ionization of the SAMO states in Ho3N@C-80 is responsible for the n = 3 power law for singly charged parent molecules at intensities lower than 1.2 x 10(14) W/cm(2).
Fragmentation of endohedral fullerene Ho3N@C-80 in an intense femtosecond near-infrared laser field
(2018)
The fragmentation of gas phase endohedral fullerene, Ho3N@C-80, was investigated using femtosecond near-infrared laser pulses with an ion velocity map imaging spectrometer. We observed that Ho+ abundance associated with carbon cage opening dominates at an intensity of 1.1 x 10(14) W/cm(2). As the intensity increases, the Ho+ yield associated with multifragmentation of the carbon cage exceeds the prominence of Ho+ associated with the gentler carbon cage opening. Moreover, the power law dependence of Ho+ on laser intensity indicates that the transition of the most likely fragmentation mechanisms occurs around 2.0 x 10(14) W/cm(2).
In this study we investigated conditions for loss of GPS signals observed by the Swarm satellites during a 2 year period, from December 2013 to November 2015. Our result shows that the Swarm satellites encountered most of the total loss of GPS signal at the ionization anomaly crests, between +/- 5 degrees and +/- 20 degrees magnetic latitude, forming two bands along the magnetic equator, and these low-latitude events mainly appear around postsunset hours from 19: 00 to 22: 00 local time. By further checking the in situ electron density measurements of Swarm, we found that practically, all the total loss of GPS signal events at low latitudes are related to equatorial plasma irregularities (EPIs) that show absolute density depletions larger than 10 x 10(11) m(-3); then, the Swarm satellites encountered for up to 95% loss of GPS signal for at least one channel and up to 45% tracked less than four GPS satellites (making precise orbit determination impossible). For those EPIs with density depletions less than 10 x 10(11) m(-3), the chance of tracked GPS signals less than four reduces to only 1.0%. Swarm also observed total loss of all GPS signal at high latitudes, mainly around local noon, and these events are related to large spatial density gradients due to polar patches or increased geomagnetic/auroral activities. We further found that the loss of GPS signals were less frequent after appropriate settings of the Swarm GPS receivers had been updated. However, the more recent period of the mission, e.g., after the GPS receiver settings have been updated, also coincides with less severe electron density depletions due to the declining solar cycle, making GPS loss events less likely. We conclude that both lower electron density gradients and appropriate GPS receiver settings reduce the probability for Swarm satellites loss of GPS signals.
We show that coadsorbed oxygen atoms have a dramatic influence on the CO desorption dynamics from Ru(0001). In contrast to the precursor-mediated desorption mechanism on Ru(0001), the presence of surface oxygen modifies the electronic structure of Ru atoms such that CO desorption occurs predominantly via the direct pathway. This phenomenon is directly observed in an ultrafast pump-probe experiment using a soft x-ray free-electron laser to monitor the dynamic evolution of the valence electronic structure of the surface species. This is supported with the potential of mean force along the CO desorption path obtained from density-functional theory calculations. Charge density distribution and frozen-orbital analysis suggest that the oxygen-induced reduction of the Pauli repulsion, and consequent increase of the dative interaction between the CO 5 sigma and the charged Ru atom, is the electronic origin of the distinct desorption dynamics. Ab initio molecular dynamics simulations of CO desorption from Ru(0001) and oxygen-coadsorbed Ru(0001) provide further insights into the surface bond-breaking process.
The pendant drop technique was used to determine p/A isotherms of docosanic acid spread on the drop surface of an aqueous polymer solution. Two water soluble polymers were used, poly(dimethyl-diallyl-ammoniumchloride) and sodium poly(styrene sulfonate-b-ethylethylene). By fast changes of the drop volume, the monolayers were compressed and dilated. The stress relaxation was monitored and surface rheological dilation parameters were obtained. It is shown that the fatty acid monolayer can be mechanically stabilized by both interacting anionic and cationic polymers. In the case of the anionic polymer, the interaction becomes more pronounced in the presence of salts in the subphase (counterions). Brewster angle microscopy shows that the typical tilt-orientation of crystalline domains of the fatty acid monolayers transforms into a more uniform and fluid-like structure caused by the polymer/monolayer interaction. The surface rheological behavior is dramatically influenced by the polymer binding. The interaction results in surface dilational viscoelastic properties and show that there is a strong resistance against expansion of the complex fatty acid/polymer layer.