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We introduce azobenzene-functionalized polyelectrolyte multilayers as efficient, inexpensive optoacoustic transducers for hyper-sound strain waves in the GHz range. By picosecond transient reflectivity measurements we study the creation of nanoscale strain waves, their reflection from interfaces, damping by scattering from nanoparticles and propagation in soft and hard adjacent materials like polymer layers, quartz and mica. The amplitude of the generated strain ε ∼ 5 × 10−4 is calibrated by ultrafast X-ray diffraction.
We introduce azobenzene-functionalized polyelectrolyte multilayers as efficient, inexpensive optoacoustic transducers for hyper-sound strain waves in the GHz range. By picosecond transient reflectivity measurements we study the creation of nanoscale strain waves, their reflection from interfaces, damping by scattering from nanoparticles and propagation in soft and hard adjacent materials like polymer layers, quartz and mica. The amplitude of the generated strain epsilon similar to 5 x 10(-4) is calibrated by ultrafast X-ray diffraction.
On the basis of the layer-by-layer deposition of polyelectrolytes, we have designed hybrid nanolayer composites for integrated optoacoustic experiments. The femtosecond-laser-excitation of an Azo functionalized film launches nanoscale strain waves at GHz frequencies into a transparent polymer layer. Gold nanorods deposited on the surface sense the arrival of these hyper-sound-waves on the picosecond time scale via a modification of their longitudinal plasmon resonance. We simulated the strain waves using a simple linear masses-and-springs model, which yields good agreement with the observed time scales associated with the nanolayer thicknesses of the constituent materials. From systematic experiments with calibrated strain amplitudes we conclude that reversible viscoelastic deformations of the polyelectrolyte multilayers are triggered by ultrashort pressure transients of about 4 MPa. Our experiments show that strain-mediated interactions in nanoarchitectures composed of molecular photoswitches and plasmonic particles may be used to design new functionalities. The approach combines the highly flexible and cost-effective preparation of polyelectrolyte multilayers with ultrafast molecular strain actuation and plasmonic sensing. Although we use simple flat layered structures for demonstration, this new concept can be used for three-dimensional nanoassemblies with different functionalities. The ultrafast and reversible nature of the response is highly desirable, and the short wavelength associated with the high frequency of the hyper-sound-waves connecting photoactive molecules and nanoparticles inherently gives spectroscopic access to the nanoscale. High-frequency elastic moduli are derived from the ultrafast spectroscopy of the hypersonic response in polyelectrolyte multilayers.
The goal of the presented work is to explore the interaction between gold nanorods (GNRs) and hyper-sound waves. For the generation of the hyper-sound I have used Azobenzene-containing polymer transducers. Multilayer polymer structures with well-defined thicknesses and smooth interfaces were built via layer-by-layer deposition. Anionic polyelectrolytes with Azobenzene side groups (PAzo) were alternated with cationic polymer PAH, for the creation of transducer films. PSS/PAH multilayer were built for spacer layers, which do not absorb in the visible light range. The properties of the PAzo/PAH film as a transducer are carefully characterized by static and transient optical spectroscopy. The optical and mechanical properties of the transducer are studied on the picosecond time scale. In particular the relative change of the refractive index of the photo-excited and expanded PAH/PAzo is Δn/n = - 2.6*10‐4. Calibration of the generated strain is performed by ultrafast X-ray diffraction calibrated the strain in a Mica substrate, into which the hyper-sound is transduced. By simulating the X-ray data with a linear-chain-model the strain in the transducer under the excitation is derived to be Δd/d ~ 5*10‐4.
Additional to the investigation of the properties of the transducer itself, I have performed a series of experiments to study the penetration of the generated strain into various adjacent materials. By depositing the PAzo/PAH film onto a PAH/PSS structure with gold nanorods incorporated in it, I have shown that nanoscale impurities can be detected via the scattering of hyper-sound.
Prior to the investigation of complex structures containing GNRs and the transducer, I have performed several sets of experiments on GNRs deposited on a small buffer of PSS/PAH. The static and transient response of GNRs is investigated for different fluence of the pump beam and for different dielectric environments (GNRs covered by PSS/PAH).
A systematic analysis of sample architectures is performed in order to construct a sample with the desired effect of GNRs responding to the hyper-sound strain wave. The observed shift of a feature related to the longitudinal plasmon resonance in the transient reflection spectra is interpreted as the event of GNRs sensing the strain wave. We argue that the shift of the longitudinal plasmon resonance is caused by the viscoelastic deformation of the polymer around the nanoparticle. The deformation is induced by the out of plane difference in strain in the area directly under a particle and next to it. Simulations based on the linear chain model support this assumption. Experimentally this assumption is proven by investigating the same structure, with GNRs embedded in a PSS/PAH polymer layer.
The response of GNRs to the hyper-sound wave is also observed for the sample structure with GNRs embedded in PAzo/PAH films. The response of GNRs in this case is explained to be driven by the change of the refractive index of PAzo during the strain propagation.
Time-delayed collection field experiments are applied to planar organometal halide perovskite (CH3NH3PbI3) based solar cells to investigate charge carrier recombination in a fully working solar cell at the nanosecond to microsecond time scale. Recombination of mobile (extractable) charges is shown to follow second-order recombination dynamics for all fluences and time scales tested. Most importantly, the bimolecular recombination coefficient is found to be time-dependent, with an initial value of ca. 10(-9) cm(3)/s and a progressive reduction within the first tens of nanoseconds. Comparison to the prototypical organic bulk heterojunction device PTB7:PC71BM yields important differences with regard to the mechanism and time scale of free carrier recombination. (C) 2016 AIP Publishing LLC.
Many previous studies have shown that the turbulent mixing layer under periodic forcing tends to adopt a lock-on state, where the major portion of the fluctuations in the flow are synchronized at the forcing frequency. The goal of this experimental study is to apply closed-loop control in order to provoke the lock-on state, using information from the flow itself. We aim to determine the range of frequencies for which the closed-loop control can establish the lock-on, and what mechanisms are contributing to the selection of a feedback frequency. In order to expand the solution space for optimal closed-loop control laws, we use the genetic programming control (CPC) framework. The best closed-loop control laws obtained by CPC are analysed along with the associated physical mechanisms in the mixing layer flow. The resulting closed-loop control significantly outperforms open-loop forcing in terms of robustness to changes in the free-stream velocities. In addition, the selection of feedback frequencies is not locked to the most amplified local mode, but rather a range of frequencies around it.
A combined dynamics consisting of Brownian motion and Levy flights is exhibited by a variety of biological systems performing search processes. Assessing the search reliability of ever locating the target and the search efficiency of doing so economically of such dynamics thus poses an important problem. Here we model this dynamics by a one-dimensional fractional Fokker-Planck equation combining unbiased Brownian motion and Levy flights. By solving this equation both analytically and numerically we show that the superposition of recurrent Brownian motion and Levy flights with stable exponent alpha < 1, by itself implying zero probability of hitting a point on a line, leads to transient motion with finite probability of hitting any point on the line. We present results for the exact dependence of the values of both the search reliability and the search efficiency on the distance between the starting and target positions as well as the choice of the scaling exponent a of the Levy flight component.
We investigate the influence of the Coriolis force on mass motion related to the Rheasilvia impact on asteroid Vesta. Observations by the NASA Dawn mission revealed a pattern of curved radial ridges, which are related to Coriolis-deflected mass-wasting during the initial modification stage of the crater. Utilizing the projected curvature of the mass-wasting trajectories, we developed a method that enabled investigation of the initial mass wasting of the Rheasilvia impact by observational means. We demonstrate that the Coriolis force can strongly affect the crater formation processes on rapidly rotating objects, and we derive the material's velocities (28.9 ± 22.5 m/s), viscosities (1.5–9.0 × 106 Pa s) and coefficients of friction (0.02–0.81) during the impact modification stage. The duration of the impact modification stage could be estimated to (1.1 ± 0.5) h. By analyzing the velocity distribution with respect to the topography, we deduce that the Rheasilvia impactor hit a heterogeneous target and that the initial crater walls were significantly steeper during the modification stage.
Massive stars are extremely luminous and drive strong winds, blowing a large part of their matter into the galactic environment before they finally explode as a supernova. Quantitative knowledge of massive star feedback is required to understand our Universe as we see it. Traditionally, massive stars have been studied under the assumption that their winds are homogeneous and stationary, largely relying on the Sobolev approximation. However, Observations with the newest instruments, together with progress in model calculations, ultimately dictate a cardinal change of this paradigm: stellar winds are highly inhomogeneous. Hence, we are now advancing to a new stage in our understanding of stellar winds. Using the foundations laid by V.V. Sobolev and his school, we now update and further develop the stellar spectral analysis techniques. New sophisticated 3-D models of radiation transfer in inhomogeneous expanding media elucidate the physics of stellar winds and improve classical empiric mass-loss rate diagnostics. Applications of these new techniques to multiwavelength observations of massive stars yield consistent and robust stellar wind parameters. (C) 2016 Elsevier Ltd. All rights reserved.
Nearly all types of massive stars with radiatively driven stellar winds are X-ray sources that can be observed by the presently operating powerful X-ray telescopes. In this review I briefly address recent advances in our understanding of stellar winds obtained from X-ray observations. X-rays may strongly influence the dynamics of weak winds of main sequence B-type stars. X-ray pulsations were detected in a beta Cep type variable giving evidence of tight photosphere-wind connections. The winds of OB dwarfs with subtypes later than O9V may be predominantly in a hot phase, and X-ray observations offer the best window for their studies. The X-ray properties of OB super giants are largely determined by the effects of radiative transfer in their clumped stellar winds. The recently suggested method to directly measure mass-loss rates of O stars by fitting the shapes of X-ray emission lines is considered but its validity cannot be confirmed. To obtain robust quantitative information on stellar wind parameters from X-ray spectroscopy, a multiwavelength analysis by means of stellar atmosphere models is required. Independent groups are now performing such analyses with encouraging results. Joint analyses of optical, UV, and X-ray spectra of OB supergiants yield consistent mass-loss rates. Depending on the adopted clumping parameters, the empirically derived mass-loss rates are a factor of a few smaller or comparable to those predicted by standard recipes (Vink et al., 2001). All sufficiently studied O stars display variable X-ray emission that might be related to corotating interaction regions in their winds. In the latest stages of stellar evolution, single red supergiants (RSG) and luminous blue variable (LBV) stars do not emit observable amounts of X-rays. On the other hand, nearly all types of Wolf-Rayet (WR) stars are X-ray sources. X-ray spectroscopy allows a sensitive probe of WR wind abundances and opacities. (C) 2016 COSPAR. Published by Elsevier Ltd. All rights reserved.