Institut für Physik und Astronomie
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Institute
The problem of the existence of strange nonchaotic attractors (SNA's) in autonomous systems is discussed. It is demonstrated that the recently reported example of a SNA in an autonomous system [V. S. Anishchenko et al., Phys. Rev. E 54, 3231 (1996)] is in fact a chaotic attractor with positive largest Lyapunov exponent.
Photosynthetically active pigments are usually organized into pigment-protein complexes. These include light-harvesting antenna complexes (LHCs) and reaction centers. Site energies of the bound pigments are determined by interactions with their environment, i.e., by pigment-protein as well as pigment-pigment interactions. Thus, resolution of spectral substructures of the pigment-protein complexes may provide valuable insight into structure-function relationships.
By means of conventional (linear) and time-resolved spectroscopic techniques, however, it is often difficult to resolve the spectral substructures of complex pigment-protein assemblies. Nonlinear polarization spectroscopy in the frequency domain (NLPF) is shown to be a valuable technique in this regard. Based on initial experimental work with purple bacterial antenna complexes as well as model systems NLPF has been extended to analyse the substructure(s) of very complex spectra, including analyses of interactions between chlorophylls and "optically dark" states of carotenoids in LHCs. The paper reviews previous work and outlines perspectives regarding the application of NLPF spectroscopy to disentangle structure-function relationships in pigment-protein complexes.
Langmuir monolayer degradation (LMD) experiments with polymers possessing outstanding biomedical application potential yield information regarding the kinetics of their hydrolytic or enzymatic chain scission under well-defined and adjustable degradation conditions. A brief review is given of LMD investigations, including the author's own work on 2-dimensional (2D) polymer systems, providing chain scission data, which are not disturbed by simultaneously occurring transport phenomena, such as water penetration into the sample or transport of scission fragments out of the sample.
A knowledge-based approach for the description and simulation of polymer hydrolytic and enzymatic degradation based on a combination of fast LMD experiments and computer simulation of the water penetration is briefly introduced. Finally, the advantages and disadvantages of this approach are discussed.
Over the past decade, microfluidic techniques have been established as a versatile platform to perform live cell experiments under well-controlled conditions. To investigate the directional responses of cells, stable concentration profiles of chemotactic factors can be generated in microfluidic gradient mixers that provide a high degree of spatial control. However, the times for built-up and switching of gradient profiles are in general too slow to resolve the intracellular protein translocation events of directional sensing of eukaryotes. Here, we review an example of a conventional microfluidic gradient mixer as well as the novel flow photolysis technique that achieves an increased temporal resolution by combining the photo-activation of caged compounds with the advantages of microfluidic chambers.
We report the discovery of two new Galactic candidate luminous blue variable (LBV) stars via detection of circular shells (typical of confirmed and candidate LBVs) and follow-up spectroscopy of their central stars. The shells were detected at 22 mu m in the archival data of the Mid-Infrared All Sky Survey carried out with the Wide-field Infrared Survey Explorer (WISE). Follow-up optical spectroscopy of the central stars of the shells conducted with the renewed Southern African Large Telescope (SALT) showed that their spectra are very similar to those of the well-known LBVs P Cygni and AG Car, and the recently discovered candidate LBV MN112, which implies the LBV classification for these stars as well. The LBV classification of both stars is supported by detection of their significant photometric variability: one of them brightened in the R and I bands by 0.68 +/- 0.10 and 0.61 +/- 0.04 mag, respectively, during the last 1318 years, while the second one (known as Hen 3-1383) varies its B, V, R, I and Ks brightnesses by similar or equal to 0.50.9 mag on time-scales from 10 d to decades. We also found significant changes in the spectrum of Hen 3-1383 on a time-scale of similar or equal to 3 months, which provides additional support for the LBV classification of this star. Further spectrophotometric monitoring of both stars is required to firmly prove their LBV status. We discuss a connection between the location of massive stars in the field and their fast rotation, and suggest that the LBV activity of the newly discovered candidate LBVs might be directly related to their possible runaway status.
In this review we confront the current theoretical understanding of particle acceleration at relativistic outflows with recent observational results on various source classes thought to involve such outflows, e.g. gamma-ray bursts, active galactic nuclei, and pulsar wind nebulae. We highlight the possible contributions of these sources to ultra-high-energy cosmic rays.
Polyelectrolytes are macromolecules composed of charged monomers and exhibit unique properties due to the interplay of their flexibility and electrostatic interactions. In solution, they are attracted to oppositely charged surfaces and interfaces and exhibit a transition to an adsorbed state when certain conditions are met concerning the charge densities of the polymer and surface and the properties of the solution. In this review, we discuss two limiting cases for adsorption of flexible polyelectrolytes on curved surfaces: weak and strong adsorption. In the first case, adsorption is strongly influenced by the entropic degrees of freedom of a flexible polyelectrolyte. By contrast, in the strong adsorption limit, electrostatic interactions dominate, which leads to particular adsorption patterns, specifically on spherical surfaces. We discuss the corresponding theoretical approaches, applying a mean-field description for the polymer and the polymer-surface interaction. For weak adsorption, we discuss the critical adsorption behavior by exactly solvable models for planar and spherical geometries and a generic approximation scheme, which is additionally applied to cylindrical surfaces. For strong adsorption, we investigate various polyelectrolyte patterns on cylinders and spheres and evaluate their stability. The results are discussed in the light of experimental results, mostly of DNA adsorption experiments.
Probably no other field of statistical physics at the borderline of soft matter and biological physics has caused such a flurry of papers as polymer translocation since the 1994 landmark paper by Bezrukov, Vodyanoy, and Parsegian and the study of Kasianowicz in 1996. Experiments, simulations, and theoretical approaches are still contributing novel insights to date, while no universal consensus on the statistical understanding of polymer translocation has been reached. We here collect the published results, in particular, the famous-infamous debate on the scaling exponents governing the translocation process. We put these results into perspective and discuss where the field is going. In particular, we argue that the phenomenon of polymer translocation is non-universal and highly sensitive to the exact specifications of the models and experiments used towards its analysis.
When state-of-the-art bulk heterojunction organic solar cells with ideal morphology are exposed to prolonged storage or operation at elevated temperatures, a thermally induced disruption of the active layer blend can occur, in the form of a separation of donor and acceptor domains, leading to diminished photovoltaic performance. Toward the long-term use of organic solar cells in real-life conditions, an important challenge is, therefore, the development of devices with a thermally stable active layer morphology. Several routes are being explored, ranging from the use of high glass transition temperature, cross-linkable and/or side-chain functionalized donor and acceptor materials, to light-induced dimerization of the fullerene acceptor. A better fundamental understanding of the nature and underlying mechanisms of the phase separation and stabilization effects has been obtained through a variety of analytical, thermal analysis, and electro-optical techniques. Accelerated aging systems have been used to study the degradation kinetics of bulk heterojunction solar cells in situ at various temperatures to obtain aging models predicting solar cell lifetime. The following contribution gives an overview of the current insights regarding the intrinsic thermally induced aging effects and the proposed solutions, illustrated by examples of our own research groups. (C) The Authors. Published by SPIE under a Creative Commons Attribution 3.0 Unported License.
Each year we are bombarded with B.Sc. and Ph.D. applications from students that want to improve the world. They have learned that their future depends on changing the type of fuel we use and that solar energy is our future. The hope and energy of these young people will transform future energy technologies, but it will not happen quickly. Organic photovoltaic devices are easy to sketch, but the materials, processing steps, and ways of measuring the properties of the materials are very complicated. It is not trivial to make a systematic measurement that will change the way other research groups think or practice. In approaching this chapter, we thought about what a new researcher would need to know about organic photovoltaic devices and materials in order to have a good start in the subject. Then, we simplified that to focus on what a new researcher would need to know about poly-3-hexylthiophene: phenyl-C61-butyric acid methyl ester blends (P3HT: PCBM) to make research progress with these materials. This chapter is by no means authoritative or a compendium of all things on P3HT: PCBM. We have selected to explain how the sample fabrication techniques lead to control of morphology and structural features and how these morphological features have specific optical and electronic consequences for organic photovoltaic device applications.
The majority of the matter in the universe is still unidentified and under investigation by both direct and indirect means. Many experiments searching for the recoil of dark-matter particles off target nuclei in underground laboratories have established increasingly strong constraints on the mass and scattering cross sections of weakly interacting particles, and some have even seen hints at a possible signal. Other experiments search for a possible mixing of photons with light scalar or pseudo-scalar particles that could also constitute dark matter. Furthermore, annihilation or decay of dark matter can contribute to charged cosmic rays, photons at all energies, and neutrinos. Many existing and future ground-based and satellite experiments are sensitive to such signals. Finally, data from the Large Hadron Collider at CERN are scrutinized for missing energy as a signature of new weakly interacting particles that may be related to dark matter. In this review article we summarize the status of the field with an emphasis on the complementarity between direct detection in dedicated laboratory experiments, indirect detection in the cosmic radiation, and searches at particle accelerators. (C) 2015 Elsevier B.V. All rights reserved.
Supernova remnants (SNRs) are among the most important targets for gamma-ray observatories. Being prominent non-thermal sources, they are very likely responsible for the acceleration of the bulk of Galactic cosmic rays (CRS). To firmly establish the SNR paradigm for the origin of cosmic rays, it should be confirmed that protons are indeed accelerated in, and released from, SNRs with the appropriate flux and spectrum. This can be done by detailed theoretical models which account for microphysics of acceleration and various radiation processes of hadrons and leptons. The current generation of Cherenkov telescopes has insufficient sensitivity to constrain theoretical models. A new facility, the Cherenkov Telescope Array (CTA), will have superior capabilities and may finally resolve this long standing issue of high-energy astrophysics. We want to assess the capabilities of CTA to reveal the physics of various types of SNRs in the initial 2000 years of their evolution. During this time, the efficiency to accelerate cosmic rays is highest. We perform time-dependent simulations of the hydrodynamics, the magnetic fields, the cosmic-ray acceleration, and the non-thermal emission for type Ia, Ic and IIP SNRs. We calculate the CTA response to the y-ray emission from these SNRs for various ages and distances, and we perform a realistic analysis of the simulated data. We derive distance limits for the detectability and resolvability of these SNR types at several ages. We test the ability of CTA to reconstruct their morphological and spectral parameters as a function of their distance. Finally, we estimate how well CTA data will constrain the theoretical models. (C) 2014 Elsevier B.V. All rights reserved.
Monitoring Ultrafast Chemical Dynamics by Time-Domain X-ray Photo- and Auger-Electron Spectroscopy
(2016)
The directed flow of charge and energy is at the heart of all chemical processes. Extraordinary efforts are underway to monitor and understand the concerted motion of electrons and nuclei with ever increasing spatial and temporal sensitivity. The element specificity, chemical sensitivity, and temporal resolution of ultrafast X-ray spectroscopy techniques hold great promise to provide new insight into the fundamental interactions underlying chemical dynamics in systems ranging from isolated molecules to application-like devices. Here, we focus on the potential of ultrafast X-ray spectroscopy techniques based on the detection of photo- and Auger electrons to provide new fundamental insight into photochemical processes of systems with various degrees of complexity. Isolated nucleobases provide an excellent testing ground for our most fundamental understanding of intramolecular coupling between electrons and nuclei beyond the traditionally applied Born-Oppenheimer approximation. Ultrafast electronic relaxation dynamics enabled by the breakdown of this approximation is the major component of the nucleobase photoprotection mechanisms. Transient X-ray induced Auger electron spectroscopy on photoexcited thymine molecules provides atomic-site specific details of the extremely efficient coupling that converts potentially bond changing ultraviolet photon energy into benign heat. In particular, the time-dependent spectral shift of a specific Auger band is sensitive to the length of a single bond within the molecule. The X-ray induced Auger transients show evidence for an electronic transition out of the initially excited state within only similar to 200 fs in contrast to theoretically predicted picosecond population trapping behind a reaction barrier. Photoinduced charge transfer dynamics between transition metal complexes and semiconductor nanostructures are of central importance for many emerging energy and climate relevant technologies. Numerous demonstrations of photovoltaic and photocatalytic activity have been performed based on the combination of strong light absorption in dye molecules with charge separation and transport in adjacent semiconductor nanostructures. However, a fundamental understanding of the enabling and limiting dynamics on critical atomic length- and time scales is often still lacking. Femtosecond time-resolved X-ray photoelectron spectroscopy is employed to gain a better understanding of a short-lived intermediate that may be linked to the unexpectedly limited performance of ZnO based dye-sensitized solar cells by delaying the generation of free charge carriers. The transient spectra strongly suggest that photoexcited dye molecules attached to ZnO nanocrystals inject their charges into the substrate within less than 1 ps but the electrons are then temporarily trapped at the surface of the semiconductor in direct vicinity of the injecting molecules. The experiments are extended to monitor the electronic response of the semiconductor substrate to the collective injection from a monolayer of dye molecules and the subsequent electron-ion recombination dynamics. The results indicate some qualitative similarities but quantitative differences between the recombination dynamics at molecule-semiconductor interfaces and previously studied bulk-surface electron-hole recombination dynamics in photoexcited semiconductors.
The dynamics of constituents and the surface response of cellular membranes also in connection to the binding of various particles and macromolecules to the membrane are still a matter of controversy in the membrane biophysics community, particularly with respect to crowded membranes of living biological cells. We here put into perspective recent single particle tracking experiments in the plasma membranes of living cells and supercomputing studies of lipid bilayer model membranes with and without protein crowding. Special emphasis is put on the observation of anomalous, non-Brownian diffusion of both lipid molecules and proteins embedded in the lipid bilayer. While single component, pure lipid bilayers in simulations exhibit only transient anomalous diffusion of lipid molecules on nanosecond time scales, the persistence of anomalous diffusion becomes significantly longer ranged on the addition of disorder through the addition of cholesterol or proteins and on passing of the membrane lipids to the gel phase. Concurrently, experiments demonstrate the anomalous diffusion of membrane embedded proteins up to macroscopic time scales in the minute time range. Particular emphasis will be put on the physical character of the anomalous diffusion, in particular, the occurrence of ageing observed in the experiments the effective diffusivity of the measured particles is a decreasing function of time. Moreover, we present results for the time dependent local scaling exponent of the mean squared displacement of the monitored particles. Recent results finding deviations from the commonly assumed Gaussian diffusion patterns in protein crowded membranes are reported. The properties of the displacement autocorrelation function of the lipid molecules are discussed in the light of their appropriate physical anomalous diffusion models, both for non-crowded and crowded membranes. In the last part of this review we address the upcoming field of membrane distortion by elongated membrane-binding particles. We discuss how membrane compartmentalisation and the particle-membrane binding energy may impact the dynamics and response of lipid membranes. This article is part of a Special Issue entitled: Biosimulations edited by Ilpo Vattulainen and Tomasz Rog. (C) 2016 The Authors. Published by Elsevier B.V.
The main physical features and operating principles of isothermal nanomachines in the microworld, common to both classical and quantum machines, are reviewed. Special attention is paid to the dual, constructive role of dissipation and thermal fluctuations, the fluctuation-dissipation theorem, heat losses and free energy transduction, thermodynamic efficiency, and thermodynamic efficiency at maximum power. Several basic models are considered and discussed to highlight generic physical features. This work examines some common fallacies that continue to plague the literature. In particular, the erroneous beliefs that one should minimize friction and lower the temperature for high performance of Brownian machines, and that the thermodynamic efficiency at maximum power cannot exceed one-half are discussed. The emerging topic of anomalous molecular motors operating subdiffusively but very efficiently in the viscoelastic environment of living cells is also discussed.
We demonstrate in situ recorded motion of nano-objects adsorbed on a photosensitive polymer film. The motion is induced by a mass transport of the underlying photoresponsive polymer material occurring during irradiation with interference pattern. The polymer film contains azobenzene molecules that undergo reversible photoisomerization reaction from trans-to cis-conformation. Through a multi-scale chain of physico-chemical processes, this finally results in the macro-deformations of the film due to the changing elastic properties of polymer. The topographical deformation of the polymer surface is sensitive to a local distribution of the electrical field vector that allows for the generation of dynamic changes in the surface topography during irradiation with different light interference patterns. Polymer film deformation together with the motion of the adsorbed nano-particles are recorded using a homemade set-up combining an optical part for the generation of interference patterns and an atomic force microscope for acquiring the surface deformation. The particles undergo either translational or rotational motion. The direction of particle motion is towards the topography minima and opposite to the mass transport within the polymer film. The ability to relocate particles by photo-induced dynamic topography fluctuation offers a way for a non-contact simultaneous manipulation of a large number of adsorbed particles just in air at ambient conditions.
The biomolecule is among the most important building blocks of biological systems, and a full understanding of its function forms the scaffold for describing the mechanisms of higher order structures as organelles and cells. Force is a fundamental regulatory mechanism of biomolecular interactions driving many cellular processes. The forces on a molecular scale are exactly in the range that can be manipulated and probed with single molecule force spectroscopy. The natural environment of a biomolecule is inside a living cell, hence, this is the most relevant environment for probing their function. In vivo studies are, however, challenged by the complexity of the cell. In this review, we start with presenting relevant theoretical tools for analyzing single molecule data obtained in intracellular environments followed by a description of state-of-the art visualization techniques. The most commonly used force spectroscopy techniques, namely optical tweezers, magnetic tweezers, and atomic force microscopy, are described in detail, and their strength and limitations related to in vivo experiments are discussed. Finally, recent exciting discoveries within the field of in vivo manipulation and dynamics of single molecule and organelles are reviewed.