TY - THES A1 - Hantschmann, Markus T1 - Stimulated resonant inelastic X-ray scattering in transition metal systems T1 - Resonante Inelastische Röntgenstreuung in Übergangsmetall-Komplexen N2 - With the implementation of intense, short pulsed light sources throughout the last years, the powerful technique of resonant inelastic X-ray scattering (RIXS) became feasible for a wide range of experiments within femtosecond dynamics in correlated materials and molecules. In this thesis I investigate the potential to bring RIXS into the fluence regime of nonlinear X-ray-matter interactions, especially focusing on the impact of stimulated scattering on RIXS in transition metal systems in a transmission spectroscopy geometry around transition metal L-edges. After presenting the RIXS toolbox and the capabilities of free electron laser light sources for ultrafast intense X-ray experiments, the thesis explores an experiment designed to understand the impact of stimulated scattering on diffraction and direct beam transmission spectroscopy on a CoPd multilayer system. The experiments require short X-ray pulses that can only be generated at free electron lasers (FEL). Here the pulses are not only short, but also very intense, which opens the door to nonlinear X-ray-matter interactions. In the second part of this thesis, we investigate observations in the nonlinear interaction regime, look at potential difficulties for classic spectroscopy and investigate possibilities to enhance the RIXS through stimulated scattering. Here, a study on stimulated RIXS is presented, where we investigate the light field intensity dependent CoPd demagnetization in transmission as well as scattering geometry. Thereby we show the first direct observation of stimulated RIXS as well as light field induced nonlinear effects, namely the breakdown of scattering intensity and the increase in sample transmittance. The topic is of ongoing interest and will just increase in relevance as more free electron lasers are planned and the number of experiments at such light sources will continue to increase in the near future. Finally we present a discussion on the accessibility of small DOS shifts in the absorption-band of transition metal complexes through stimulated resonant X-ray scattering. As these shifts occur for example in surface states this finding could expand the experimental selectivity of NEXAFS and RIXS to the detectability of surface states. We show how stimulation can indeed enhance the visibility of DOS shifts through the detection of stimulated spectral shifts and enhancements in this theoretical study. We also forecast the observation of stimulated enhancements in resonant excitation experiments at FEL sources in systems with a high density of states just below the Fermi edge and in systems with an occupied to unoccupied DOS ratio in the valence band above 1. N2 - In dieser Arbeit wird die Weiterentwicklung der Technik ’Resonante Inelastische Röntgenstreuung’ (RIXS) thematisiert. Vor allem wird das Thema der nichtlinearen Röntgen-Materie-Wechselwirkung an Freien Elektronenlasern wird ausführlich diskutiert. Mit der Etablierung von intensiven kurzpulsigen Röntgenquellen auf Basis von freien Elektronenlasern, ist die Möglichkeit entstanden, zeitaufgelöste Experimente im Femtosekundenbereich mit Röntgenstrahlung durchzuführen. Die dort erzeugten Pulse sind so intensiv und kurz, dass neue Effekte, die analogien in der nichtlinearen Optik haben, auftreten können. Diese neu auftretenden Effekte sind für die Röntgengemeinschaft vollkommen neu und müssen verstanden werden um freie Elektronenlaser sinnvoll auf größerer Skala, sinnvoll nutzen zu können. Außerdem könnten diese Effekte auch ganz neue experimentelle Möglichkeiten eröffnen. Deswegen beschäftigt sich diese Arbeit vor allem mit der potentiellen Möglichkeit, die RIXS Technik im nicht-linearen Licht-Materie Wechselwirkungsbereich zu bringen, die geänderten Interaktionen zu verstehen und vielleicht sogar nutzbar zu machen. Zu Beginn werden die Möglichkeiten der RIXS Technik vorgestellt. Im Anschluss wird ein von uns in Kollaboration mit dem SLAC entwickeltes und durchgeführtes Experiment vorgestellt, welches unter anderem die erste direkte Beobachtung von stimulierter resonanter inelastischer Röntgenbeugung an dünnen CoPd Multischichtsystemen ermöglicht hat. Außerdem sind intensitätsabhängige Veränderungen der Licht-Materie Wechselwirkung beobachtet worden. Speziell konnten wir einen klaren Zusammenhang zwischen dem Zusammenbruch von Streuintensität (entspricht etwa der Intensit¨ at, die nicht in direkter Strahlrichtung abgestrahlt wird) und der Vergrößerung der Transmittivität (Intensität, die in Strahlrichtung durch die Probe propagiert) feststellen. Dies konnte mit der Verschiebung von Auger und Streueffekten zu stimulierten Effekten verknüpft werden. Um das Experiment besser zu verstehen wurde ein Ratengleichungsmodell entwickelt, das intensitätsabhängige Wirkungsquerschnitte inkludiert und damit intensitätsabhängige Puls-induzierte Effekte abschätzen kann. Es konnte gezeigt werden wie die Intensitätsabhängikeit von Puls-Induzierter Transparenz, Puls-induziertem zusammenbruch der Röntgenstreuung, und die Verstärkung von Teilen des Pulses mit stimulierten Emissionen verknüpft sind. Außerdem konnten einige Aspekte identifiziert werden, die dabei helfen können um neue Experimente zu designen, die in der Lage wären durch das Ausnutzen von stimulierter Emission und damit verbundenen Spektralen verschiebungen zusätzliche Informationen aus den zu untersuchenden Systemen zu gewinnen, wie zum Beispiel über die elektronische Zustandsdichte in einer Oberflächen- oder Interface-Schicht. KW - RIXS KW - free electron laser KW - transition metal systems KW - rate equation KW - RIXS KW - resonante inelastische Röntgenstreuung KW - Freie Elektronen Laser KW - Übergangsmetall - Komplexe Y1 - 2023 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-584761 ER - TY - JOUR A1 - Henkel, Carsten A1 - Jacob, Georg A1 - Stopp, Felix A1 - Schmidt-Kaler, Ferdinand A1 - Keil, Mark A1 - Japha, Yonathan A1 - Folman, Ron T1 - Stern-Gerlach splitting of low-energy ion beams JF - New journal of physics : the open-access journal for physics N2 - We present a feasibility study with several magnetic field configurations for creating spin-dependent forces that can split a low-energy ion beam by the Stern-Gerlach (SG) effect. To the best of our knowledge, coherent spin-splittings of charged particles have yet to be realised. Our proposal is based on ion source parameters taken from a recent experiment that demonstrated single-ion implantation from a high-brightness ion source combined with a radio-frequency Paul trap. The inhomogeneous magnetic fields can be created by permanently magnetised microstructures or from current-carrying wires with sizes in the micron range, such as those recently used in a successful implementation of the SG effect with neutral atoms. All relevant forces (Lorentz force and image charges) are taken into account, and measurable splittings are found by analytical and numerical calculations. KW - spin-dependent forces KW - Stern-Gerlach effect KW - ion optics KW - beam splitter KW - magnetic microstructures Y1 - 2019 U6 - https://doi.org/10.1088/1367-2630/ab36c7 SN - 1367-2630 VL - 21 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Regenstein, Wolfgang T1 - Statistische Beschreibung des Resonanzenergietransfers in Lösungen N2 - In resonance energy transfer, photons are transferred from an excited donor to an acceptor over an interaction distance. According to Förster's quantum mechanical theory, this distance can be calculated using the overlap integral of the fluorescence spectrum of the donor and the absorption spectrum of the acceptor. Another possibility of determination is obtained with the help of statistical models, which are compiled in an overview. The distance can be determined by evaluating the extinction curve. In this work, a further statistical variant of the determination of the interaction radius is added and demonstrated in detail using an example. N2 - Beim Resonanzenergietransfer werden Fotonen von einem angeregten Donator über einen Wechselwirkungsabstand auf einen Akzeptor übertragen. Nach der quantenmechanischen Theorie von FÖRSTER kann dieser Abstand mit Hilfe des Überlappungsintegrals von Fluoreszenzspektrum des Donators und Absorp-tionsspektrum des Akzeptors berechnet werden. Eine andere Möglichkeit der Bestimmung erhält man mit Hilfe von statistischen Modellen, die in einem Überblick zusammengestellt sind. Dabei kann der Abstand durch Auswertung der Löschkurve bestimmt werden. In dieser Arbeit wird dazu eine weitere statistische Variante der Bestimmung des Wechselwirkungsradius hinzugefügt und an einem Beispiel ausführlich demonstriert. KW - resonant energy transfer KW - statistical models KW - theory of Förster KW - quenching curve KW - interaction distance KW - Resonanzenergietransfer KW - statistische Modelle KW - Theorie von Förster KW - Löschkurve KW - Wechselwirkungsabstand Y1 - 2022 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-565009 ER - TY - JOUR A1 - Regenstein, Wolfgang T1 - Statistische Beschreibung des Resonanzenergietransfers in Lösungen N2 - Beim Resonanzenergietransfer werden Fotonen von einem angeregten Donator über einen Wechselwirkungsabstand auf einen Akzeptor übertragen. Nach der quantenmechanischen Theorie von FÖRSTER kann dieser Abstand mit Hilfe des Überlappungsintegrals von Fluoreszenzspektrum des Donators und Absorp-tionsspektrum des Akzeptors berechnet werden. Eine andere Möglichkeit der Bestimmung erhält man mit Hilfe von statistischen Modellen, die in einem Überblick zusammengestellt sind. Dabei kann der Abstand durch Auswertung der Löschkurve bestimmt werden. In dieser Arbeit wird dazu eine weitere statistische Variante der Bestimmung des Wechselwirkungsradius hinzugefügt und an einem Beispiel ausführlich demonstriert. N2 - In resonance energy transfer, photons are transferred from an excited donor to an acceptor over an interaction distance. According to Förster's quantum mechanical theory, this distance can be calculated using the overlap integral of the fluorescence spectrum of the donor and the absorption spectrum of the acceptor. Another possibility of determination is obtained with the help of statistical models, which are compiled in an overview. The distance can be determined by evaluating the extinction curve. In this work, a further statistical variant of the determination of the interaction radius is added and demonstrated in detail using an example. KW - resonant energy transfer KW - statistical models KW - theory of Förster KW - quenching curve KW - interaction distance KW - Resonanzenergietransfer KW - statistische Modelle KW - Theorie von Förster KW - Löschkurve KW - Wechselwirkungsabstand Y1 - 2022 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-565977 ET - 2. Version ER - TY - JOUR A1 - Gorobtsov, O. Yu. A1 - Mercurio, G. A1 - Brenner, G. A1 - Lorenz, Ulf A1 - Gerasimova, N. A1 - Kurta, R. P. A1 - Hieke, F. A1 - Skopintsev, P. A1 - Zaluzhnyy, I. A1 - Lazarev, S. A1 - Dzhigaev, D. A1 - Rose, M. A1 - Singer, A. A1 - Wurth, W. A1 - Vartanyants, I. A. T1 - Statistical properties of a free-electron laser revealed by Hanbury Brown-Twiss interferometry JF - Physical review : A, Atomic, molecular, and optical physics N2 - We present a comprehensive experimental analysis of statistical properties of the self-amplified spontaneous emission free-electron laser (FEL) FLASH by means of Hanbury Brown and Twiss interferometry. The experiments were performed at FEL wavelengths of 5.5, 13.4, and 20.8 nm. We determined the second-order intensity correlation function for all wavelengths and different operation conditions of FLASH. In all experiments a high degree of spatial coherence (above 50%) was obtained. Our analysis performed in spatial and spectral domains provided us with the independent measurements of an average pulse duration of the FEL that were below 60 fs. To explain the complicated behavior of the second-order intensity correlation function we developed an advanced theoretical model that includes the presence of multiple beams and external positional jitter of the FEL pulses. By this analysis we determined that in one of the experiments external positional jitter was about 25% of the beam size. We envision that methods developed in our study will be used widely for analysis and diagnostics of FEL radiation. Y1 - 2017 U6 - https://doi.org/10.1103/PhysRevA.95.023843 SN - 2469-9926 SN - 2469-9934 VL - 95 IS - 2 PB - American Physical Society CY - College Park ER - TY - THES A1 - Zillmer, Rüdiger T1 - Statistical properties and scaling of the Lyapunov exponents in stochastic systems N2 - Die vorliegende Arbeit umfaßt drei Abhandlungen, welche allgemein mit einer stochastischen Theorie für die Lyapunov-Exponenten befaßt sind. Mit Hilfe dieser Theorie werden universelle Skalengesetze untersucht, die in gekoppelten chaotischen und ungeordneten Systemen auftreten. Zunächst werden zwei zeitkontinuierliche stochastische Modelle für schwach gekoppelte chaotische Systeme eingeführt, um die Skalierung der Lyapunov-Exponenten mit der Kopplungsstärke ('coupling sensitivity of chaos') zu untersuchen. Mit Hilfe des Fokker-Planck-Formalismus werden Skalengesetze hergeleitet, die von Ergebnissen numerischer Simulationen bestätigt werden. Anschließend wird gezeigt, daß 'coupling sensitivity' im Fall gekoppelter ungeordneter Ketten auftritt, wobei der Effekt sich durch ein singuläres Anwachsen der Lokalisierungslänge äußert. Numerische Ergebnisse für gekoppelte Anderson-Modelle werden bekräftigt durch analytische Resultate für gekoppelte raumkontinuierliche Schrödinger-Gleichungen. Das resultierende Skalengesetz für die Lokalisierungslänge ähnelt der Skalierung der Lyapunov-Exponenten gekoppelter chaotischer Systeme. Schließlich wird die Statistik der exponentiellen Wachstumsrate des linearen Oszillators mit parametrischem Rauschen studiert. Es wird gezeigt, daß die Verteilung des zeitabhängigen Lyapunov-Exponenten von der Normalverteilung abweicht. Mittels der verallgemeinerten Lyapunov-Exponenten wird der Parameterbereich bestimmt, in welchem die Abweichungen von der Normalverteilung signifikant sind und Multiskalierung wesentlich wird. N2 - This work incorporates three treatises which are commonly concerned with a stochastic theory of the Lyapunov exponents. With the help of this theory universal scaling laws are investigated which appear in coupled chaotic and disordered systems. First, two continuous-time stochastic models for weakly coupled chaotic systems are introduced to study the scaling of the Lyapunov exponents with the coupling strength (coupling sensitivity of chaos). By means of the the Fokker-Planck formalism scaling relations are derived, which are confirmed by results of numerical simulations. Next, coupling sensitivity is shown to exist for coupled disordered chains, where it appears as a singular increase of the localization length. Numerical findings for coupled Anderson models are confirmed by analytic results for coupled continuous-space Schrödinger equations. The resulting scaling relation of the localization length resembles the scaling of the Lyapunov exponent of coupled chaotic systems. Finally, the statistics of the exponential growth rate of the linear oscillator with parametric noise are studied. It is shown that the distribution of the finite-time Lyapunov exponent deviates from a Gaussian one. By means of the generalized Lyapunov exponents the parameter range is determined where the non-Gaussian part of the distribution is significant and multiscaling becomes essential. KW - Lyapunov-Exponenten KW - Chaos KW - ungeordnete Systeme KW - Lokalisierung KW - stochastische Systeme KW - 'coupling sensitivity' KW - parametrisch erregter Oszillator KW - Lyapunov exponents KW - chaos KW - disordered systems KW - localization KW - stochastic systems KW - coupling sensitivity KW - parametrically excited oscillator Y1 - 2003 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-0001147 ER - TY - JOUR A1 - Seyrich, Maximilian A1 - Alirezaeizanjani, Zahra A1 - Beta, Carsten A1 - Stark, Holger T1 - Statistical parameter inference of bacterial swimming strategies JF - New journal of physics : the open-access journal for physics N2 - We provide a detailed stochastic description of the swimming motion of an E. coli bacterium in two dimension, where we resolve tumble events in time. For this purpose, we set up two Langevin equations for the orientation angle and speed dynamics. Calculating moments, distribution and autocorrelation functions from both Langevin equations and matching them to the same quantities determined from data recorded in experiments, we infer the swimming parameters of E. coli. They are the tumble rate lambda, the tumble time r(-1), the swimming speed v(0), the strength of speed fluctuations sigma, the relative height of speed jumps eta, the thermal value for the rotational diffusion coefficient D-0, and the enhanced rotational diffusivity during tumbling D-T. Conditioning the observables on the swimming direction relative to the gradient of a chemoattractant, we infer the chemotaxis strategies of E. coli. We confirm the classical strategy of a lower tumble rate for swimming up the gradient but also a smaller mean tumble angle (angle bias). The latter is realized by shorter tumbles as well as a slower diffusive reorientation. We also find that speed fluctuations are increased by about 30% when swimming up the gradient compared to the reversed direction. KW - E.coli KW - run and tumble KW - chemotaxis KW - stochastic processes KW - bacterial swimming strategies KW - parameter inference Y1 - 2018 U6 - https://doi.org/10.1088/1367-2630/aae72c SN - 1367-2630 VL - 20 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Kim, Kyung-Chan A1 - Shprits, Yuri T1 - Statistical Analysis of Hiss Waves in Plasmaspheric Plumes Using Van Allen Probe Observations JF - Journal of geophysical research : Space physics N2 - Plasmaspheric hiss waves commonly observed in high‐density regions in the Earth's magnetosphere are known to be one of the main contributors to the loss of radiation belt electrons. There has been a lot of effort to investigate the distributions of hiss waves in the plasmasphere, while relatively little attention has been given to those in the plasmaspheric plume. In this study, we present for the first time a statistical analysis of the occurrence and the spatial distribution of wave amplitudes and wave normal angles for hiss waves in plumes using Van Allen Probes observations during the period of October 2012 to December 2016. Statistical results show that a wide range of hiss wave amplitudes in plumes from a few picotesla to >100 pT is observed, but a modest (<20 pT) wave amplitude is more commonly observed regardless of geomagnetic activity in both the midnight‐to‐dawn and dusk sector. By contrast, stronger amplitude hiss occurs preferentially during geomagnetically active times in the dusk sector. The wave normal angles are distributed over a broad range from 0° to 90° with a bimodal distribution: a quasi‐field‐aligned population (<20°) with an occurrence rate of <60% and an oblique one (>50°) with a relative low occurrence rate of ≲20%. Therefore, from a statistical point of view, we confirm that the hiss intensity (a few tens of picotesla) and field‐aligned hiss wave adopted in previous simulation studies are a reasonable assumption but stress that the activity dependence of the wave amplitude should be considered. KW - plasmaspheric hiss KW - plasmaspheric plume KW - Van Allen Probes Y1 - 2019 U6 - https://doi.org/10.1029/2018JA026458 SN - 2169-9380 SN - 2169-9402 VL - 124 IS - 3 SP - 1904 EP - 1915 PB - American Geophysical Union CY - Washington ER - TY - JOUR A1 - Zeiske, Stefan A1 - Sandberg, Oskar J. A1 - Zarrabi, Nasim A1 - Wolff, Christian Michael A1 - Raoufi, Meysam A1 - Peña-Camargo, Francisco A1 - Gutierrez-Partida, Emilio A1 - Meredith, Paul A1 - Stolterfoht, Martin A1 - Armin, Ardalan T1 - Static disorder in lead halide perovskites JF - The journal of physical chemistry letters N2 - In crystalline and amorphous semiconductors, the temperature-dependent Urbach energy can be determined from the inverse slope of the logarithm of the absorption spectrum and reflects the static and dynamic energetic disorder. Using recent advances in the sensitivity of photocurrent spectroscopy methods, we elucidate the temperature-dependent Urbach energy in lead halide perovskites containing different numbers of cation components. We find Urbach energies at room temperature to be 13.0 +/- 1.0, 13.2 +/- 1.0, and 13.5 +/- 1.0 meV for single, double, and triple cation perovskite. Static, temperature-independent contributions to the Urbach energy are found to be as low as 5.1 ?+/- 0.5, 4.7 +/- 0.3, and 3.3 +/- 0.9 meV for the same systems. Our results suggest that, at a low temperature, the dominant static disorder in perovskites is derived from zero-point phonon energy rather than structural disorder. This is unusual for solution-processed semiconductors but broadens the potential application of perovskites further to quantum electronics and devices. KW - Cations KW - External quantum efficiency KW - Perovskites KW - Solar cells KW - Solar energy Y1 - 2022 U6 - https://doi.org/10.1021/acs.jpclett.2c01652 SN - 1948-7185 VL - 13 IS - 31 SP - 7280 EP - 7285 PB - American Chemical Society CY - Washington ER - TY - THES A1 - Kiel, Mareike T1 - Static and ultrafast optical properties of nanolayered composites : gold nanoparticles embedded in polyelectrolytes T1 - Statische und ultraschnelle optische Eigenschaften von nanogeschichteten Kompositmaterialien. Gold-Nanopartikel in Polyelektrolytschichten. N2 - In the course of this thesis gold nanoparticle/polyelectrolyte multilayer structures were prepared, characterized, and investigated according to their static and ultrafast optical properties. Using the dip-coating or spin-coating layer-by-layer deposition method, gold-nanoparticle layers were embedded in a polyelectrolyte environment with high structural perfection. Typical structures exhibit four repetition units, each consisting of one gold-particle layer and ten double layers of polyelectrolyte (cationic+anionic polyelectrolyte). The structures were characterized by X-ray reflectivity measurements, which reveal Bragg peaks up to the seventh order, evidencing the high stratication of the particle layers. In the same measurements pronounced Kiessig fringes were observed, which indicate a low global roughness of the samples. Atomic force microscopy (AFM) images veried this low roughness, which results from the high smoothing capabilities of polyelectrolyte layers. This smoothing effect facilitates the fabrication of stratified nanoparticle/polyelectrolyte multilayer structures, which were nicely illustrated in a transmission electron microscopy image. The samples' optical properties were investigated by static spectroscopic measurements in the visible and UV range. The measurements revealed a frequency shift of the reflectance and of the plasmon absorption band, depending on the thickness of the polyelectrolyte layers that cover a nanoparticle layer. When the covering layer becomes thicker than the particle interaction range, the absorption spectrum becomes independent of the polymer thickness. However, the reflectance spectrum continues shifting to lower frequencies (even for large thicknesses). The range of plasmon interaction was determined to be in the order of the particle diameter for 10 nm, 20 nm, and 150 nm particles. The transient broadband complex dielectric function of a multilayer structure was determined experimentally by ultrafast pump-probe spectroscopy. This was achieved by simultaneous measurements of the changes in the reflectance and transmittance of the excited sample over a broad spectral range. The changes in the real and imaginary parts of the dielectric function were directly deduced from the measured data by using a recursive formalism based on the Fresnel equations. This method can be applied to a broad range of nanoparticle systems where experimental data on the transient dielectric response are rare. This complete experimental approach serves as a test ground for modeling the dielectric function of a nanoparticle compound structure upon laser excitation. N2 - Im Rahmen dieser Arbeit wurden Gold-Nanopartikel/Polyelektrolyt Multischichtstrukturen hergestellt, strukturell charakterisiert und bezüglich ihrer optischen Eigenschaften sowohl statisch als auch zeitaufgelöst analysiert. Die Strukturen wurden mithilfe der Dip-coating oder der Spin-coating Methode hergestellt. Beide Methoden ermöglichen das Einbetten einzelner Partikellagen in eine Polyelektrolytumgebung. Typische Strukturen in dieser Arbeit bestehen aus vier Wiederholeinheiten, wobei jede aus einer Nanopartikelschicht und zehn Polyelektrolyt-Doppellagen (kationisches und anionisches Polyelektrolyt) zusammengesetzt ist. Die Stratizierung der Gold-Nanopartikellagen wurde mittels Röntgenreflektometrie-Messungen im Kleinwinkelbereich nachgewiesen, welche Bragg Reflexionen bis zur siebten Ordnung aufzeigen. Das ausgeprägte Kiessig Interferenzmuster dieser Messungen weist zudem auf eine geringe globale Rauheit hin, die durch Oberflächenanalysen mit einem Rasterkraftmikroskop bestätigt werden konnte. Diese geringe Rauheit resultiert aus den glättenden Eigenschaften der Polyelektrolyte, die die Herstellung von Multilagensystemen mit mehreren Partikellagen erst ermöglichen. Die Aufnahme eines Transmissionselektronenmikroskops veranschaulicht eindrucksvoll die Anordnung der Partikel in einzelne Schichten. Durch photospektroskopische Messungen wurden die optischen Eigenschaften der Strukturen im UV- und sichtbaren Bereich untersucht. Beispielsweise wird eine Verschiebung und Verstärkung der Plasmonenresonanz beobachtet, wenn eine Goldnanopartikellage mit transparenten Polyelektrolyten beschichtet wird. Erst wenn die bedeckende Schicht dicker als die Reichweite der Plasmonen wird, bleibt die Absorption konstant. Die spektrale Reflektivität jedoch ändert sich auch mit jeder weiteren adsorbierten Polyelektrolytschicht. Die Reichweite der Plasmonenresonanz konnte auf diese Art für Partikel der Größe 10 nm, 20 nm und 150 nm bestimmt werden. Die Ergebnisse wurden im Kontext einer Effektiven Mediums Theorie diskutiert. Die komplexe dielektrische Funktion einer Multilagenstruktur wurde zeitabhängig nach Laserpulsanregung für einen breiten spektralen Bereich bestimmt. Dazu wurden zuerst die Änderungen der Reflektivität und Transmittivität simultan mittels der Pump-Probe (Anrege-Abtast) Spektroskopie gemessen. Anschließend wurden aus diesen Daten, mithilfe eines Formalismus, der auf den Fresnelschen Formeln basiert, die Änderungen im Real- und Imaginärteil der dielektrischen Funktion ermittelt. Diese Methode eignet sich zur Bestimmung der transienten dielektrischen Funktion einer Vielzahl von Nanopartikelsystemen. Der rein experimentelle Ansatz ermöglicht es, effektive Medien Theorien und Simulationen der dielektrischen Funktion nach Laserpulsanregung zu überprüfen. KW - Nanopartikel KW - Polyelektrolyte KW - Dielektrische Funktion KW - Anrege-Abtast Spektroskopie KW - nanoparticles KW - polyelectrolytes KW - dielectric function KW - pump-probe spectroscopy Y1 - 2012 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus-61823 ER - TY - THES A1 - Kölsch, Patrick T1 - Static and dynamic properties of soluble surfactants at the air/water interface T1 - Statische und dynamische Eigenschaften von löslichen Amphiphilen an der Wasser/Luft Grenzfläche N2 - Amphiphilic molecules contain a hydrophilic headgroup and a hydrophobic tail. The headgroup is polar or ionic and likes water, the tail is typically an aliphatic chain that cannot be accommodated in a polar environment. The prevailing molecular asymmetry leads to a spontaneous adsorption of amphiphiles at the air/water or oil/water interfaces. As a result, the surface tension and the surface rheology is changed. Amphiphiles are important tools to deliberately modify the interfacial properties of liquid interfaces and enable new phenomena such as foams which cannot be formed in a pure liquid. In this thesis we investigate the static and dynamic properties of adsorption layers of soluble amphiphiles at the air/water interface, the so called Gibbs monolayers. The classical way for an investigation of these systems is based on a thermodynamic analysis of the equilibrium surface tension as a function of the bulk composition in the framework of Gibbs theory. However, thermodynamics does not provide any structural information and several recent publications challenge even fundamental text book concepts. The experimental investigation faces difficulties imposed by the low surface coverage and the presence of dissolved amphiphiles in the adjacent bulk phase. In this thesis we used a suite of techniques with the sensitivity to detect less than a monolayer of molecules at the air-water interface. Some of these techniques are extremely complex such as infrared visible sum frequency generation (IR-VIS SFG) spectroscopy or second harmonic generation (SHG). Others are traditional techniques, such as ellipsometry employed in new ways and pushed to new limits. Each technique probes selectively different parts of the interface and the combination provides a profound picture of the interfacial architecture. The first part of the thesis is dedicated to the distribution of ions at interfaces. Adsorption layers of ionic amphiphiles serve as model systems allowing to produce a defined surface charge. The charge of the monolayer is compensated by the counterions. As a result of a complex zoo of interactions there will be a defined distribution of ions at the interface, however, its experimental determination is a big scientific challenge. We could demonstrate that a combination of linear and nonlinear techniques gives direct insights in the prevailing ion distribution. Our investigations reveal specific ion effects which cannot be described by classical Poisson-Boltzmann mean field type theories. Adsorption layer and bulk phase are in thermodynamic equilibrium, however, it is important to stress that there is a constant molecular exchange between adsorbed and dissolved species. This exchange process is a key element for the understanding of some of the thermodynamic properties. An excellent way to study Gibbs monolayers is to follow the relaxation from a non-equilibrium to an equilibrium state. Upon compression amphiphiles must leave the adsorption layer and dissolve in the adjacent bulk phase. Upon expansion amphiphiles must adsorb at the interface to restore the equilibrium coverage. Obviously the frequency of the expansion and compression cycles must match the molecular exchange processes. At too low frequencies the equilibrium is maintained at all times. If the frequency is too fast the system behaves as a monolayer of insoluble surfactants. In this thesis we describe an unique variant of an oscillating bubble technique that measures precisely the real and imaginary part of the complex dilational modulus E in a frequency range up to 500 Hz. The extension of about two decades in the time domain in comparison to the conventional method of an oscillating drop is a tremendous achievement. The imaginary part of the complex dilational modulus E is a consequence of a dissipative process which is interpreted as an intrinsic surface dilational viscosity. The IR-VIS SFG spectra of the interfacial water provide a molecular interpretation of the underlying dissipative process. N2 - Amphiphile Moleküle vereinen zwei gegensätzliche Strukturelemente. Sie bestehen aus einer polaren oder ionischen Kopfgruppe und einem unpolaren Molekülteil, häufig einer Kohlenwasserstoffkette. Die vorliegende molekulare Asymmetrie bewirkt eine spontane Adsorption der Amphiphile an der Wasser/Luft Grenzschicht. Als Folge verändern sich Oberflächenspannung und Grenzflächenrheologie. Amphiphile Moleküle werden benutzt, um die Eigenschaften flüssiger Grenzflächen zu verändern und begegnen uns z.B. in Form von Seifen oder anderen waschaktiven Substanzen im täglichen Leben. Der erste Teil dieser Doktorarbeit widmet sich der Verteilung von Ionen an geladenen flüssigen Grenzflächen. Adsorbtionsschichten ionischer Amphiphile bieten Modellsysteme zur Untersuchung dieses klassischen Bereiches der Kolloid- und Grenzflächenforschung. Durch die Adsorption der Amphiphile in der Grenzschicht werden definierte Oberflächenladungen erzeugt, welche durch die angrenzenden Gegenionen in der Sublage kompensiert werden. In dieser Arbeit wird gezeigt, dass eine Kombination aus linearen und komplexen nichtlinearen optischen Methoden, die experimentelle Bestimmung der Verteilung der Gegenionen an geladenen Grenzflächen ermöglicht. Unsere Messungen zeigen ionenspezifische Effekte, die sich nicht in Reihenfolge des Periodensystems ordnen lassen. Insbesondere wurde ein Phasenübergang in der Verteilung der Gegenionen von einem Zustand, in dem sich die Ionen in der Sublage befinden, zu einem Zustand bestehend aus direkt kondensierten Ionen beobachtet. Dieser Phasenübergang geschieht innerhalb einer geringen Erhöhung der Oberflächenladung und lässt sich nicht mit klassischen Theorien beschreiben. Der zweite Teil dieser Arbeit widmet sich der Stabilität von Schaumlamellen. Eine Schaumlamelle ist ein dünner Wasserfilm, der durch die Adsorption von oberflächenaktiven Molekülen an beiden Seiten stabilisiert wird. In Zusammenhang von Schäumen muss zwischen zwei Prozessen unterschieden werden: Der Schaumbildung und der Schaumstabilität. Die zugrundeliegenden Mechanismen der Schaumbildung sind weitestgehend verstanden, die der Schaumstabilität jedoch noch nicht. Um die Stabilität von Schäumen zu untersuchen, müssen Nichtgleichgewichtszustände erzeugt und die anschließende Relaxation in das Gleichgewicht beobachtet werden. In dieser Arbeit wurde ein neues Verfahren entwickelt, welches es ermöglicht, das Elastizitätsmodul von Grenzflächen in einem Frequenzbereich von 1-500 Hz zu bestimmen. Dies bedeutet eine Erweiterung um zwei Dekaden gegenüber herkömmlichen Methoden. Die Idee ist denkbar einfach: In einer mit Flüssigkeit gefüllten Kammer wird über die Bewegung eines Piezos eine Luftblase in Schwingung versetzt und mit einem in der Kammer befindlichen Drucksensor die Schwingungsantwort der Blase aufgezeichnet. Unsere Untersuchungen zeigen, dass die Voraussetzung für die Ausbildung einer stabilen Schaumlamelle das Vorkommen einer intrinsischen Oberflächenviskosität ist. Eine anschauliche Erklärung verdeutlicht dies: Eine viskose Oberfläche ist in der Lage, eine eingehende Störung lokal zu dämpfen, im Gegensatz zu einer komplett elastischen Oberfläche, wo sich die Störung über die gesamte Schaumlamelle verbreiten kann. Untersuchungen mittels der IR-VIS SFG Spektroskopie ergaben, dass die Struktur des Wassers bei der Beschreibung der Schaumstabilität auf molekularer Ebene eine entscheidende Rolle spielt: Die Oberflächenviskosität ist mit einem dissipativen Vorgang innerhalb der Grenzschicht verbunden. Dieser dissipative Vorgang konnte auf molekularer Ebene durch das Aufbrechen von Wasserstoffbrückenbindungen identifiziert werden. Ausschlaggebend war dabei der Austausch der adsorbierten Amphiphile in der Grenzfläche und der angrenzenden Sublage. KW - Nichtlineare Optik KW - Ellipsometrie KW - Schaum KW - Tensidlösung KW - Tensidschaum KW - Tensid KW - Ionisches Tensid KW - Hofmeister KW - Ionenspezifisch KW - Schaumstabilität KW - Schaumbildung KW - Summenfrequenzspektroskopie KW - Hofmeister KW - ions KW - foam KW - NLO KW - SFG KW - SHG Y1 - 2005 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus-5716 ER - TY - JOUR A1 - Hörmann, Ulrich A1 - Zeiske, Stefan A1 - Piersimoni, Fortunato A1 - Hoffmann, Lukas A1 - Schlesinger, Raphael A1 - Koch, Norbert A1 - Riedl, Thomas A1 - Andrienko, Denis A1 - Neher, Dieter T1 - Stark effect of hybrid charge transfer states at planar ZnO/organic interfaces JF - Physical review : B, Condensed matter and materials physics N2 - We investigate the bias dependence of the hybrid charge transfer state emission at planar heterojunctions between the metal oxide acceptor ZnO and three donor molecules. The electroluminescence peak energy linearly increases with the applied bias, saturating at high fields. Variation of the organic layer thickness and deliberate change of the ZnO conductivity through controlled photodoping allow us to confirm that this bias-induced spectral shift relates to the internal electric field in the organic layer rather than the filling of states at the hybrid interface. We show that existing continuum models overestimate the hole delocalization and propose a simple electrostatic model in which the linear and quadratic Stark effects are explained by the electrostatic interaction of a strongly polarizable molecular cation with its mirror image. Y1 - 2018 U6 - https://doi.org/10.1103/PhysRevB.98.155312 SN - 2469-9950 SN - 2469-9969 VL - 98 IS - 15 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Zeuschner, Steffen Peer A1 - Wang, Xi-Guang A1 - Deb, Marwan A1 - Popova, Elena A1 - Malinowski, Gregory A1 - Hehn, Michel A1 - Keller, Niels A1 - Berakdar, Jamal A1 - Bargheer, Matias T1 - Standing spin wave excitation in Bi BT - YIG films via temperature-induced anisotropy changes and magneto-elastic coupling JF - Physical review : B, Condensed matter and materials physics N2 - Based on micromagnetic simulations and experimental observations of the magnetization and lattice dynamics after the direct optical excitation of the magnetic insulator Bi : YIG or indirect excitation via an optically opaque Pt/Cu double layer, we disentangle the dynamical effects of magnetic anisotropy and magneto-elastic coupling. The strain and temperature of the lattice are quantified via modeling ultrafast x-ray diffraction data. Measurements of the time-resolved magneto-optical Kerr effect agree well with the magnetization dynamics simulated according to the excitation via two mechanisms: the magneto-elastic coupling to the experimentally verified strain dynamics and the ultrafast temperature-induced transient change in the magnetic anisotropy. The numerical modeling proves that, for direct excitation, both mechanisms drive the fundamental mode with opposite phase. The relative ratio of standing spin wave amplitudes of higher-order modes indicates that both mechanisms are substantially active. Y1 - 2022 U6 - https://doi.org/10.1103/PhysRevB.106.134401 SN - 2469-9950 SN - 2469-9969 VL - 106 IS - 13 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Feldmann, Johannes A1 - Levermann, Anders A1 - Mengel, Matthias T1 - Stabilizing the West Antarctic Ice Sheet by surface mass deposition JF - Science Advances N2 - There is evidence that a self-sustaining ice discharge from the West Antarctic Ice Sheet (WAIS) has started, potentially leading to its disintegration. The associated sea level rise of more than 3m would pose a serious challenge to highly populated areas including metropolises such as Calcutta, Shanghai, New York City, and Tokyo. Here, we show that the WAIS may be stabilized through mass deposition in coastal regions around Pine Island and Thwaites glaciers. In our numerical simulations, a minimum of 7400 Gt of additional snowfall stabilizes the flow if applied over a short period of 10 years onto the region (-2 mm year(-1) sea level equivalent). Mass deposition at a lower rate increases the intervention time and the required total amount of snow. We find that the precise conditions of such an operation are crucial, and potential benefits need to be weighed against environmental hazards, future risks, and enormous technical challenges. Y1 - 2019 U6 - https://doi.org/10.1126/sciadv.aaw4132 SN - 2375-2548 VL - 5 IS - 7 PB - American Assoc. for the Advancement of Science CY - Washington ER - TY - JOUR A1 - Schlemm, Tanja A1 - Feldmann, Johannes A1 - Winkelmann, Ricarda A1 - Levermann, Anders T1 - Stabilizing effect of melange buttressing on the marine ice-cliff instability of the West Antarctic Ice Sheet JF - The Cryosphere : TC ; an interactive open access journal of the European Geosciences Union N2 - Owing to global warming and particularly high regional ocean warming, both Thwaites and Pine Island Glaciers in the Amundsen region of the Antarctic Ice Sheet could lose their buttressing ice shelves over time. We analyse the possible consequences using the parallel ice sheet model (PISM), applying a simple cliff-calving parameterization and an ice melange-buttressing model. We find that the instantaneous loss of ice-shelf buttressing, due to enforced ice-shelf melting, initiates grounding-line retreat and triggers marine ice sheet instability (MISI). As a consequence, the grounding line progresses into the interior of the West Antarctic Ice Sheet and leads to a sea level contribution of 0.6 m within 100 a. By subjecting the exposed ice cliffs to cliff calving using our simplified parameterization, we also analyse marine ice cliff instability (MICI). In our simulations it can double or even triple the sea level contribution depending on the only loosely constrained parameter that determines the maximum cliff-calving rate. The speed of MICI depends on this upper bound of the calving rate, which is given by the ice melange buttressing the glacier. However, stabilization of MICI may occur for geometric reasons. Because the embayment geometry changes as MICI advances into the interior of the ice sheet, the upper bound on calving rates is reduced and the progress of MICI is slowed down. Although we cannot claim that our simulations bear relevant quantitative estimates of the effect of ice-melange buttressing on MICI, the mechanism has the potential to stop the instability. Further research is needed to evaluate its role for the past and future evolution of the Antarctic Ice Sheet. Y1 - 2022 U6 - https://doi.org/10.5194/tc-16-1979-2022 SN - 1994-0416 SN - 1994-0424 VL - 16 IS - 5 SP - 1979 EP - 1996 PB - Copernicus CY - Göttingen ER - TY - THES A1 - Kalbitz, René T1 - Stability of polarization in organic ferroelectric metal-insulator-semiconductor structures T1 - Stabilität der Ferroelektrischen Polarisation in Organischen Metall-Isolator-Halbleiter Strukturen N2 - Organic thin film transistors (TFT) are an attractive option for low cost electronic applications and may be used for active matrix displays and for RFID applications. To extend the range of applications there is a need to develop and optimise the performance of non-volatile memory devices that are compatible with the solution-processing fabrication procedures used in plastic electronics. A possible candidate is an organic TFT incorporating the ferroelectric co-polymer poly(vinylidenefluoride-trifluoroethylene)(P(VDF-TrFE)) as the gate insulator. Dielectric measurements have been carried out on all-organic metal-insulator-semiconductor structures with the ferroelectric polymer poly(vinylidenefluoride-trifluoroethylene) (P(VDF-TrFE)) as the gate insu-lator. The capacitance spectra of MIS devices, were measured under different biases, showing the effect of charge accumulation and depletion on the Maxwell-Wagner peak. The position and height of this peak clearly indicates the lack of stable depletion behavior and the decrease of mobility when increasing the depletion zone width, i.e. upon moving into the P3HT bulk. The lack of stable depletion was further investigated with capacitance-voltage (C-V) measurements. When the structure was driven into depletion, C-V plots showed a positive flat-band voltage shift, arising from the change in polarization state of the ferroelectric insulator. When biased into accumulation, the polarization was reversed. It is shown that the two polarization states are stable i.e. no depolarization occurs below the coercive field. However, negative charge trapped at the semiconductor-insulator interface during the depletion cycle masks the negative shift in flat-band voltage expected during the sweep to accumulation voltages. The measured output characteristics of the studied ferroelectric-field-effect transistors confirmed the results of the C-V plots. Furthermore, the results indicated a trapping of electrons at the positively charged surfaces of the ferroelectrically polarized P(VDF-TrFE) crystallites near the insulator/semiconductor in-terface during the first poling cycles. The study of the MIS structure by means of thermally stimulated current (TSC) revealed further evidence for the stability of the polarization under depletion voltages. It was shown, that the lack of stable depletion behavior is caused by the compensation of the orientational polarization by fixed electrons at the interface and not by the depolarization of the insulator, as proposed in several publications. The above results suggest a performance improvement of non-volatile memory devices by the optimization of the interface. N2 - Organische Transistoren sind besonders geeignet für die Herstellung verschiedener preisgünstiger, elektronischer Anwendungen, wie zum Beispiel Radio-Frequenz-Identifikations-Anhänger (RFID). Für die Erweiterung dieser Anwendung ist es notwendig die Funktion von organischen Speicherelementen weiter zu verbessern. Das ferroelektrische Polymer Poly(vinylidene-Fluoride-Trifluoroethylene) (P(VDF-TrFE)) eignet sich besonders gut als remanent polarisierbarer Isolator in Dünnschich-Speicherelementen. Um Schalt- und Polarisationsverhalten solcher Speicherelemente zu untersuchen, wurden P(VDF-TrFE)-Kondensatoren und Metall-Halbleiter-Isolator-Proben sowie ferroelektrische Feld-Effekt-Transistoren (Fe-FET) aus dem Halbleiter Poly(3-Hexylthiophene) (P3HT) und P(VDF-TrFE) hergestellt und dielektrisch untersucht. Die Charakterisierung der MIS-Strukturen mittels spannungsabhängiger Kapazitätsspektren machte deutlich, dass es nicht möglich ist, einen stabilen Verarmungzustand (Aus-Zustand) zu realisieren. Kapazität-Spannungs-Messungen (C-V) an MIS-Proben mit uni/bi-polaren Spannungszyklen zeigten eine stabile ferroelektrische Polarisation des P(VDF-TrFE)-Films. Eine Depolarisation des Isolators durch den Mangel an Minoritäts-Ladungsträgern konnte als Grund für die Instabilität des Verarmungs-Zustandes ausgeschlossen werden. Die C-V-Kurven wiesen vielmehr auf die Existenz fixierter, negativer Ladungsträger an der Grenzfläche hin. Zusammenfassend kann festgestellt werden: die Ursache der Ladungsträgerinstabilitäten in organischen ferroelektrischen Speicherelementen ist auf die Kompensation der ferroelektrischen Orientierungspolarisation durch "getrappte"(fixierte) negative Ladungsträger zurückzuführen. Dieses Ergebnis liefert nun eine Grundlage für die Optimierung der Isolator/Halbleiter-Grenzfläche mit dem Ziel, die Zahl der Fallenzustände zu minimieren. Auf diesem Wege könnte die Stabilität des Speicherzustandes in organischen Dünnschichtspeicherelementen deutlich verbessert werden. KW - ferroelektrische Polarisation KW - Metall-Isolator-Halbleiter KW - organische Elektronik KW - Dielektrische Spektroskopie KW - Feld-Effekt-Transistoren KW - organic electronic KW - dielectric spectroskopie KW - non-volatile memory KW - organic electronic KW - ferroelectric polarization Y1 - 2011 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus-57276 ER - TY - JOUR A1 - Schirdewahn, Daniel T1 - Stability of a parametric harmonic oscillator with dichotomic noise JF - Chaos : an interdisciplinary journal of nonlinear science N2 - The harmonic oscillator is a powerful model that can appear as a limit case when examining a nonlinear system. A well known fact is that, without driving, the inclusion of a friction term makes the origin of the phase space-which is a fixed point of the system-linearly stable. In this work, we include a telegraph process as perturbation of the oscillator's frequency, for example, to describe the motion of a particle with fluctuating charge gyrating in an external magnetic field. Increasing intensity of this colored noise is capable of changing the quality of the fixed point. To characterize the stability of the system, we use a stability measure that describes the growth of the displacement of the system's phase space position and express it in a closed form. We expand the respective exponent for light friction and low noise intensity and compare both the exact analytic solution and the expansion to numerical values. Our findings allow stability predictions for several physical systems. Y1 - 2020 U6 - https://doi.org/10.1063/5.0012946 SN - 1054-1500 SN - 1089-7682 VL - 30 IS - 9 PB - American Institute of Physics CY - Melville ER - TY - THES A1 - Kuhlbrodt, Till T1 - Stability and variability of open-ocean deep convection in deterministic and stochastic simple models N2 - Die Tiefenkonvektion ist ein wesentlicher Bestandteil der Zirkulation im Nordatlantik. Sie beeinflusst den nordwärtigen Wärmetransport der thermohalinen Zirkulation. Ein Verständnis ihrer Stabilität und Variabilität ist daher nötig, um Klimaveränderungen im Bereich des Nordatlantiks einschätzen zu können. Diese Arbeit hat zum Ziel, das konzeptionelle Verständnis der Stabilität und der Variabilität der Tiefenkonvektion zu verbessern. Beobachtungsdaten aus der Labradorsee zeigen Phasen mit und ohne Tiefenkonvektion. Ein einfaches Modell mit zwei Boxen wird an diese Daten angepasst. Das Ergebnis legt nahe, dass die Labradorsee zwei koexistierende stabile Zustände hat, einen mit regelmäßiger Tiefenkonvektion und einen ohne Tiefenkonvektion. Diese Bistabilität ergibt sich aus einer positiven Salzgehalts-Rückkopplung, deren Ursache ein Netto-Süßwassereintrag in die Deckschicht ist. Der konvektive Zustand kann schnell instabil werden, wenn der mittlere Antrieb sich hin zu wärmeren oder weniger salzhaltigen Bedingungen ändert. Die wetterbedingte Variabilität des externen Antriebs wird durch die Addition eines stochastischen Antriebsterms in das Modell eingebaut. Es zeigt sich, dass dann die Tiefenkonvektion häufig an- und wieder ausgeschaltet wird. Die mittlere Aufenthaltszeit in beiden Zuständen ist ein Maß ihrer stochastischen Stabilität. Die stochastische Stabilität hängt in glatter Weise von den Parametern des Antriebs ab, im Gegensatz zu der deterministischen (nichtstochastischen) Stabilität, die sich abrupt ändern kann. Sowohl das Mittel als auch die Varianz des stochastischen Antriebs beeinflussen die Häufigkeit von Tiefenkonvektion. Eine Abnahme der Konvektionshäufigkeit, als Reaktion auf eine Abnahme des Salzgehalts an der Oberfläche, kann zum Beispiel durch eine Zunahme der Variabilität in den Wärmeflüssen kompensiert werden. Mit einem weiter vereinfachten Box-Modell werden einige Eigenschaften der stochastischen Stabilität analytisch untersucht. Es wird ein neuer Effekt beschrieben, die wandernde Monostabilität: Auch wenn die Tiefenkonvektion aufgrund geänderter Parameter des Antriebs kein stabiler Zustand mehr ist, kann der stochastische Antrieb immer noch häufig Konvektionsereignisse auslösen. Die analytischen Gleichungen zeigen explizit, wie die wandernde Monostabilität sowie andere Effekte von den Modellparametern abhängen. Diese Abhängigkeit ist für die mittleren Aufenthaltszeiten immer exponentiell, für die Wahrscheinlichkeit langer nichtkonvektiver Phasen dagegen nur dann, wenn diese Wahrscheinlichkeit gering ist. Es ist zu erwarten, dass wandernde Monostabilität auch in anderen Teilen des Klimasystems eine Rolle spielt. Insgesamt zeigen die Ergebnisse, dass die Stabilität der Tiefenkonvektion in der Labradorsee sehr empfindlich auf den Antrieb reagiert. Die Rolle der Variabilität ist entscheidend für ein Verständnis dieser Empfindlichkeit. Kleine Änderungen im Antrieb können bereits die Häufigkeit von Tiefenkonvektionsereignissen deutlich mindern, was sich vermutlich stark auf das regionale Klima auswirkt. N2 - Deep convection is an essential part of the circulation in the North Atlantic Ocean. It influences the northward heat transport achieved by the thermohaline circulation. Understanding its stability and variability is therefore necessary for assessing climatic changes in the area of the North Atlantic. This thesis aims at improving the conceptual understanding of the stability and variability of deep convection. Observational data from the Labrador Sea show phases with and without deep convection. A simple two-box model is fitted to these data. The results suggest that the Labrador Sea has two coexisting stable states, one with regular deep convection and one without deep convection. This bistability arises from a positive salinity feedback that is due to the net freshwater input into the surface layer. The convecting state can easily become unstable if the mean forcing shifts to warmer or less saline conditions. The weather-induced variability of the external forcing is included into the box model by adding a stochastic forcing term. It turns out that deep convection is then switched "on" and "off" frequently. The mean residence time in either state is a measure of its stochastic stability. The stochastic stability depends smoothly on the forcing parameters, in contrast to the deterministic (non-stochastic) stability which may change abruptly. The mean and the variance of the stochastic forcing both have an impact on the frequency of deep convection. For instance, a decline in convection frequency due to a surface freshening may be compensated for by an increased heat flux variability. With a further simplified box model some stochastic stability features are studied analytically. A new effect is described, called wandering monostability: even if deep convection is not a stable state due to changed forcing parameters, the stochastic forcing can still trigger convection events frequently. The analytical expressions explicitly show how wandering monostability and other effects depend on the model parameters. This dependence is always exponential for the mean residence times, but for the probability of long nonconvecting phases it is exponential only if this probability is small. It is to be expected that wandering monostability is relevant in other parts of the climate system as well. All in all, the results demonstrate that the stability of deep convection in the Labrador Sea reacts very sensitively to the forcing. The presence of variability is crucial for understanding this sensitivity. Small changes in the forcing can already significantly lower the frequency of deep convection events, which presumably strongly affects the regional climate. ----Anmerkung: Der Autor ist Träger des durch die Physikalische Gesellschaft zu Berlin vergebenen Carl-Ramsauer-Preises 2003 für die jeweils beste Dissertation der vier Universitäten Freie Universität Berlin, Humboldt-Universität zu Berlin, Technische Universität Berlin und Universität Potsdam. KW - Labradorsee ; Thermohaline Konvektion ; Stochastisches Modell KW - Stochastische dynamische Systeme KW - Nichtlineare Dynamik KW - Bistabilität KW - Nordatlantik KW - Stochastic dynamical systems KW - Nonlinear dynamics KW - Bistability KW - North Atlantic Y1 - 2002 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-0000622 ER - TY - INPR A1 - Seehafer, Norbert A1 - Schumacher, Jörg T1 - Squire‘s theorem for the magnetohydrodynamic sheet pinch N2 - The stability of the quiescent ground state of an incompressible viscous fluid sheet bounded by two parallel planes, with an electrical conductivity varying across the sheet, and driven by an external electric field tangential to the boundaries is considered. It is demonstrated that irrespective of the conductivity profile, as magnetic and kinetic Reynolds numbers (based on the Alfvén velocity) are raised from small values, two-dimensional perturbations become unstable first. T3 - NLD Preprints - 40 Y1 - 1997 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus-14628 ER - TY - JOUR A1 - Mardoukhi, Yousof A1 - Chechkin, Aleksei V. A1 - Metzler, Ralf T1 - Spurious ergodicity breaking in normal and fractional Ornstein–Uhlenbeck process JF - New Journal of Physics N2 - The Ornstein–Uhlenbeck process is a stationary and ergodic Gaussian process, that is fully determined by its covariance function and mean. We show here that the generic definitions of the ensemble- and time-averaged mean squared displacements fail to capture these properties consistently, leading to a spurious ergodicity breaking. We propose to remedy this failure by redefining the mean squared displacements such that they reflect unambiguously the statistical properties of any stochastic process. In particular we study the effect of the initial condition in the Ornstein–Uhlenbeck process and its fractional extension. For the fractional Ornstein–Uhlenbeck process representing typical experimental situations in crowded environments such as living biological cells, we show that the stationarity of the process delicately depends on the initial condition. KW - Ornstein–Uhlenbeck process KW - stationary stochastic process KW - ensemble and time averaged mean squared displacement Y1 - 2020 U6 - https://doi.org/10.1088/1367-2630/ab950b SN - 1367-2630 VL - 22 PB - IOP CY - London ER - TY - GEN A1 - Mardoukhi, Yousof A1 - Chechkin, Aleksei V. A1 - Metzler, Ralf T1 - Spurious ergodicity breaking in normal and fractional Ornstein–Uhlenbeck process T2 - Postprints der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe N2 - The Ornstein–Uhlenbeck process is a stationary and ergodic Gaussian process, that is fully determined by its covariance function and mean. We show here that the generic definitions of the ensemble- and time-averaged mean squared displacements fail to capture these properties consistently, leading to a spurious ergodicity breaking. We propose to remedy this failure by redefining the mean squared displacements such that they reflect unambiguously the statistical properties of any stochastic process. In particular we study the effect of the initial condition in the Ornstein–Uhlenbeck process and its fractional extension. For the fractional Ornstein–Uhlenbeck process representing typical experimental situations in crowded environments such as living biological cells, we show that the stationarity of the process delicately depends on the initial condition. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 981 KW - Ornstein–Uhlenbeck process KW - stationary stochastic process KW - ensemble and time averaged mean squared displacement Y1 - 2020 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-474875 SN - 1866-8372 IS - 981 ER - TY - JOUR A1 - Decker, Regis A1 - Born, Artur A1 - Ruotsalainen, Kari A1 - Bauer, Karl A1 - Haverkamp, Robert A1 - Büchner, Robby A1 - Pietzsch, Annette A1 - Föhlisch, Alexander T1 - Spin-lattice angular momentum transfer of localized and valence electrons in the demagnetization transient state of gadolinium JF - Applied physics letters N2 - The electron-phonon scattering is one of the main microscopic mechanisms responsible for the spin-flip in the transient state of ultrafast demagnetization. Here, we present an experimental determination of the temperature-dependent electron-phonon scattering rate in Gd. Using a static x-ray emission spectroscopy method, where the reduction of the decay peak intensities when increasing the temperature is quantified, we measure independently the electron-phonon scattering rate for the 5d and the 4f electrons. We deduce the temperature dependence of scattering for the 5d electrons, while no effect on the phonon population is observed for the 4f electrons. Our results suggest that the ultrafast magnetization dynamics in Gd is triggered by the spin-flip in the 5d electrons. We also evidence the existence of a temperature threshold, above which spin-flip scattering of the 5d electrons takes place. We deduce that during the transient state of ultrafast demagnetization, the exchange energy between 5d electrons has to be overcome before the microscopic electron-phonon scattering process can occur. Y1 - 2021 U6 - https://doi.org/10.1063/5.0063404 SN - 0003-6951 SN - 1077-3118 VL - 119 IS - 15 PB - AIP Publishing CY - Melville ER - TY - THES A1 - Krivenkov, Maxim T1 - Spin textures and electron scattering in nanopatterned monolayer graphene N2 - The current thesis is focused on the properties of graphene supported by metallic substrates and specifically on the behaviour of electrons in such systems. Methods of scanning tunneling microscopy, electron diffraction and photoemission spectroscopy were applied to study the structural and electronic properties of graphene. The purpose of the first part of this work is to introduce the most relevant aspects of graphene physics and the methodical background of experimental techniques used in the current thesis. The scientific part of this work starts with the extensive study by means of scanning tunneling microscopy of the nanostructures that appear in Au intercalated graphene on Ni(111). This study was aimed to explore the possible structural explanations of the Rashba-type spin splitting of ~100 meV experimentally observed in this system — much larger than predicted by theory. It was demonstrated that gold can be intercalated under graphene not only as a dense monolayer, but also in the form of well-periodic arrays of nanoclusters, a structure previously not reported. Such nanocluster arrays are able to decouple graphene from the strongly interacting Ni substrate and render it quasi-free-standing, as demonstrated by our DFT study. At the same time calculations confirm strong enhancement of the proximity-induced SOI in graphene supported by such nanoclusters in comparison to monolayer gold. This effect, attributed to the reduced graphene-Au distance in the case of clusters, provides a large Rashba-type spin splitting of ~60 meV. The obtained results not only provide a possible mechanism of SOI enhancement in this particular system, but they can be also generalized for graphene on other strongly interacting substrates intercalated by nanostructures of heavy noble d metals. Even more intriguing is the proximity of graphene to heavy sp-metals that were predicted to induce an intrinsic SOI and realize a spin Hall effect in graphene. Bismuth is the heaviest stable sp-metal and its compounds demonstrate a plethora of exciting physical phenomena. This was the motivation behind the next part of the current thesis, where structural and electronic properties of a previously unreported phase of Bi-intercalated graphene on Ir(111) were studied by means of scanning tunneling microscopy, spin- and angle-resolved photoemission spectroscopy and electron diffraction. Photoemission experiments revealed a remarkable, nearly ideal graphene band structure with strongly suppressed signatures of interaction between graphene and the Ir(111) substrate, moreover, the characteristic moiré pattern observed in graphene on Ir(111) by electron diffraction and scanning tunneling microscopy was strongly suppressed after intercalation. The whole set of experimental data evidences that Bi forms a dense intercalated layer that efficiently decouples graphene from the substrate. The interaction manifests itself only in the n-type charge doping (~0.4 eV) and a relatively small band gap at the Dirac point (~190 meV). The origin of this minor band gap is quite intriguing and in this work it was possible to exclude a wide range of mechanisms that could be responsible for it, such as induced intrinsic spin-orbit interaction, hybridization with the substrate states and corrugation of the graphene lattice. The main origin of the band gap was attributed to the A-B symmetry breaking and this conclusion found support in the careful analysis of the interference effects in photoemission that provided the band gap estimate of ~140 meV. While the previous chapters were focused on adjusting the properties of graphene by proximity to heavy metals, graphene on its own is a great object to study various physical effects at crystal surfaces. The final part of this work is devoted to a study of surface scattering resonances by means of photoemission spectroscopy, where this effect manifests itself as a distinct modulation of photoemission intensity. Though scattering resonances were widely studied in the past by means of electron diffraction, studies about their observation in photoemission experiments started to appear only recently and they are very scarce. For a comprehensive study of scattering resonances graphene was selected as a versatile model system with adjustable properties. After the theoretical and historical introduction to the topic of scattering resonances follows a detailed description of the unusual features observed in the photoemission spectra obtained in this work and finally the equivalence between these features and scattering resonances is proven. The obtained photoemission results are in a good qualitative agreement with the existing theory, as verified by our calculations in the framework of the interference model. This simple model gives a suitable explanation for the general experimental observations. The possibilities of engineering the scattering resonances were also explored. A systematic study of graphene on a wide range of substrates revealed that the energy position of the resonances is in a direct relation to the magnitude of charge transfer between graphene and the substrate. Moreover, it was demonstrated that the scattering resonances in graphene on Ir(111) can be suppressed by nanopatterning either by a superlattice of Ir nanoclusters or by atomic hydrogen. These effects were attributed to strong local variations of tork function and/or destruction of long-range order of thephene lattice. The tunability of scattering resonances can be applied for optoelectronic devices based on graphene. Moreover, the results of this study expand the general understanding of the phenomenon of scattering resonances and are applicable to many other materials besides graphene. N2 - Die vorliegende Arbeit beschäftigt sich mit den Eigenschaften von Graphen auf metallischen Substraten und speziell mit dem Verhalten von Elektronen in solchen Systemen. Der wissenschaftliche Teil dieser Arbeit beginnt mit der umfassenden Untersuchung von Nanostrukturen, die in Au-interkaliertem Graphen auf Ni(111) auftreten, mittels Rastertunnelmikroskopie (RTM). Diese Studie zielte darauf ab, die möglichen strukturellen Erklärungen der experimentell in diesem System beobachteten Rashba- Spin-Aufspaltung von ~100 meV zu untersuchen — die viel größer als theoretisch vorhergesagt ist. Es wurde gezeigt, dass Gold unter Graphen nicht nur als dichte Monolage interkaliert werden kann, sondern auch in Form von exakt periodischen Anordnungen von Nanoclustern, einer Struktur, die bisher nicht beschrieben wurde. Solche Nanocluster-Arrays können Graphen von dem stark wechselwirkenden Ni-Substrat entkoppeln und es quasi freistehend machen, wie unsere Dichtefunktionaltheorie-Studie zeigt. Gleichzeitig bestätigen die Dichtefunktionaltheorie-Rechnungen eine starke Erhöhung der durch Proximity induzierten Spin-Bahn-Wechselwirkung (SBW) in Graphen durch solche Nanocluster im Vergleich zu einer homogenen Gold-Monolage. Dieser Effekt, der im Falle von Clustern auf den verringerten Graphen-Au-Abstand zurückgeführt wird, liefert eine große Spinaufspaltung vom Rashba-Typ von ~60 meV. Die erhaltenen Ergebnisse liefern nicht nur einen möglichen Mechanismus zur Erhöhung der SBW in diesem speziellen System, sondern können auch auf Graphen auf anderen stark wechselwirkenden Substraten verallgemeinert werden, die mit Nanostrukturen von schweren Edelmetallen interkaliert sind. Noch faszinierender ist die Nähe von Graphen zu schweren sp-Metallen, von denen vorhergesagt wurde, dass sie eine intrinsische SBW induzieren und einen Spin-Hall-Effekt in Graphen realisieren. Wismut ist das schwerste stabile sp-Metall und seine Verbindungen zeigen eine Vielzahl aufregender physikalischer Phänomene. Dies war die Motivation für den nächsten Teil der vorliegenden Arbeit, in dem strukturelle und elektronische Eigenschaften einer bisher nicht beschriebenen Phase von Bismuth-interkaliertem Graphen auf Ir(111) untersucht werden. Experimente ergaben eine nahezu ideale Graphenbandstruktur mit stark unterdrückten Wechselwirkungssignaturen zwischen Graphen und dem Ir(111)-Substrat. Die gesamten experimentellen Daten belegen, dass Bi eine dichte interkalierte Schicht bildet, die Graphen effizient vom Substrat entkoppelt. Die Wechselwirkung manifestiert sich nur in der Ladungsdotierung vom n-Typ (~0,4 eV) und einer Bandlücke am Dirac-Punkt (~190 meV). Den Ursprung dieser Bandlücke zu ermitteln ist sehr komplex, und in dieser Arbeit konnte eine Vielzahl von Mechanismen ausgeschlossen werden, die dafür verantwortlich sein könnten, wie etwa induzierte intrinsische SBW, Hybridisierung mit den Substratzuständen und Riffelung des Graphen-Gitters. Der Hauptursprung der Bandlücke wurde einem Bruch der A-B -Symmetrie zugeschrieben, und diese Schlussfolgerung stützte sich auf eine eingehende Analyse der Interferenzeffekte bei der Photoemission, die eine Abschätzung der Bandlücke von ~140 meV lieferte. Während sich die vorherigen Kapitel auf die Anpassung der Eigenschaften von Graphen durch die Nähe zu Schwermetallen konzentrierten, ist Graphen allein ein großartiges Objekt, um verschiedene physikalische Effekte an Kristalloberflächen zu untersuchen. Der letzte Teil dieser Arbeit befasst sich mit der Photoemissionsspektroskopie Untersuchung von Oberflächenstreuresonanzen, deren Effekt sich in einer deutlichen Modulation der Photoemissionsintensität manifestiert. Obwohl Streuresonanzen in der Vergangenheit häufig mittels Elektronenbeugung untersucht wurden, erschienen einige wenige Studien über ihre Beobachtung in Photoemissionsexperimenten erst vor kurzem. Für eine umfassende Untersuchung der Streuresonanzen wurde Graphen als vielseitiges Modellsystem mit einstellbaren Eigenschaften ausgewählt. Das Kapitel beginnt mit einer historischen Einführung in das Thema Streuresonanzen, gefolgt von der Beschreibung der ungewöhnlichen Photoemissionsspektralmerkmale, die in dieser Arbeit erhalten wurden. Schließlich wird die Äquivalenz zwischen diesen Merkmalen und Streuresonanzen bewiesen. Die erhaltenen Photoemissionsergebnisse stimmen qualitativ gut mit der bestehenden Theorie überein, wie unsere Berechnungen im Rahmen des Interferenzmodells belegen. Dieses einfache Modell liefert eine geeignete Erklärung für die Gesamtheit der experimentellen Beobachtungen. Möglichkeiten, die Streuresonanzen zu modifizieren wurden ebenfalls untersucht. Eine systematische Untersuchung von Graphen auf einer Vielzahl von Substraten ergab, dass die Energieposition der Resonanzen in direktem Zusammenhang mit der Größe des Ladungstransfers zwischen Graphen und Substrat steht. Darüber hinaus wurde gezeigt, dass die Streuresonanzen in Graphen auf Ir(111) durch Nanostrukturierung entweder durch ein Übergitter von Ir-Nanoclustern oder durch atomaren Wasserstoff unterdrückt werden können. Diese Effekte wurden auf starke lokale Variationen der Austrittsarbeit und/oder die Zerstörung der langreichweitigen Ordnung des Graphengitters zurückgeführt. Die Abstimmbarkeit von Streuresonanzen kann für optoelektronische Bauelemente auf der Basis von Graphen verwendet werden. Darüber hinaus erweitern die Ergebnisse dieser Studie das allgemeine Verständnis des Phänomens der Streuresonanzen und sind neben Graphen auch auf viele andere Materialien anwendbar. T2 - Spin-Texturen und Elektronenstreuung in nanostrukturiertem Monolage-Graphen KW - graphene KW - spin texture KW - scattering resonances KW - Rashba effect KW - bismuth KW - Rashba-Effekt KW - Wismut KW - Graphen KW - Streuresonanzen KW - Spin Textur Y1 - 2020 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-487017 ER - TY - THES A1 - Scholz, Markus Reiner T1 - Spin polarization, circular dichroism, and robustness of topological surface states T1 - Spinpolarisation, Zirkulardichroismus und Robustheit Topologischer Oberflächenzustände BT - a photoemission study BT - eine Photoemissionsstudie N2 - Dreidimensionale topologische Isolatoren sind ein neues Materialsystem, welches dadurch charakterisiert ist, dass es in seinem Inneren isolierend an der Ober äche jedoch leitend ist. Ursächlich für die Leitfähigkeit an der Ober äche sind sogenannte topologische Ober- ächenzustände, welche das Valenzband des Inneren mit dem Leitungsband des Inneren verbinden. An der Ober äche ist also die Bandlücke, welche die isolierende Eigenschaft verursacht, geschlossen. Die vorliegende Arbeit untersucht diese Ober ächenzustände mittels spin- und winkelauf- gelöster Photoemissionsspektroskopie. Es wird gezeigt, dass in den Materialien Bi2Se3 und Bi2Te3, in übereinstimmung mit der Literatur, die entscheidenden Charakteristika eines topologischen Ober ächenzustands vorzu nden sind: Die Ober ächenzustände dieser Sys- teme durchqueren die Bandlücke in ungerader Anzahl, sie sind nicht entartet und weisen folgerichtig eine hohe Spinpolarisation auf. Weiterhin wird durch Aufdampfen diverser Adsorbate gezeigt, dass der Ober ächenzustän- de von Bi2Se3 und Bi2Te3, wie erwartet, extrem robust ist. Ober ächenzustände topologisch trivialer Systeme erfüllen diese Eigenschaft nicht; bereits kleine Verunreinigungen kön- nen diese Zustände zerstören, bzw. die Ober äche isolierend machen. Die topologischen Ober ächenzustände können in der vorliegenden Arbeit noch bis zur Detektionsgrenze der experimentellen Messmethode nachgewiesen werden und die Ober äche bleibt Leitfähig. Unter den Adsorbaten be ndet sich auch Eisen, ein bekanntermaßen magnetisches Materi- al. Eine der Grundvoraussetzungen für topologische Isolatoren ist die Zeitumkehrsymme- trie, die Elektronen, welche den topologischen Ober ächenzustand besetzen, vorschreibt, dass sie eine bestimmte Spinrichtung haben müssen, wenn sie sich beispielsweise nach links bewegen und den entgegengesetzten Spin wenn sie sich nach rechts bewegen. In magnetischen Materialien ist die Zeitumkehrsymmetrie jedoch explizit gebrochen und die gezeigte Robustheit des Ober ächenzustands gegen magnetische Materialien daher uner- wartet. Die Zeitumkehrsymmetrie sorgt auch dafür, dass eine Streuung der Elektronen um 180°, beispielsweise an einem Gitterdefekt oder an einem Phonon strikt verboten ist. Bei einem solchen Streuprozess bleibt die Spinrichtung erhalten, da aber in der Gegenrichtung nur Zustände mit entgegengesetztem Spin vorhanden sind kann das Elektron nicht in diese Richtung gestreut werden. Dieses Prinzip wird anhand der Lebensdauer der durch Pho- toemission angeregten Zustände untersucht. Hierbei wird gezeigt, dass die Kopplung der Elektronen des Ober ächenzustands von Bi2Te3 an Phononen unerwartet hoch ist und dass sich eine Anisotropie in der Bandstruktur des Selbigen auch in den Lebensdauern der ange- regten Zustände widerspiegelt. Weiterhin wird gezeigt, dass sich die Ein üsse von magne- tischen und nicht-magnetischen Verunreinigungen auf die Lebensdauern stark voneinander unterscheiden. Im letzten Teil der vorliegenden Arbeit wird untersucht, ob eine Asymmetrie in der Inten- sitätsverteilung der winkelaufgelösten Photoemissionsspektren, bei Anregung mit zirku- lar polarisiertem Licht, in Bi2Te3 Rückschlüsse auf die Spinpolarisation der Elektronen erlaubt. Bei Variation der Energie des eingestrahlten Lichts wird ein Vorzeichenwechsel der Asymmetrie beobachtet. Daraus lässt sich schlussfolgern, dass die Asymmetrie keine Rückschlüsse auf die Spinpolarisation erlaubt. N2 - This thesis is focussed on the electronic properties of the new material class named topological insulators. Spin and angle resolved photoelectron spectroscopy have been applied to reveal several unique properties of the surface state of these materials. The first part of this thesis introduces the methodical background of these quite established experimental techniques. In the following chapter, the theoretical concept of topological insulators is introduced. Starting from the prominent example of the quantum Hall effect, the application of topological invariants to classify material systems is illuminated. It is explained how, in presence of time reversal symmetry, which is broken in the quantum Hall phase, strong spin orbit coupling can drive a system into a topologically non trivial phase. The prediction of the spin quantum Hall effect in two dimensional insulators an the generalization to the three dimensional case of topological insulators is reviewed together with the first experimental realization of a three dimensional topological insulator in the Bi1-xSbx alloys given in the literature. The experimental part starts with the introduction of the Bi2X3 (X=Se, Te) family of materials. Recent theoretical predictions and experimental findings on the bulk and surface electronic structure of these materials are introduced in close discussion to our own experimental results. Furthermore, it is revealed, that the topological surface state of Bi2Te3 shares its orbital symmetry with the bulk valence band and the observation of a temperature induced shift of the chemical potential is to a high probability unmasked as a doping effect due to residual gas adsorption. The surface state of Bi2Te3 is found to be highly spin polarized with a polarization value of about 70% in a macroscopic area, while in Bi2Se3 the polarization appears reduced, not exceeding 50%. We, however, argue that the polarization is most likely only extrinsically limited in terms of the finite angular resolution and the lacking detectability of the out of plane component of the electron spin. A further argument is based on the reduced surface quality of the single crystals after cleavage and, for Bi2Se3 a sensitivity of the electronic structure to photon exposure. We probe the robustness of the topological surface state in Bi2X3 against surface impurities in Chapter 5. This robustness is provided through the protection by the time reversal symmetry. Silver, deposited on the (111) surface of Bi2Se3 leads to a strong electron doping but the surface state is observed up to a deposited Ag mass equivalent to one atomic monolayer. The opposite sign of doping, i.e., hole-like, is observed by exposing oxygen to Bi2Te3. But while the n-type shift of Ag on Bi2Se3 appears to be more or less rigid, O2 is lifting the Dirac point of the topological surface state in Bi2Te3 out of the valence band minimum at $\Gamma$. After increasing the oxygen dose further, it is possible to shift the Dirac point to the Fermi level, while the valence band stays well beyond. The effect is found reversible, by warming up the samples which is interpreted in terms of physisorption of O2. For magnetic impurities, i.e., Fe, we find a similar behavior as for the case of Ag in both Bi2Se3 and Bi2Te3. However, in that case the robustness is unexpected, since magnetic impurities are capable to break time reversal symmetry which should introduce a gap in the surface state at the Dirac point which in turn removes the protection. We argue, that the fact that the surface state shows no gap must be attributed to a missing magnetization of the Fe overlayer. In Bi2Te3 we are able to observe the surface state for deposited iron mass equivalents in the monolayer regime. Furthermore, we gain control over the sign of doping through the sample temperature during deposition. Chapter6 is devoted to the lifetime broadening of the photoemission signal from the topological surface states of Bi2Se3 and Bi2Te3. It is revealed that the hexagonal warping of the surface state in Bi2Te3 introduces an anisotropy for electrons traveling along the two distinct high symmetry directions of the surface Brillouin zone, i.e., $\Gamma$K and $\Gamma$M. We show that the phonon coupling strength to the surface electrons in Bi2Te3 is in nice agreement with the theoretical prediction but, nevertheless, higher than one may expect. We argue that the electron-phonon coupling is one of the main contributions to the decay of photoholes but the relatively small size of the Fermi surface limits the number of phonon modes that may scatter off electrons. This effect is manifested in the energy dependence of the imaginary part of the electron self energy of the surface state which shows a decay to higher binding energies in contrast to the monotonic increase proportional to E$^2$ in the Fermi liquid theory due to electron-electron interaction. Furthermore, the effect of the surface impurities of Chapter 5 on the quasiparticle life- times is investigated. We find that Fe impurities have a much stronger influence on the lifetimes as compared to Ag. Moreover, we find that the influence is stronger independently of the sign of the doping. We argue that this observation suggests a minor contribution of the warping on increased scattering rates in contrast to current belief. This is additionally confirmed by the observation that the scattering rates increase further with increasing silver amount while the doping stays constant and by the fact that clean Bi2Se3 and Bi2Te3 show very similar scattering rates regardless of the much stronger warping in Bi2Te3. In the last chapter we report on a strong circular dichroism in the angle distribution of the photoemission signal of the surface state of Bi2Te3. We show that the color pattern obtained by calculating the difference between photoemission intensities measured with opposite photon helicity reflects the pattern expected for the spin polarization. However, we find a strong influence on strength and even sign of the effect when varying the photon energy. The sign change is qualitatively confirmed by means of one-step photoemission calculations conducted by our collaborators from the LMU München, while the calculated spin polarization is found to be independent of the excitation energy. Experiment and theory together unambiguously uncover the dichroism in these systems as a final state effect and the question in the title of the chapter has to be negated: Circular dichroism in the angle distribution is not a new spin sensitive technique. KW - topological insulators KW - angle resolved photoelectron spectroscopy KW - spin resolved photoelectron spectroscopy KW - Bi2Se3 KW - Bi2Te3 KW - quasiparticle interactions KW - circular dichroism KW - spin-orbit coupling KW - time reversal symmetry KW - surface states KW - Spinpolarisation KW - Zirkulardichroismus KW - topologische Isolatoren KW - Oberflächenzustände KW - winkelaufgelöste Photoelektronenspektroskopie KW - spinaufgelöste Photoelektronenspektroskopie KW - Magnetismus KW - Bi2Te3 KW - Bi2Se3 Y1 - 2012 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-96686 ER - TY - JOUR A1 - Horovitz, Baruch A1 - Henkel, Carsten T1 - Spin entanglement via scanning tunneling microscope current JF - Physical review : B, Condensed matter and materials physics N2 - We consider a system of two spins under a scanning tunneling microscope bias and derive its master equation. We find that the tunneling elements to the electronic contacts (tip and substrate) generate an exchange interaction between the spins as well as a Dzyaloshinskii-Moriya interaction in the presence of spin-orbit coupling. The tunnel current spectrum then shows additional lines compared to conventional spin-resonance experiments. When the spins have degenerate Larmor frequencies and equal tunneling amplitudes (without spin orbit), there is a dark state with a vanishing decay rate. The coupling to the electronic environment generates significant spin-spin entanglement via the dark state, even if the initial state is nonentangled. Y1 - 2021 U6 - https://doi.org/10.1103/PhysRevB.104.L081405 SN - 2469-9950 SN - 2469-9969 VL - 104 IS - 8 PB - American Physical Society CY - Ridge, NY ER - TY - THES A1 - Maerten, Lena T1 - Spectroscopic perspectives on ultrafast coupling phenomena in perovskite oxides T1 - Spektroskopische Untersuchung ultraschneller Kopplungsphänomene in Perowskit-Oxiden N2 - In this thesis, I study ultrafast dynamics in perovskite oxides using time resolved broadband spectroscopy. I focus on the observation of coherent phonon propagation by time resolved Brillouin scattering: following the excition of metal transducer films with a femtosecond infrared pump pulse, coherent phonon dynamics in the GHz frequency range are triggered. Their propagation is monitored using a delayed white light probe pulse. The technique is illustrated on various thin films and multilayered samples. I apply the technique to investigate the linear and nonlinear acoustic response in bulk SrTiO_3, which displays a ferroelastic phase transition from a cubic to a tetragonal structural phase at T_a=105 K. In the linear regime, I observe a coupling of the observed acoustic phonon mode to the softening optic modes describing the phase transition. In the nonlinear regime, I find a giant slowing down of the sound velocity in the low temperature phase that is only observable for a strain amplitude exceeding the tetragonality of the material. It is attributed to a coupling of the high frequency phonons to ferroelastic domain walls in the material. I propose a new mechanism for the coupling of strain waves to the domain walls that is only effective for high amplitude strain. A detailed study of the phonon attenuation across a wide temperature range shows that the phonon attenuation at low temperatures is influenced by the domain configuration, which is determined by interface strain. Preliminary measurements on magnetic-ferroelectric multilayers reveal that the excitation fluence needs to be carefully controlled when dynamics at phase transitions are studied. N2 - In dieser Doktorarbeit untersuche ich ultraschnelle Dynamik in perovskitischen Oxiden mittels zeitaufgelöster optischer Spektroskopie. Der Schwerpunkt liegt dabei auf Phononendynamik, die mithilfe von zeitaufgelöster Brillouin-Streuung sichtbar gemacht wird: durch die Anregung einer metallischen Transducer-Schicht mit einem ultrakurzen Anregepuls wird eine kohärente Phononendynamik im GHz Frequenzbereich erzeugt. Die Ausbreitung der Schallpulse wird mit einem Weißlicht-Abfragepuls aufgezeichnet. Diese Methode wird am Beispiel verschiedener Dünnschicht- und Übergitterproben illustriert. Die Methode und das gewonnene Verständnis wende ich an, um lineare und nichtlineare akustische Eigenschaften an einem SrTiO_3-Kristall zu untersuchen. Dieser weist einen ferroelastischen Phasenübergang von kubischer zu tetragonaler Kristallstruktur bei T_a=105 K auf. Im linearen Regime beobachte ich eine Kopplung der untersuchten akustischen Mode an eine weichwerdende optische Mode, welche den Phasenübergang charakterisiert. Im nichtlinearen Regime tritt eine gigantische Verlangsamung der Schallgeschwindigkeit unterhalb von T_a auf, wenn die induzierte Gitterverzerrung die Tetragonalität des Materials übersteigt. Dies kann auf eine Kopplung der hochfrequenten akustischen Mode an ferroelastische Domänenwände bei tiefen Temperaturen zurückgeführt werden. Ich entwickle einen neuen Mechanismus, der die Kopplung der Verzerrungswelle an die Domänenwände beschreibt. Eine detaillierte Untersuchung der Phononendämpfung in SrTiO_3 über einen weiten Temperaturbereich zeigt, dass diese bei tiefen Temperaturen durch die Domänenkonfiguration beeinflusst ist. Die Domänenkonfiguration ist durch Verzerrungen an der Kristall-Transducer Grenzfläche bestimmt. Erste Untersuchungen an magnetisch-ferroelektrischen Übergittern zeigen, dass die Anregungsfluenz vorsichtig eingestellt werden muss, um die Dynamik an Phasenübergängen zu untersuchen. KW - coherent phonons KW - phonon dynamics KW - time resolved KW - Brillouin scattering KW - perovskite oxides KW - optical spectroscopy KW - hypersound propagation KW - phonon damping KW - domain wall motion KW - phonon backfolding KW - superlattice dispersion KW - kohärente Phononen KW - Phononen Dynamik KW - zeitaufgelöst KW - Brillouin Streuung KW - Perowskit-Oxide KW - optische Spektroskopie KW - Hyperschall Propagation KW - Phononen Dämpfung KW - Domänenwandbewegung KW - Phononen Rückfaltung KW - Übergitter Dispersion Y1 - 2015 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-77623 ER - TY - JOUR A1 - Keles, Engin T1 - Spectral signature of atmospheric winds in high-resolution transit observations JF - Monthly Notices of the Royal Astronomical Society N2 - The study of exoplanet atmospheres showed large diversity compared to the planets in our Solar system. Especially Jupiter-type exoplanets orbiting their host star in close orbits, the so-called hot and ultra-hot Jupiters, have been studied in detail due to their enhanced atmospheric signature. Due to their tidally locked status, the temperature difference between the day- and nightside triggers atmospheric winds that can lead to various fingerprints in the observations. Spatially resolved absorption lines during transit such as sodium (Na) could be a good tracer for such winds. Different works resolved the Na absorption lines on different exoplanets which show different line widths. Assuming that this could be attributed to such zonal jet streams, this work models the effect of such winds on synthetic absorption lines. For this, transiting Jupiter-type planets with rotational velocities similar to hot and ultra-hot Jupiter are considered. The investigation shows that high wind velocities could reproduce the broadening of Na-line profiles inferred in different high-resolution transit observations. There is a tendency that the broadening values decrease for planets with lower equilibrium temperature. This could be explained by atmospheric drag induced by the ionization of alkali lines that slow down the zonal jet streams, favouring their existence on hot Jupiter rather than ultra-hot Jupiter. Y1 - 2021 U6 - https://doi.org/10.1093/mnras/stab099 VL - 502 IS - 1 SP - 1456 EP - 1468 PB - Oxford Univ. Press CY - Oxford ER - TY - JOUR A1 - Krapf, Diego A1 - Lukat, Nils A1 - Marinari, Enzo A1 - Metzler, Ralf A1 - Oshanin, Gleb A1 - Selhuber-Unkel, Christine A1 - Squarcini, Alessio A1 - Stadler, Lorenz A1 - Weiss, Matthias A1 - Xu, Xinran T1 - Spectral Content of a Single Non-Brownian Trajectory JF - Physical review : X, Expanding access N2 - Time-dependent processes are often analyzed using the power spectral density (PSD) calculated by taking an appropriate Fourier transform of individual trajectories and finding the associated ensemble average. Frequently, the available experimental datasets are too small for such ensemble averages, and hence, it is of a great conceptual and practical importance to understand to which extent relevant information can be gained from S(f, T), the PSD of a single trajectory. Here we focus on the behavior of this random, realization-dependent variable parametrized by frequency f and observation time T, for a broad family of anomalous diffusions-fractional Brownian motion with Hurst index H-and derive exactly its probability density function. We show that S(f, T) is proportional-up to a random numerical factor whose universal distribution we determine-to the ensemble-averaged PSD. For subdiffusion (H < 1/2), we find that S(f, T) similar to A/f(2H+1) with random amplitude A. In sharp contrast, for superdiffusion (H > 1/2) S(f, T) similar to BT2H-1/f(2) with random amplitude B. Remarkably, for H > 1/2 the PSD exhibits the same frequency dependence as Brownian motion, a deceptive property that may lead to false conclusions when interpreting experimental data. Notably, for H > 1/2 the PSD is ageing and is dependent on T. Our predictions for both sub-and superdiffusion are confirmed by experiments in live cells and in agarose hydrogels and by extensive simulations. KW - Biological Physics KW - Interdisciplinary Physics KW - Statistical Physics Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevX.9.011019 SN - 2160-3308 VL - 9 IS - 1 PB - American Physical Society CY - College Park ER - TY - GEN A1 - Finch, Nicolle L. A1 - Braker, I. P. A1 - Reindl, Nicole A1 - Barstow, Martin A. A1 - Casewell, Sarah L. A1 - Burleigh, M. A1 - Kupfer, Thomas A1 - Kilkenny, D. A1 - Geier, Stephan A1 - Schaffenroth, Veronika A1 - Bertolami Miller, Marcelo Miguel A1 - Taubenberger, Stefan A1 - Freudenthal, Joseph T1 - Spectral Analysis of Binary Pre-white Dwarf Systems T2 - Radiative signatures from the cosmos N2 - Short period double degenerate white dwarf (WD) binaries with periods of less than similar to 1 day are considered to be one of the likely progenitors of type Ia supernovae. These binaries have undergone a period of common envelope evolution. If the core ignites helium before the envelope is ejected, then a hot subdwarf remains prior to contracting into a WD. Here we present a comparison of two very rare systems that contain two hot subdwarfs in short period orbits. We provide a quantitative spectroscopic analysis of the systems using synthetic spectra from state-of-the-art non-LTE models to constrain the atmospheric parameters of the stars. We also use these models to determine the radial velocities, and thus calculate dynamical masses for the stars in each system. Y1 - 2019 SN - 978-1-58381-925-8 SN - 1050-3390 VL - 519 SP - 231 EP - 238 PB - Astronomical soc pacific CY - San Fransisco ER - TY - JOUR A1 - Bolotov, Maxim I. A1 - Smirnov, Lev A. A1 - Bubnova, E. S. A1 - Osipov, Grigory V. A1 - Pikovskij, Arkadij T1 - Spatiotemporal regimes in the Kuramoto-Battogtokh system of nonidentical oscillators JF - Journal of experimental and theoretical physics N2 - We consider the spatiotemporal states of an ensemble of nonlocally coupled nonidentical phase oscillators, which correspond to different regimes of the long-term evolution of such a system. We have obtained homogeneous, twisted, and nonhomogeneous stationary solutions to the Ott-Antonsen equations corresponding to key variants of the realized collective rotational motion of elements of the medium in question with nonzero mesoscopic characteristics determining the degree of coherence of the dynamics of neighboring particles. We have described the procedures of the search for the class of nonhomogeneous solutions as stationary points of the auxiliary point map and of determining the stability based on analysis of the eigenvalue spectrum of the composite operator. Static and breather cluster regimes have been demonstrated and described, as well as the regimes with an irregular behavior of averaged complex fields including, in particular, the local order parameter. Y1 - 2021 U6 - https://doi.org/10.1134/S1063776121010106 SN - 1063-7761 SN - 1090-6509 VL - 132 IS - 1 SP - 127 EP - 147 PB - Springer CY - Heidelberg [u.a.] ER - TY - GEN A1 - Mawass, Mohamad-Assaad A1 - Arora, Ashima A1 - Sandig, Oliver A1 - Luo, Chen A1 - Unal, Ahmet A. A1 - Radu, Florin A1 - Valencia, Sergio A1 - Kronast, Florian T1 - Spatially resolved investigation of all optical magnetization switching in TbFe alloys T2 - 2018 IEEE International Magnetics Conference (INTERMAG) N2 - High storage density magnetic devices rely on the precise, reliable and ultrafast switching times of the magnetic states. Optical control of magnetization using femtosecond laser without applying any external magnetic field offers the advantage of switching magnetic states at ultrashort time scales, which has attracted a significant attention. Recently, it has been reported and demonstrated the,so-called, all-optical helicity-dependent switching (AO-HDS) in which a circularly polarized femtosecond laser pulse switches the magnetization of a ferromagnetic thin film as function of laser helicity [1]. Afterward, in more recent studies, it has been reported that AO-HDS is a general phenomenon existing in magnetic materials ranging from rare earth - transition metals ferrimagnetic (e.g. alloys, multilayers and hetero-structures system) to even ferromagnetic thin films. Among numerous studies in the literature which are discussing the microscopic origin of AO-HDS in ferromagnets or ferrimagnetic alloys, the most renowned concepts are momentum transfer via Inverse Faraday Effect (IFE) [1-3]and the concept of preferential thermal demagnetization for one magnetization direction by heating close to Tc (Curie temperature) in the presence of magnetic circular dichroism (MCD) [4-6]. In this study, we investigate all-optical magnetic switching using a stationary femtosecond laser spot (3-5 μm) in TbFe alloys via photoemission electron microscopy (PEEM) and x-ray magnetic circular dichroism (XMCD) with a spatial resolution of approximately 30 nm. We spatially characterize the effect of laser heating and local temperature profile created across the laser spot on AO-HDS in TbFe thin films. We find that AO-HDS occurs only in a `ring' shaped region surrounding the thermally demagnetized region formed by the laser spot and the formation of switched domains relies further on thermally induced domain wall motion. Our temperature dependent measurements highlight the importance of attainin... Y1 - 2018 SN - 978-1-5386-6425-4 U6 - https://doi.org/10.1109/INTMAG.2018.8508211 PB - IEEE CY - New York ER - TY - JOUR A1 - Quade, Markus A1 - Abel, Markus A1 - Kutz, J. Nathan A1 - Brunton, Steven L. T1 - Sparse identification of nonlinear dynamics for rapid model recovery JF - Chaos : an interdisciplinary journal of nonlinear science N2 - Big data have become a critically enabling component of emerging mathematical methods aimed at the automated discovery of dynamical systems, where first principles modeling may be intractable. However, in many engineering systems, abrupt changes must be rapidly characterized based on limited, incomplete, and noisy data. Many leading automated learning techniques rely on unrealistically large data sets, and it is unclear how to leverage prior knowledge effectively to re-identify a model after an abrupt change. In this work, we propose a conceptual framework to recover parsimonious models of a system in response to abrupt changes in the low-data limit. First, the abrupt change is detected by comparing the estimated Lyapunov time of the data with the model prediction. Next, we apply the sparse identification of nonlinear dynamics (SINDy) regression to update a previously identified model with the fewest changes, either by addition, deletion, or modification of existing model terms. We demonstrate this sparse model recovery on several examples for abrupt system change detection in periodic and chaotic dynamical systems. Our examples show that sparse updates to a previously identified model perform better with less data, have lower runtime complexity, and are less sensitive to noise than identifying an entirely new model. The proposed abrupt-SINDy architecture provides a new paradigm for the rapid and efficient recovery of a system model after abrupt changes. Y1 - 2018 U6 - https://doi.org/10.1063/1.5027470 SN - 1054-1500 SN - 1089-7682 VL - 28 IS - 6 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Wang, Jingwen A1 - Rychkov, Dmitry A1 - Gerhard, Reimund T1 - Space-charge electret properties of polypropylene films with transcrystalline or spherulitic structures BT - a comparison of functionalities at interfaces JF - Journal of applied physics : AIP's archival journal for significant new results in applied physics / publ. by the American Institute of Physics N2 - Spherulite-related space-charge electret properties of polypropylene (PP) have been widely discussed in the past decades. In the present paper, a less-common crystalline structure in PP-transcrystalline PP-is studied regarding its electret behavior in comparison with the typical spherulitic morphology. Polarized light microscopy and differential scanning calorimetry were employed to characterize the crystallite types and crystallinities of transcrystalline and spherulitic PP. Their electret functionality is investigated by means of thermally stimulated discharge experiments, where the cross-over phenomenon is observed on transcrystalline PP films, whereas surface-potential saturation and undercharging on the surface occur on the spherulitic samples. Besides, an asymmetrical behavior of positive and negative surface-charge stabilities is found on PP with spherulites, the negatively charged spherulitic surfaces show a better charge stability. It is shown that PP electrets are very sensitive to changes in the microscopic crystalline structures and their interfaces as well as in the molecular conformations controlled through adjustments of the respective processing steps. In addition, surface and bulk nanocomposites of PP or low-density polyethylene with inorganic particles are included in the comparison. In view of recent developments in the areas of PP-based electret-fiber filters and cellular-foam ferroelectrets, the observed changes in the charge-storage properties may have particular relevance, as the required film, fiber, or foam processing might significantly modify crystalline morphologies and nano-scale interfaces in PP electrets. Limitations in the charge-storage capabilities of interface structures may also be of interest in the context of high-voltage electrical-insulation materials where reduced space-charge accumulation and slightly increased charge transport can be advantageous. Y1 - 2021 U6 - https://doi.org/10.1063/5.0039867 SN - 0021-8979 SN - 1089-7550 VL - 129 IS - 6 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Silanteva, Irina A. A1 - Komolkin, Andrei A1 - Mamontova, Veronika V. A1 - Vorontsov-Velyaminov, Pavel N. A1 - Santer, Svetlana A1 - Kasyanenko, Nina A. T1 - Some features of surfactant organization in DNA solutions at various NaCl concentrations JF - ACS omega / American Chemical Society N2 - The photosensitive azobenzene-containing surfactant C-4-Azo-OC(6)TMAB is a promising agent for reversible DNA packaging in a solution. The simulation of the trans-isomer surfactant organization into associates in a solution with and without salt as well as its binding to DNA at different NaCl concentrations was carried out by molecular dynamics. Experimental data obtained by spectral and hydrodynamic methods were used to verify the results of simulation. It was shown that head-to-tail aggregates with close to antiparallel orientation of surfactant molecules were formed at certain NaCl and surfactant concentrations (below critical micelle concentration). Such aggregates have two positively charged ends, and therefore, they can be attracted to negatively charged DNA phosphates far located along the chain, as well as those that belong to different molecules. This contributes to the formation of intermolecular DNA-DNA contacts, and this way, the experimentally observed precipitation of DNA can be explained. Y1 - 2020 U6 - https://doi.org/10.1021/acsomega.0c01850 SN - 2470-1343 VL - 5 IS - 29 SP - 18234 EP - 18243 PB - ACS Publications CY - Washington ER - TY - JOUR A1 - Letellier, Christophe A1 - Abraham, Ralph A1 - Shepelyansky, Dima L. A1 - Rossler, Otto E. A1 - Holmes, Philip A1 - Lozi, Rene A1 - Glass, Leon A1 - Pikovsky, Arkady A1 - Olsen, Lars F. A1 - Tsuda, Ichiro A1 - Grebogi, Celso A1 - Parlitz, Ulrich A1 - Gilmore, Robert A1 - Pecora, Louis M. A1 - Carroll, Thomas L. T1 - Some elements for a history of the dynamical systems theory JF - Chaos : an interdisciplinary journal of nonlinear science N2 - Writing a history of a scientific theory is always difficult because it requires to focus on some key contributors and to "reconstruct" some supposed influences. In the 1970s, a new way of performing science under the name "chaos" emerged, combining the mathematics from the nonlinear dynamical systems theory and numerical simulations. To provide a direct testimony of how contributors can be influenced by other scientists or works, we here collected some writings about the early times of a few contributors to chaos theory. The purpose is to exhibit the diversity in the paths and to bring some elements-which were never published-illustrating the atmosphere of this period. Some peculiarities of chaos theory are also discussed. Y1 - 2021 U6 - https://doi.org/10.1063/5.0047851 SN - 1054-1500 SN - 1089-7682 VL - 31 IS - 5 PB - AIP Publishing CY - Melville ER - TY - JOUR A1 - Jelken, Joachim A1 - Henkel, Carsten A1 - Santer, Svetlana T1 - Solving an old puzzle: fine structure of diffraction spots from an azo-polymer surface relief grating JF - Applied physics : B, Lasers and optics N2 - We report on the experimental and theoretical interpretation of the diffraction of a probe beam during inscription of a surface relief grating with an interference pattern into a photo-responsive polymer film. For this, we developed a set-up allowing for the simultaneous recording of the diffraction efficiency (DE), the fine structure of the diffraction spot and the topographical changes, in situ and in real time while the film is irradiated. The time dependence of the DE, as the surface relief deepens, follows a Bessel function exhibiting maxima and minima. The size of the probe beam relative to the inscribed grating (i.e., to the size of the writing beams) matters and has to be considered for the interpretation of the DE signal. It is also at the origin of a fine structure within the diffraction spot where ring-shaped features appear once an irradiation time corresponding to the first maximum of the DE has been exceeded. Y1 - 2019 U6 - https://doi.org/10.1007/s00340-019-7331-8 SN - 0946-2171 SN - 1432-0649 VL - 125 IS - 11 PB - Springer CY - Heidelberg ER - TY - JOUR A1 - Smirnov, Lev A. A1 - Osipov, Grigory V. A1 - Pikovskij, Arkadij T1 - Solitary synchronization waves in distributed oscillator populations JF - Physical review : E, Statistical, nonlinear and soft matter physics N2 - We demonstrate the existence of solitary waves of synchrony in one-dimensional arrays of oscillator populations with Laplacian coupling. Characterizing each community with its complex order parameter, we obtain lattice equations similar to those of the discrete nonlinear Schrodinger system. Close to full synchrony, we find solitary waves for the order parameter perturbatively, starting from the known phase compactons and kovatons; these solutions are extended numerically to the full domain of possible synchrony levels. For nonidentical oscillators, the existence of dissipative solitons is shown. Y1 - 2018 U6 - https://doi.org/10.1103/PhysRevE.98.062222 SN - 2470-0045 SN - 2470-0053 VL - 98 IS - 6 SP - 062222-1 EP - 062222-7 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Teichmann, Erik A1 - Rosenblum, Michael T1 - Solitary states and partial synchrony in oscillatory ensembles with attractive and repulsive interactions JF - Chaos : an interdisciplinary journal of nonlinear science N2 - We numerically and analytically analyze transitions between different synchronous states in a network of globally coupled phase oscillators with attractive and repulsive interactions. The elements within the attractive or repulsive group are identical, but natural frequencies of the groups differ. In addition to a synchronous two-cluster state, the system exhibits a solitary state, when a single oscillator leaves the cluster of repulsive elements, as well as partially synchronous quasiperiodic dynamics. We demonstrate how the transitions between these states occur when the repulsion starts to prevail over attraction. Y1 - 2019 U6 - https://doi.org/10.1063/1.5118843 SN - 1054-1500 SN - 1089-7682 VL - 29 IS - 9 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Rosenau, Philip A1 - Pikovskij, Arkadij T1 - Solitary phase waves in a chain of autonomous oscillators JF - Chaos : an interdisciplinary journal of nonlinear science N2 - In the present paper, we study phase waves of self-sustained oscillators with a nearest-neighbor dispersive coupling on an infinite lattice. To analyze the underlying dynamics, we approximate the lattice with a quasi-continuum (QC). The resulting partial differential model is then further reduced to the Gardner equation, which predicts many properties of the underlying solitary structures. Using an iterative procedure on the original lattice equations, we determine the shapes of solitary waves, kinks, and the flat-like solitons that we refer to as flatons. Direct numerical experiments reveal that the interaction of solitons and flatons on the lattice is notably clean. All in all, we find that both the QC and the Gardner equation predict remarkably well the discrete patterns and their dynamics. Y1 - 2020 U6 - https://doi.org/10.1063/1.5144939 SN - 1054-1500 SN - 1089-7682 VL - 30 IS - 5 PB - American Institute of Physics, AIP CY - Melville, NY ER - TY - JOUR A1 - Vafin, Sergei A1 - Lazar, M. A1 - Fichtner, H. A1 - Schlickeiser, R. A1 - Drillisch, M. T1 - Solar wind temperature anisotropy constraints from streaming instabilities JF - Astronomy and astrophysics : an international weekly journal N2 - Due to the relatively low rate of particle-particle collisions in the solar wind, kinetic instabilities (e.g., the mirror and firehose) play an important role in regulating large deviations from temperature isotropy. These instabilities operate in the high beta(parallel to) > 1 plasmas, and cannot explain the other limits of the temperature anisotropy reported by observations in the low beta beta(parallel to) < 1 regimes. However, the instability conditions are drastically modified in the presence of streaming (or counterstreaming) components, which are ubiquitous in space plasmas. These effects have been analyzed for the solar wind conditions in a large interval of heliospheric distances, 0.3-2.5 AU. It was found that proton counter-streams are much more crucial for plasma stability than electron ones. Moreover, new instability thresholds can potentially explain all observed bounds on the temperature anisotropy, and also the level of differential streaming in the solar wind. KW - solar wind KW - instabilities KW - waves KW - turbulence Y1 - 2018 U6 - https://doi.org/10.1051/0004-6361/201731852 SN - 1432-0746 VL - 613 PB - EDP Sciences CY - Les Ulis ER - TY - THES A1 - Stoyanov, Hristiyan T1 - Soft nanocomposites with enhanced electromechanical response for dielectric elastomer actuators T1 - Elastomer-Nanokomposite mit erhöhter elektro-mechanischer Sensitivität für dielektrische Elastomer Aktoren N2 - Electromechanical transducers based on elastomer capacitors are presently considered for many soft actuation applications, due to their large reversible deformation in response to electric field induced electrostatic pressure. The high operating voltage of such devices is currently a large drawback, hindering their use in applications such as biomedical devices and biomimetic robots, however, they could be improved with a careful design of their material properties. The main targets for improving their properties are increasing the relative permittivity of the active material, while maintaining high electric breakdown strength and low stiffness, which would lead to enhanced electrostatic storage ability and hence, reduced operating voltage. Improvement of the functional properties is possible through the use of nanocomposites. These exploit the high surface-to-volume ratio of the nanoscale filler, resulting in large effects on macroscale properties. This thesis explores several strategies for nanomaterials design. The resulting nanocomposites are fully characterized with respect to their electrical and mechanical properties, by use of dielectric spectroscopy, tensile mechanical analysis, and electric breakdown tests. First, nanocomposites consisting of high permittivity rutile TiO2 nanoparticles dispersed in thermoplastic block copolymer SEBS (poly-styrene-coethylene-co-butylene-co-styrene) are shown to exhibit permittivity increases of up to 3.7 times, leading to 5.6 times improvement in electrostatic energy density, but with a trade-off in mechanical properties (an 8-fold increase in stiffness). The variation in both electrical and mechanical properties still allows for electromechanical improvement, such that a 27 % reduction of the electric field is found compared to the pure elastomer. Second, it is shown that the use of nanofiller conductive particles (carbon black (CB)) can lead to a strong increase of relative permittivity through percolation, however, with detrimental side effects. These are due to localized enhancement of the electric field within the composite, which leads to sharp reductions in electric field strength. Hence, the increase in permittivity does not make up for the reduction in breakdown strength in relation to stored electrical energy, which may prohibit their practical use. Third, a completely new approach for increasing the relative permittivity and electrostatic energy density of a polymer based on 'molecular composites' is presented, relying on chemically grafting soft π-conjugated macromolecules to a flexible elastomer backbone. Polarization caused by charge displacement along the conjugated backbone is found to induce a large and controlled permittivity enhancement (470 % over the elastomer matrix), while chemical bonding, encapsulates the PANI chains manifesting in hardly any reduction in electric breakdown strength, and hence resulting in a large increase in stored electrostatic energy. This is shown to lead to an improvement in the sensitivity of the measured electromechanical response (83 % reduction of the driving electric field) as well as in the maximum actuation strain (250 %). These results represent a large step forward in the understanding of the strategies which can be employed to obtain high permittivity polymer materials with practical use for electro-elastomer actuation. N2 - Die Palette von elektro-mechanischen Aktuatoren, basierend auf dem Prinzip weicher dehnbarer Kondensatoren, scheint besonders für Anwendungen in der Medizin und für biomimetische Applikationen unbegrenzt. Diese Wandler zeichnen sich sowohl durch hohe Reversibilität bei großer mechanischer Deformation als auch durch ihre Flexibilität aus, wobei die mechanischen Deformationen durch elektrische Felder induziert werden. Die Notwendigkeit von hoher elektrischer Spannung zur Erzeugung dieser mechanischen Deformationen verzögert jedoch die technisch einfache und breite Markteinführung dieser Technologie. Diesem Problem kann durch eine gezielte Materialmodifikation begegnet werden. Eine Modifikation hat das Ziel, die relative Permittivität zu erhöhen, wobei die Flexibilität und die hohe elektrische Durchbruchsfeldstärke beibehalten werden sollten. Durch eine Materialmodifikation kann die Energiedichte des Materials bedeutend erhöht und somit die notwendige Betriebsspannung des Aktuators herabgesetzt werden. Eine Verbesserung der funktionalen Materialeigenschaften kann durch die Verwendung von Nanokompositen erzielt werden, welche die fundamentalen Eigenschaften der Nanopartikel, d.h. ein gutes Verhältnis von Oberfläche zu Volumen nutzen, um eine gezielte makroskopische Materialmodifikation zu bewirken. Diese Arbeit behandelt die Anwendung innovativer Strategien für die Erzeugung von Nanomaterialien mit hoher Permittivität. Die so erzeugten Materialien und deren relevante Aktuatorkenngrößen werden durch elektrische und mechanische Experimente vollständig erfasst. Mittels der klassischen Mischansätze zur Erzeugung von Kompositmaterialen mit hoher Permittivität konnte durch nichtleitendes Titaniumdioxid TiO2 (Rutile) in einem Thermoplastischen-Block-Co-Polymer SEBS (poly-styrene-co-ethylene-cobutylene-co-styrene) die Permittivität bereits um 370 % erhöht und die elektrische Energiedichte um 570 % gesteigert werden. Diese Veränderungen führten jedoch zu einem signifikanten Anstieg der Steifigkeit des Materials. Aufgrund der positiven Rückkopplung von elektrischen und mechanischen Eigenschaften des Kompositmaterials ermöglicht bereits dieser einfache Ansatz eine Verbesserung der Aktuation, bei einer 27 %-igen Reduktion der Aktuatorbetriebsspannung. Eine direkte Verwendung von leitfähigen Nanopartikeln kann ebenso zu einem Anstieg der relativen Permittivität beitragen, wobei jedoch die Leitfähigkeit dieser Nanopartikel bedeutende Wechselwirkungen verursacht, welche somit die Energiedichte des Materials negativ beeinflusst und die praktische Verwendung dieses Kompositsystems ausschließt. Als ein völlig neuer Ansatz zur Steigerung der relativen Permittivität und Energiedichte und abweichend vom klassischen Mischverfahren, wird die Herstellung eines "Molekularen Komposits", basierend auf einem chemischen Propfverfahren, präsentiert. In diesem Ansatz wird ein π-konjugiertes leitfähiges Polymer (PANI) an die Hauptkette des Elastomers der Polymermatrix gebunden. Die daraus resultierende Ladungsverteilung entlang der Elastomerhauptkette bewirkt eine 470 %-ige Steigerung der Permittivität des "Molekularen Komposits" im Vergleich zur Permittivität des unbehandelten Elastomermaterials. Aufgrund der Verkapselung der chemischen Bindungen der PANI-Kette entstehen kaum negative Rückwirkungen auf die elektrischen und mechanischen Eigenschaften des so erzeugten Komposits. Diese Materialeigenschaften resultieren in einem signifikanten Anstieg der Energiedichte des Materials. Das mittels dieses Verfahrens erzeugte Komposit zeigt sowohl eine Steigerung der Sensitivität der elektromechanischen Antwort (Reduktion des elektrischen Felds um 83 %) als auch eine bedeutende Steigerung der maximalen Aktuation (250 %). Die Ergebnisse und Ideen dieser Arbeit stellen einen wesentlichen Sprung im Verständnis zur Permittivitätssteigerung in Polymermaterialien dar und werden deshalb in der Erforschung und Entwicklung von Elastomeraktuatoren Beachtung finden. KW - dielektrische Elastomere KW - Nanokomposite KW - hohe Permittivität KW - elektrostatische Energiedichte KW - elektromechanische Reaktion KW - dielectric elastomers KW - nanocomposites KW - high permittivity KW - electrostatic energy density KW - electromechanical response Y1 - 2011 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus-51194 ER - TY - JOUR A1 - Stete, Felix A1 - Schossau, Phillip A1 - Bargheer, Matias A1 - Koopman, Wouter-Willem Adriaan T1 - Size-Dependent coupling of Hybrid Core-Shell Nanorods BT - Toward Single-Emitter Strong-Coupling JF - The journal of physical chemistry : C, Nanomaterials and interfaces N2 - Owing to their ability of concentrating electromagnetic fields to subwavelength mode volumes, plasmonic nanoparticles foster extremely high light-matter coupling strengths reaching far into the strong-coupling regime of light matter interaction. In this article, we present an experimental investigation on the dependence of coupling strength on the geometrical size of the nanoparticle. The coupling strength for differently sized hybrid plasmon-core exciton-shell nanorods was extracted from the typical resonance anticrossing of these systems, obtained by controlled modification of the environment permittivity using layer-by-layer deposition of polyelectrolytes. The observed size dependence of the coupling strength can be explained by a simple model approximating the electromagnetic mode volume by the geometrical volume of the particle. On the basis of this model, the coupling strength for particles of arbitrary size can be predicted, including the particle size necessary to support single-emitter strong coupling. Y1 - 2018 U6 - https://doi.org/10.1021/acs.jpcc.8b04204 SN - 1932-7447 VL - 122 IS - 31 SP - 17976 EP - 17982 PB - American Chemical Society CY - Washington ER - TY - GEN A1 - Stete, Felix A1 - Schossau, Phillip Gerald A1 - Koopman, Wouter-Willem Adriaan A1 - Bargheer, Matias T1 - Size Dependence of the Coupling Strength in Plasmon-Exciton Nanoparticles T2 - Quantum Nano-Photonics N2 - The coupling between molecular excitations and nanoparticles leads to promising applications. It is for example used to enhance the optical cross-section of molecules in surface enhanced Raman scattering, Purcell enhancement or plasmon enhanced dye lasers. In a coupled system new resonances emerge resulting from the original plasmon (ωpl) and exciton (ωex) resonances as ω±=12(ωpl+ωex)±14(ωpl−ωex)2+g2−−−−−−−−−−−−−−−√, (1) where g is the coupling parameter. Hence, the new resonances show a separation of Δ = ω+ − ω− from which the coupling strength can be deduced from the minimum distance between the two resonances, Ω = Δ(ω+ = ω−). Y1 - 2018 SN - 978-94-024-1546-9 SN - 978-94-024-1544-5 SN - 978-94-024-1543-8 U6 - https://doi.org/10.1007/978-94-024-1544-5_26 SN - 1871-465X SP - 381 EP - 383 PB - Springer CY - Dordrecht ER - TY - INPR A1 - Pikovskij, Arkadij A1 - Zaks, Michael A. A1 - Feudel, Ulrike A1 - Kurths, Jürgen T1 - Singular continuous spectra in dissipative dynamics N2 - We demonstrate the occurrence of regimes with singular continuous (fractal) Fourier spectra in autonomous dissipative dynamical systems. The particular example in an ODE system at the accumulation points of bifurcation sequences associated to the creation of complicated homoclinic orbits. Two different machanisms responsible for the appearance of such spectra are proposed. In the first case when the geometry of the attractor is symbolically represented by the Thue-Morse sequence, both the continuous-time process and its descrete Poincaré map have singular power spectra. The other mechanism owes to the logarithmic divergence of the first return times near the saddle point; here the Poincaré map possesses the discrete spectrum, while the continuous-time process displays the singular one. A method is presented for computing the multifractal characteristics of the singular continuous spectra with the help of the usual Fourier analysis technique. T3 - NLD Preprints - 15 Y1 - 1995 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus-13787 ER - TY - GEN A1 - Sposini, Vittoria A1 - Metzler, Ralf A1 - Oshanin, Gleb T1 - Single-trajectory spectral analysis of scaled Brownian motion T2 - Postprints der Universität Potsdam Mathematisch-Naturwissenschaftliche Reihe N2 - Astandard approach to study time-dependent stochastic processes is the power spectral density (PSD), an ensemble-averaged property defined as the Fourier transform of the autocorrelation function of the process in the asymptotic limit of long observation times, T → ∞. In many experimental situations one is able to garner only relatively few stochastic time series of finite T, such that practically neither an ensemble average nor the asymptotic limit T → ∞ can be achieved. To accommodate for a meaningful analysis of such finite-length data we here develop the framework of single-trajectory spectral analysis for one of the standard models of anomalous diffusion, scaled Brownian motion.Wedemonstrate that the frequency dependence of the single-trajectory PSD is exactly the same as for standard Brownian motion, which may lead one to the erroneous conclusion that the observed motion is normal-diffusive. However, a distinctive feature is shown to be provided by the explicit dependence on the measurement time T, and this ageing phenomenon can be used to deduce the anomalous diffusion exponent.Wealso compare our results to the single-trajectory PSD behaviour of another standard anomalous diffusion process, fractional Brownian motion, and work out the commonalities and differences. Our results represent an important step in establishing singletrajectory PSDs as an alternative (or complement) to analyses based on the time-averaged mean squared displacement. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 753 KW - diffusion KW - anomalous diffusion KW - power spectral analysis KW - single trajectory analysis Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-436522 SN - 1866-8372 IS - 753 ER - TY - JOUR A1 - Sposini, Vittoria A1 - Metzler, Ralf A1 - Oshanin, Gleb T1 - Single-trajectory spectral analysis of scaled Brownian motion JF - New Journal of Physics N2 - Astandard approach to study time-dependent stochastic processes is the power spectral density (PSD), an ensemble-averaged property defined as the Fourier transform of the autocorrelation function of the process in the asymptotic limit of long observation times, T → ∞. In many experimental situations one is able to garner only relatively few stochastic time series of finite T, such that practically neither an ensemble average nor the asymptotic limit T → ∞ can be achieved. To accommodate for a meaningful analysis of such finite-length data we here develop the framework of single-trajectory spectral analysis for one of the standard models of anomalous diffusion, scaled Brownian motion.Wedemonstrate that the frequency dependence of the single-trajectory PSD is exactly the same as for standard Brownian motion, which may lead one to the erroneous conclusion that the observed motion is normal-diffusive. However, a distinctive feature is shown to be provided by the explicit dependence on the measurement time T, and this ageing phenomenon can be used to deduce the anomalous diffusion exponent.Wealso compare our results to the single-trajectory PSD behaviour of another standard anomalous diffusion process, fractional Brownian motion, and work out the commonalities and differences. Our results represent an important step in establishing singletrajectory PSDs as an alternative (or complement) to analyses based on the time-averaged mean squared displacement. KW - diffusion KW - anomalous diffusion KW - power spectral analysis KW - single trajectory analysis Y1 - 2019 U6 - https://doi.org/10.1088/1367-2630/ab2f52 SN - 1367-2630 VL - 21 PB - Deutsche Physikalische Gesellschaft ; IOP, Institute of Physics CY - Bad Honnef und London ER - TY - JOUR A1 - Raoufi, Meysam A1 - Hörmann, Ulrich A1 - Ligorio, Giovanni A1 - Hildebrandt, Jana A1 - Pätzel, Michael A1 - Schultz, Thorsten A1 - Perdigón-Toro, Lorena A1 - Koch, Norbert A1 - List-Kratochvil, Emil A1 - Hecht, Stefan A1 - Neher, Dieter T1 - Simultaneous effect of ultraviolet radiation and surface modification on the work function and hole injection properties of ZnO thin films JF - Physica Status Solidi. A , Applications and materials science N2 - The combined effect of ultraviolet (UV) light soaking and self-assembled monolayer deposition on the work function (WF) of thin ZnO layers and on the efficiency of hole injection into the prototypical conjugated polymer poly(3-hexylthiophen-2,5-diyl) (P3HT) is systematically investigated. It is shown that the WF and injection efficiency depend strongly on the history of UV light exposure. Proper treatment of the ZnO layer enables ohmic hole injection into P3HT, demonstrating ZnO as a potential anode material for organic optoelectronic devices. The results also suggest that valid conclusions on the energy-level alignment at the ZnO/organic interfaces may only be drawn if the illumination history is precisely known and controlled. This is inherently problematic when comparing electronic data from ultraviolet photoelectron spectroscopy (UPS) measurements carried out under different or ill-defined illumination conditions. KW - charge injection across hybrid interfaces KW - energy-level alignments KW - hybrid metal oxides KW - organic interfaces Y1 - 2020 U6 - https://doi.org/10.1002/pssa.201900876 SN - 1862-6300 SN - 1862-6319 VL - 217 IS - 5 SP - 1 EP - 6 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Castillo, Angelica M. A1 - Shprits, Yuri A1 - Ganushkina, Natalia A1 - Drozdov, Alexander A1 - Aseev, Nikita A1 - Wang, Dedong A1 - Dubyagin, Stepan T1 - Simulations of the inner magnetospheric energetic electrons using the IMPTAM-VERB coupled model JF - Journal of Atmospheric and Solar-Terrestrial Physics N2 - In this study, we present initial results of the coupling between the Inner Magnetospheric Particle Transport and Acceleration Model (IMPTAM) and the Versatile Electron Radiation Belt (VERB-3D) code. IMPTAM traces electrons of 10-100 keV energies from the plasma sheet (L = 9 Re) to inner L-shell regions. The flux evolution modeled by IMPTAM is used at the low energy and outer L* computational boundaries of the VERB code (assuming a dipole approximation) to perform radiation belt simulations of energetic electrons. The model was tested on the March 17th, 2013 storm, for a six-day period. Four different simulations were performed and their results compared to satellites observations from Van Allen probes and GOES. The coupled IMPTAM-VERB model reproduces evolution and storm-time features of electron fluxes throughout the studied storm in agreement with the satellite data (within similar to 0.5 orders of magnitude). Including dynamics of the low energy population at L* = 6.6 increases fluxes closer to the heart of the belt and has a strong impact in the VERB simulations at all energies. However, inclusion of magnetopause losses leads to drastic flux decreases even below L* = 3. The dynamics of low energy electrons (max. 10s of keV) do not affect electron fluxes at energies >= 900 keV. Since the IMPTAM-VERB coupled model is only driven by solar wind parameters and the Dst and Kp indexes, it is suitable as a forecasting tool. In this study, we demonstrate that the estimation of electron dynamics with satellite-data-independent models is possible and very accurate. KW - Electron populations KW - Radiation belts KW - IMPTAM KW - VERB Y1 - 2019 U6 - https://doi.org/10.1016/j.jastp.2019.05.014 SN - 1364-6826 SN - 1879-1824 VL - 191 PB - Elsevier CY - Oxford ER - TY - THES A1 - Uyaver, Sahin T1 - Simulation of annealed polyelectrolytes in poor solvents N2 - Polymere sind lange kettenartige Moleküle. Sie bestehen aus vielen elementaren chemischen Einheiten, den Monomeren, die durch kovalente Bindungen aneinander gekettet sind. Polyelektrolyte sind Polymere, die ionisierbare Monomeren enthalten. Aufgrund ihrer speziellen Eigenschaften sind Polyelektrolyte sowohl in der Molekular- und Zellbiologie von großen Bedeutung als auch in der Chemie großtechnisch relevant. Verglichen mit ungeladenen Polymeren sind Polyelektrolyte theoretisch noch wenig verstanden. Insbesondere gilt dies für Polyelektrolyte in sogenanntem schlechten Lösungsmittel. Ein schlechtes Lösungsmittel bewirkt eine effektive Anziehung zwischen den Monomeren. Für Polyelektrolyte in schlechtem Lösungsmittel kommt es daher zu einer Konkurrenz zwischen dieser Anziehung und der elektrostatischen Abstoßung. Geladene Polymere werden im Rahmen der chemischen Klassifikation in starke und schwache Polyelektrolyte unterschieden. Erstere zeigen vollständige Dissoziation unabhängig vom pH-Wert der Lösung. Die Position der Ladungen auf der Kette wird ausschließlich während der Polymersynthese festgelegt. In der Physik spricht man deshalb von Polyelektrolyten mit eingefrorener Ladungsverteilung (quenched polyelectrolytes). Im Falle von schwachen Polyelektrolyten ist die Ladungsdichte auf der Kette nicht konstant, sondern wird durch der pH-Wert der Lösung kontrolliert. Durch Rekombinations- und Dissoziationsprozesse sind die Ladungen auf der Kette beweglich. Im allgemeinen stellt sich eine inhomogene Gleichgewichtsverteilung ein, die mit der Struktur der Kette gekoppelt ist. Diese Polymere werden deshalb auch Polyelektrolyte mit Gleichgewichtsladungsverteilung (annealed polyelectrolytes) genannt. Wegen des zusätzlichen Freiheitsgrades in der Ladungsverteilung werden eine Reihe ungewöhnlicher Eigenschaften theoretisch vorhergesagt. Mit Hilfe von Simulationen ist es zum ersten Mal gelungen, zu zeigen daß 'annealed' Polyelektrolyte in relativ schlechtem Lösungsmittel einen diskontinuierlichen Phasenübergang durchlaufen, wenn ein kritischer pH-Werts der Lösung überschritten wird. Bei diesem Phasenübergang, gehen die Polyelektolyte von einer schwach geladenen kompakten globulären Struktur zu einer stark geladenen gestreckten Konfiguration über. Aufgrund theoretischer Vorhersagen wird erwartet, daß die globuläre Struktur in weniger schlechtem Lösungsmittel instabil wird und sich eine Perlenkettenkonfiguration ausbildet. Diese Vorhersage konnte für 'annealed' Polyelektrolyte mit den durchgeführten Simulationen zum ersten Mal bestätigt werden - inzwischen auch durch erste experimentelle Ergebnisse. Schließlich zeigen die Simulationen auch, daß annealed Polyelektrolyte bei einer kritischen Salzkonzentration in der Lösung einen scharfen Übergang zwischen einem stark geladenen gestreckten Zustand und einem schwach geladenen globulären Zustand aufweisen, wiederum in Übereinstimmung mit theoretischen Erwartungen. N2 - A polymer is a large molecule made up of many elementary chemical units, joined together by covalent bonds (for example, polyethylene). Polyelectrolytes (PELs) are polymer chains containing a certain amount of ionizable monomers. With their specific properties PELs acquire big importance in molecular and cell biology as well as in technology. Compared to neutral polymers the theory of PELs is less understood. In particular, this is valid for PELs in poor solvents. A poor solvent environment causes an effective attraction between monomers. Hence, for PELs in a poor solvent, there occurs a competition between attraction and repulsion. Strong or quenched PELs are completely dissociated at any accessible pH. The position of charges along the chain is fixed by chemical synthesis. On the other hand, in weak or annealed PELs dissociation of charges depends on solution pH. For the first time the simulation results have given direct evidence that at rather poor solvents an annealed PEL indeed undergoes a first-order phase transition when the chemical potential (solution pH) reaches at a certain value. The discontinuous transition occurs between a weakly charged compact globular structure and a strongly charged stretched configuration. At not too poor solvents theory predicts that globule would become unstable with respect to the formation of pearl-necklaces. The results show that pearl-necklaces exist in annealed PELs indeed. Furthermore, as predicted by theory, the simulation results have shown that annealed PELs display a sharp transition from a highly charged stretched state to a weakly charged globule at a critical salt concentration. KW - Polymer-Plastik KW - Polyelektrolyte KW - Simulation KW - polymer KW - polyelectrolytes KW - simulation Y1 - 2004 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-0001488 ER - TY - JOUR A1 - Eberhard, Julius A1 - Schaik, N. Loes M. B. A1 - Schibalski, Anett A1 - Gräff, Thomas T1 - Simulating future salinity dynamics in a coastal marshland under different climate scenarios JF - Vadose zone journal N2 - Salinization is a well-known problem in agricultural areas worldwide. In the last 20-30 yr, rising salinity in the upper, unconfined aquifer has been observed in the Freepsumer Meer, a grassland near the German North Sea coast. For investigating long-term development of salinity and water balance during 1961-2099, the one-dimensional Soil-Water-Atmosphere-Plant (SWAP) model was set up and calibrated for a soil column in the area. The model setup involves a deep aquifer as the source of salt through upward seepage. In the vertical salt transport equation, dispersion and advection are included. Six different regional outputs of statistical downscaling methods were used as climate scenarios. These comprise different rates of increasing surface temperature and different trends in seasonal rainfall. The simulation results exhibit opposing salinity trends for topsoil and deeper layers. Although projections of some scenarios entail decreasing salinities near the surface, most of them project a rise in subsoil salinity, with the strongest trends of up to +0.9 mg cm(-3) 100 yr(-1) at -65 cm. The results suggest that topsoil salinity trends in the study area are affected by the magnitude of winter rainfall trends, whereas high subsoil salinities correspond to low winter rainfall and high summer temperature. How these projected trends affect the vegetation and thereby future land use will depend on the future management of groundwater levels in the area. Y1 - 2020 U6 - https://doi.org/10.1002/vzj2.20008 SN - 1539-1663 VL - 19 IS - 1 PB - Wiley CY - Hoboken ER -