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- van Hoof, Peter A. M. (1)
- van Roestel, Jan (1)
- van Turnhout, Jan (1)
- van der Wale, D. J. (1)
- von Nordheim, Danny (1)
- von Zander, Robert Edler (1)
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- Doctoral Thesis (379)
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- diffusion (47)
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- Institut für Physik und Astronomie (1524)
- Interdisziplinäres Zentrum für Dynamik komplexer Systeme (52)
- Institut für Chemie (46)
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- Mathematisch-Naturwissenschaftliche Fakultät (25)
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- Institut für Umweltwissenschaften und Geographie (7)
- Potsdam Institute for Climate Impact Research (PIK) e. V. (6)
This publication based thesis, which consists of seven published articles, summarizes my contributions to the research field of laser excited ultrafast structural dynamics. The coherent and incoherent lattice dynamics on microscopic length scales are detected by ultrashort optical and X-ray pulses. The understanding of the complex physical processes is essential for future improvements of technological applications. For this purpose, tabletop soruces and large scale facilities, e.g. synchrotrons, are employed to study structural dynamics of longitudinal acoustic strain waves and heat transport. The investigated effects cover timescales from hundreds of femtoseconds up to several microseconds.
The main part of this thesis is dedicated to the investigation of tailored phonon wave packets propagating in perovskite nanostructures. Tailoring is achieved either by laser excitation of nanostructured bilayer samples or by a temporal series of laser pulses. Due to the propagation of longitudinal acoustic phonons, the out-of-plane lattice spacing of a thin film insulator-metal bilayer sample is modulated on an ultrafast timescale. This leads to an ultrafast modulation of the X-ray diffraction efficiency which is employed as a phonon Bragg switch to shorten hard X-ray pulses emitted from a 3rd generation synchrotron.
In addition, we have observed nonlinear mixing of high amplitude phonon wave packets which originates from an anharmonic interatomic potential. A chirped optical pulse sequence excites a narrow band phonon wave packet with specific momentum and energy. The second harmonic generation of these phonon wave packets is followed by ultrafast X-ray diffraction. Phonon upconversion takes place because the high amplitude phonon wave packet modulates the acoustic properties of the crystal which leads to self steepening and to the successive generation of higher harmonics of the phonon wave packet.
Furthermore, we have demonstrated ultrafast strain in direction parallel to the sample surface. Two consecutive so-called transient grating excitations displaced in space and time are used to coherently control thermal gradients and surface acoustic modes. The amplitude of the coherent and incoherent surface excursion is disentangled by time resolved X-ray reflectivity measurements. We calibrate the absolute amplitude of thermal and acoustic surface excursion with measurements of longitudinal phonon propagation. In addition, we develop a diffraction model which allows for measuring the surface excursion on an absolute length scale with sub-Äangström precision. Finally, I demonstrate full coherent control of an excited surface deformation by amplifying and suppressing thermal and coherent excitations at the surface of a laser-excited Yttrium-manganite sample.
Clark, Oliver J. ; Wadgaonkar, Indrajit ; Freyse, Friedrich ; Springholz, Gunther ; Battiato, Marco ; Sanchez-Barriga, Jaime
A large Rashba effect is essential for future applications in spintronics. Particularly attractive is understanding and controlling nonequilibrium properties of ferroelectric Rashba semiconductors. Here, time- and angle-resolved photoemission is utilized to access the ultrafast dynamics of bulk and surface transient Rashba states after femtosecond optical excitation of GeTe. A complex thermalization pathway is observed, wherein three different timescales can be clearly distinguished: intraband thermalization, interband equilibration, and electronic cooling. These dynamics exhibit an unconventional temperature dependence: while the cooling phase speeds up with increasing sample temperature, the opposite happens for interband thermalization. It is demonstrated how, due to the Rashba effect, an interdependence of these timescales on the relative strength of both electron-electron and electron-phonon interactions is responsible for the counterintuitive temperature dependence, with spin-selection constrained interband electron-electron scatterings found both to dominate dynamics away from the Fermi level, and to weaken with increasing temperature. These findings are supported by theoretical calculations within the Boltzmann approach explicitly showing the opposite behavior of all relevant electron-electron and electron-phonon scattering channels with temperature, thus confirming the microscopic mechanism of the experimental findings. The present results are important for future applications of ferroelectric Rashba semiconductors and their excitations in ultrafast spintronics.
In this dissertation the lattice and the magnetic recovery dynamics of the two heavy rare-earth metals Dy and Gd after femtosecond photoexcitation are described. For the investigations, thin films of Dy and Gd were measured at low temperatures in the antiferromagnetic phase of Dy and close to room temperature in the ferromagnetic phase of Gd. Two different optical pump-x-ray probe techniques were employed: Ultrafast x-ray diffraction with hard x-rays (UXRD) yields the structural response of heavy rare-earth metals and resonant soft (elastic) x-ray diffraction (RSXD), which allows measuring directly changes in the helical antiferromagnetic order of Dy. The combination of both techniques enables to study the complex interaction between the magnetic and the phononic subsystems.
We define and study in detail utraslow scaled Brownian motion (USBM) characterized by a time dependent diffusion coefficient of the form . For unconfined motion the mean squared displacement (MSD) of USBM exhibits an ultraslow, logarithmic growth as function of time, in contrast to the conventional scaled Brownian motion. In a harmonic potential the MSD of USBM does not saturate but asymptotically decays inverse-proportionally to time, reflecting the highly non-stationary character of the process. We show that the process is weakly non-ergodic in the sense that the time averaged MSD does not converge to the regular MSD even at long times, and for unconfined motion combines a linear lag time dependence with a logarithmic term. The weakly non-ergodic behaviour is quantified in terms of the ergodicity breaking parameter. The USBM process is also shown to be ageing: observables of the system depend on the time gap between initiation of the test particle and start of the measurement of its motion. Our analytical results are shown to agree excellently with extensive computer simulations.
We define and study in detail utraslow scaled Brownian motion (USBM) characterized by a time dependent diffusion coefficient of the form . For unconfined motion the mean squared displacement (MSD) of USBM exhibits an ultraslow, logarithmic growth as function of time, in contrast to the conventional scaled Brownian motion. In a harmonic potential the MSD of USBM does not saturate but asymptotically decays inverse-proportionally to time, reflecting the highly non-stationary character of the process. We show that the process is weakly non-ergodic in the sense that the time averaged MSD does not converge to the regular MSD even at long times, and for unconfined motion combines a linear lag time dependence with a logarithmic term. The weakly non-ergodic behaviour is quantified in terms of the ergodicity breaking parameter. The USBM process is also shown to be ageing: observables of the system depend on the time gap between initiation of the test particle and start of the measurement of its motion. Our analytical results are shown to agree excellently with extensive computer simulations.
Coronal mass ejections are often considered to result from the full eruption of a magnetic flux rope (MFR). However, it is recognized that, in some events, the MFR may release only part of its flux, with the details of the implied splitting not completely established due to limitations in observations. Here, we investigate two partial eruption events including a confined and a successful one. Both partial eruptions are a consequence of the vertical splitting of a filament-hosting MFR involving internal reconnection. A loss of equilibrium in the rising part of the magnetic flux is suggested by the impulsive onset of both events and by the delayed onset of reconnection in the confined event. The remaining part of the flux might be line-tied to the photosphere in a bald patch (BP) separatrix surface, and we confirm the existence of extended BP sections for the successful eruption. The internal reconnection is signified by brightenings in the body of one filament and between the rising and remaining parts of both filaments. It evolves quickly into the standard current sheet reconnection in the wake of the eruption. As a result, regardless of being confined or successful, both eruptions produce hard X-ray sources and flare loops below the erupting but above the surviving flux, as well as a pair of flare ribbons enclosing the latter.
Scientific inquiry requires that we formulate not only what we know, but also what we do not know and by how much. In climate data analysis, this involves an accurate specification of measured quantities and a consequent analysis that consciously propagates the measurement errors at each step. The dissertation presents a thorough analytical method to quantify errors of measurement inherent in paleoclimate data. An additional focus are the uncertainties in assessing the coupling between different factors that influence the global mean temperature (GMT).
Paleoclimate studies critically rely on `proxy variables' that record climatic signals in natural archives. However, such proxy records inherently involve uncertainties in determining the age of the signal. We present a generic Bayesian approach to analytically determine the proxy record along with its associated uncertainty, resulting in a time-ordered sequence of correlated probability distributions rather than a precise time series. We further develop a recurrence based method to detect dynamical events from the proxy probability distributions. The methods are validated with synthetic examples and
demonstrated with real-world proxy records. The proxy estimation step reveals the interrelations between proxy variability and uncertainty. The recurrence analysis of the East Asian Summer Monsoon during the last 9000 years confirms the well-known `dry' events at 8200 and 4400 BP, plus an additional significantly dry event at 6900 BP.
We also analyze the network of dependencies surrounding GMT. We find an intricate, directed network with multiple links between the different factors at multiple time delays. We further uncover a significant feedback from the GMT to the El Niño Southern Oscillation at quasi-biennial timescales. The analysis highlights the need of a more nuanced formulation of influences between different climatic factors, as well as the limitations in trying to estimate such dependencies.
Reppert, Alexander von ; Mattern, Maximilian ; Pudell, Jan-Etienne ; Zeuschner, Steffen Peer ; Dumesnil, Karine ; Bargheer, Matias
Optical excitation of spin-ordered rare earth metals triggers a complex response of the crystal lattice since expansive stresses from electron and phonon excitations compete with a contractive stress induced by spin disorder. Using ultrafast x-ray diffraction experiments, we study the layer specific strain response of a dysprosium film within a metallic heterostructure upon femtosecond laser-excitation. The elastic and diffusive transport of energy to an adjacent, non-excited detection layer clearly separates the contributions of strain pulses and thermal excitations in the time domain. We find that energy transfer processes to magnetic excitations significantly modify the observed conventional bipolar strain wave into a unipolar pulse. By modeling the spin system as a saturable energy reservoir that generates substantial contractive stress on ultrafast timescales, we can reproduce the observed strain response and estimate the time- and space dependent magnetic stress. The saturation of the magnetic stress contribution yields a non-monotonous total stress within the nanolayer, which leads to unconventional picosecond strain pulses.
Reppert, Alexander von ; Mattern, Maximilian ; Pudell, Jan-Etienne ; Zeuschner, Steffen Peer ; Dumesnil, Karine ; Bargheer, Matias
Optical excitation of spin-ordered rare earth metals triggers a complex response of the crystal lattice since expansive stresses from electron and phonon excitations compete with a contractive stress induced by spin disorder. Using ultrafast x-ray diffraction experiments, we study the layer specific strain response of a dysprosium film within a metallic heterostructure upon femtosecond laser-excitation. The elastic and diffusive transport of energy to an adjacent, non-excited detection layer clearly separates the contributions of strain pulses and thermal excitations in the time domain. We find that energy transfer processes to magnetic excitations significantly modify the observed conventional bipolar strain wave into a unipolar pulse. By modeling the spin system as a saturable energy reservoir that generates substantial contractive stress on ultrafast timescales, we can reproduce the observed strain response and estimate the time- and space dependent magnetic stress. The saturation of the magnetic stress contribution yields a non-monotonous total stress within the nanolayer, which leads to unconventional picosecond strain pulses.
Bodrova, Anna S. ; Chechkin, Aleksei ; Cherstvy, Andrey G. ; Safdari, Hadiseh ; Sokolov, Igor M. ; Metzler, Ralf
It is quite generally assumed that the overdamped Langevin equation provides a quantitative description of the dynamics of a classical Brownian particle in the long time limit. We establish and investigate a paradigm anomalous diffusion process governed by an underdamped Langevin equation with an explicit time dependence of the system temperature and thus the diffusion and damping coefficients. We show that for this underdamped scaled Brownian motion (UDSBM) the overdamped limit fails to describe the long time behaviour of the system and may practically even not exist at all for a certain range of the parameter values. Thus persistent inertial effects play a non-negligible role even at significantly long times. From this study a general questions on the applicability of the overdamped limit to describe the long time motion of an anomalously diffusing particle arises, with profound consequences for the relevance of overdamped anomalous diffusion models. We elucidate our results in view of analytical and simulations results for the anomalous diffusion of particles in free cooling granular gases.