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Changes in extratropical storm track activity and their implications for extreme weather events
(2016)
Water scarcity, adaption on climate change, and risk assessment of droughts and floods are critical topics for science and society these days. Monitoring and modeling of the hydrological cycle are a prerequisite to understand and predict the consequences for weather and agriculture. As soil water storage plays a key role for partitioning of water fluxes between the atmosphere, biosphere, and lithosphere, measurement techniques are required to estimate soil moisture states from small to large scales.
The method of cosmic-ray neutron sensing (CRNS) promises to close the gap between point-scale and remote-sensing observations, as its footprint was reported to be 30 ha. However, the methodology is rather young and requires highly interdisciplinary research to understand and interpret the response of neutrons to soil moisture. In this work, the signal of nine detectors has been systematically compared, and correction approaches have been revised to account for meteorological and geomagnetic variations. Neutron transport simulations have been consulted to precisely characterize the sensitive footprint area, which turned out to be 6--18 ha, highly local, and temporally dynamic. These results have been experimentally confirmed by the significant influence of water bodies and dry roads. Furthermore, mobile measurements on agricultural fields and across different land use types were able to accurately capture the various soil moisture states. It has been further demonstrated that the corresponding spatial and temporal neutron data can be beneficial for mesoscale hydrological modeling. Finally, first tests with a gyrocopter have proven the concept of airborne neutron sensing, where increased footprints are able to overcome local effects.
This dissertation not only bridges the gap between scales of soil moisture measurements. It also establishes a close connection between the two worlds of observers and modelers, and further aims to combine the disciplines of particle physics, geophysics, and soil hydrology to thoroughly explore the potential and limits of the CRNS method.
Change points in time series are perceived as heterogeneities in the statistical or dynamical characteristics of the observations. Unraveling such transitions yields essential information for the understanding of the observed system’s intrinsic evolution and potential external influences. A precise detection of multiple changes is therefore of great importance for various research disciplines, such as environmental sciences, bioinformatics and economics. The primary purpose of the detection approach introduced in this thesis is the investigation of transitions underlying direct or indirect climate observations. In order to develop a diagnostic approach capable to capture such a variety of natural processes, the generic statistical features in terms of central tendency and dispersion are employed in the light of Bayesian inversion. In contrast to established Bayesian approaches to multiple changes, the generic approach proposed in this thesis is not formulated in the framework of specialized partition models of high dimensionality requiring prior specification, but as a robust kernel-based approach of low dimensionality employing least informative prior distributions.
First of all, a local Bayesian inversion approach is developed to robustly infer on the location and the generic patterns of a single transition. The analysis of synthetic time series comprising changes of different observational evidence, data loss and outliers validates the performance, consistency and sensitivity of the inference algorithm. To systematically investigate time series for multiple changes, the Bayesian inversion is extended to a kernel-based inference approach. By introducing basic kernel measures, the weighted kernel inference results are composed into a proxy probability to a posterior distribution of multiple transitions. The detection approach is applied to environmental time series from the Nile river in Aswan and the weather station Tuscaloosa, Alabama comprising documented changes. The method’s performance confirms the approach as a powerful diagnostic tool to decipher multiple changes underlying direct climate observations.
Finally, the kernel-based Bayesian inference approach is used to investigate a set of complex terrigenous dust records interpreted as climate indicators of the African region of the Plio-Pleistocene period. A detailed inference unravels multiple transitions underlying the indirect climate observations, that are interpreted as conjoint changes. The identified conjoint changes coincide with established global climate events. In particular, the two-step transition associated to the establishment of the modern Walker-Circulation contributes to the current discussion about the influence of paleoclimate changes on the environmental conditions in tropical and subtropical Africa at around two million years ago.
In the first part of my work I have investigated the ageing properties of the first passage time distributions in a one-dimensional subdiffusive continuous time random walk with power law distributed waiting times of the form $\psi(\tau) \sim \tau^{-1-\alpha}$ with $0<\alpha<1$ and $1<\alpha<2$. The age or ageing time $t_a$ is the time span from the start of the stochastic process to the start of the observation of this process (at $t=0$). I have calculated the results for a single target and two targets, also including the biased case, where the walker is driven towards the boundary by a constant force. I have furthermore refined the previously derived results for the non-ageing case and investigated the changes that occur when the walk is performed in a discrete quenched energy landscape, where the waiting times are fixed for every site. The results include the exact Laplace space densities and infinite (converging) series as exact results in the time space. The main results are the dominating long time power law behavior regimes, which depend on the ageing time. For the case of unbiased subdiffusion ($\alpha < 1$) in the presence of one target, I find three different dominant terms for ranges of $t$ separated by $t_a$ and another crossover time $t^{\star}$, which depends on $t_a$ as well as on the anomalous exponent $\alpha$ and the anomalous diffusion coefficient $K_{\alpha}$. In all three regimes ($t \ll t_a$, $t_a \ll t \ll t^{\star}$, $t \gg t^{\star}$) one finds power law decay with exponents depending on $\alpha$. The middle regime only exists for $t_a \ll t^{\star}$. The dominant terms in the first two regimes (ageing regimes) come from the probability distribution of the forward waiting time, the time one has to wait for the stochastic process to make the first step during the observation. When the observation time is larger than the second crossover time $t^{\star}$, the first passage time density does not show ageing and the non-ageing first passage time dominates. The power law exponents in the respective regimes are $-\alpha$ for strong ageing, $-1-\alpha$ in the intermediate regime, and $-1-\alpha/2$ in the final non-ageing regime. A similar split into three regimes can be found for $1<\alpha<2$, only with a different second crossover time $t^*$. In this regime the diffusion is normal but also age-dependent. For the diffusion in quenched energy landscapes one cannot detect ageing. The first passage time density shows a quenched power law $^\sim t^{-(1+2\alpha)/(1+\alpha)}$. For diffusion between two target sites and the biased diffusion towards a target only two scaling regimes emerge, separated by the ageing time. In the ageing case $t \ll t_a$ the forward waiting time is again dominant with power law exponent $-\alpha$, while the non-ageing power law $-1-\alpha$ is found for all times $t \gg t_a$. An intermediate regime does not exist. The bias and the confinement have similar effects on the first passage time density. For quenched diffusion, the biased case is interesting, as the bias reduces correlations due to revisiting of the same waiting time. As a result, CTRW like behavior is observed, including ageing. Extensive computer simulations support my findings.
The second part of my research was done on the subject of ageing Scher-Montroll transport, which is in parts closely related to the first passage densities. It explains the electrical current in an amorphous material. I have investigated the effect of the width of a given initial distribution of charge carriers on the transport coefficients as well as the ageing effect on the emerging power law regimes and a constant initial regime. While a spread out initial distribution has only little impact on the Scher-Montroll current, ageing alters the behavior drastically. Instead of the two classical power laws one finds four current regimes, up to three of which can appear in a single experiment. The dominant power laws differ for $t \ll t_a, t_c$, $t_a \ll t \ll t_c$, $t_c \ll t \ll t_a$, and $t \gg t_a,t_c$. Here, $t_c$ is the crossover time of the non-aged Scher-Montroll current. For strongly aged systems one can observe a constant current in the first regime while the others are dominated by decaying power laws with exponents $\alpha -1$, $-\alpha$, and $-1-\alpha$. The ageing regimes are the 1st and 3rd one, while the classical regimes are the 2nd and the 4th. I have verified the theory using numerical integration of the exact integrals and applied the new results to experimental data.
In the third part I considered a single file of subdiffusing particles in an energy landscape. Every occupied site of the landscape acts as a boundary, from which a particle is immediately reflected to its previous site, if it tries to jump there. I have analysed the effects single-file diffusion a quenched landscape compared to an annealed landscape and I have related these results to the number of steps and related quantities. The diffusion changes from ultraslow logarithmic diffusion in the annealed or CTRW case to subdiffusion with an anomalous exponent $\alpha/(1+\alpha)$ in the quenched landscape. The behavior is caused by the forward waiting time, which changes drastically from the quenched to the annealed case. Single-file effects in the quenched landscape are even more complicated to consider in the ensemble average, since the diffusion in individual landscapes shows extremely diverse behavior. Extensive simulations support my theoretical arguments, which consider mainly the long time evolution of the mean square displacement of a bulk particle.
The goal of the presented work is to explore the interaction between gold nanorods (GNRs) and hyper-sound waves. For the generation of the hyper-sound I have used Azobenzene-containing polymer transducers. Multilayer polymer structures with well-defined thicknesses and smooth interfaces were built via layer-by-layer deposition. Anionic polyelectrolytes with Azobenzene side groups (PAzo) were alternated with cationic polymer PAH, for the creation of transducer films. PSS/PAH multilayer were built for spacer layers, which do not absorb in the visible light range. The properties of the PAzo/PAH film as a transducer are carefully characterized by static and transient optical spectroscopy. The optical and mechanical properties of the transducer are studied on the picosecond time scale. In particular the relative change of the refractive index of the photo-excited and expanded PAH/PAzo is Δn/n = - 2.6*10‐4. Calibration of the generated strain is performed by ultrafast X-ray diffraction calibrated the strain in a Mica substrate, into which the hyper-sound is transduced. By simulating the X-ray data with a linear-chain-model the strain in the transducer under the excitation is derived to be Δd/d ~ 5*10‐4.
Additional to the investigation of the properties of the transducer itself, I have performed a series of experiments to study the penetration of the generated strain into various adjacent materials. By depositing the PAzo/PAH film onto a PAH/PSS structure with gold nanorods incorporated in it, I have shown that nanoscale impurities can be detected via the scattering of hyper-sound.
Prior to the investigation of complex structures containing GNRs and the transducer, I have performed several sets of experiments on GNRs deposited on a small buffer of PSS/PAH. The static and transient response of GNRs is investigated for different fluence of the pump beam and for different dielectric environments (GNRs covered by PSS/PAH).
A systematic analysis of sample architectures is performed in order to construct a sample with the desired effect of GNRs responding to the hyper-sound strain wave. The observed shift of a feature related to the longitudinal plasmon resonance in the transient reflection spectra is interpreted as the event of GNRs sensing the strain wave. We argue that the shift of the longitudinal plasmon resonance is caused by the viscoelastic deformation of the polymer around the nanoparticle. The deformation is induced by the out of plane difference in strain in the area directly under a particle and next to it. Simulations based on the linear chain model support this assumption. Experimentally this assumption is proven by investigating the same structure, with GNRs embedded in a PSS/PAH polymer layer.
The response of GNRs to the hyper-sound wave is also observed for the sample structure with GNRs embedded in PAzo/PAH films. The response of GNRs in this case is explained to be driven by the change of the refractive index of PAzo during the strain propagation.
This publications-based thesis summarizes my contribution to the scientific field of ultrafast structural dynamics. It consists of 16 publications, about the generation, detection and coupling of coherent gigahertz longitudinal acoustic phonons, also called hypersonic waves. To generate such high frequency phonons, femtosecond near infrared laser pulses were used to heat nanostructures composed of perovskite oxides on an ultrashort timescale. As a consequence the heated regions of such a nanostructure expand and a high frequency acoustic phonon pulse is generated. To detect such coherent acoustic sound pulses I use ultrafast variants of optical Brillouin and x-ray scattering. Here an incident optical or x-ray photon is scattered by the excited sound wave in the sample. The scattered light intensity measures the occupation of the phonon modes.
The central part of this work is the investigation of coherent high amplitude phonon wave packets which can behave nonlinearly, quite similar to shallow water waves which show a steepening of wave fronts or solitons well known as tsunamis. Due to the high amplitude of the acoustic wave packets in the solid, the acoustic properties can change significantly in the vicinity of the sound pulse. This may lead to a shape change of the pulse. I have observed by time-resolved Brillouin scattering, that a single cycle hypersound pulse shows a wavefront steepening. I excited hypersound pulses with strain amplitudes until 1% which I have calibrated by ultrafast x-ray diffraction (UXRD).
On the basis of this first experiment we developed the idea of the nonlinear mixing of narrowband phonon wave packets which we call "nonlinear phononics" in analogy with the nonlinear optics, which summarizes a kaleidoscope of surprising optical phenomena showing up at very high electric fields. Such phenomena are for instance Second Harmonic Generation, four-wave-mixing or solitons. But in case of excited coherent phonons the wave packets have usually very broad spectra which make it nearly impossible to look at elementary scattering processes between phonons with certain momentum and energy.
For that purpose I tested different techniques to excite narrowband phonon wave packets which mainly consist of phonons with a certain momentum and frequency. To this end epitaxially grown metal films on a dielectric substrate were excited with a train of laser pulses. These excitation pulses drive the metal film to oscillate with the frequency given by their inverse temporal displacement and send a hypersonic wave of this frequency into the substrate. The monochromaticity of these wave packets was proven by ultrafast optical Brillouin and x-ray scattering.
Using the excitation of such narrowband phonon wave packets I was able to observe the Second Harmonic Generation (SHG) of coherent phonons as a first example of nonlinear wave mixing of nanometric phonon wave packets.
The cell interior is a highly packed environment in which biological macromolecules evolve and function. This crowded media has effects in many biological processes such as protein-protein binding, gene regulation, and protein folding. Thus, biochemical reactions that take place in such crowded conditions differ from diluted test tube conditions, and a considerable effort has been invested in order to understand such differences.
In this work, we combine different computationally tools to disentangle the effects of molecular crowding on biochemical processes. First, we propose a lattice model to study the implications of molecular crowding on enzymatic reactions. We provide a detailed picture of how crowding affects binding and unbinding events and how the separate effects of crowding on binding equilibrium act together. Then, we implement a lattice model to study the effects of molecular crowding on facilitated diffusion. We find that obstacles on the DNA impair facilitated diffusion. However, the extent of this effect depends on how dynamic obstacles are on the DNA. For the scenario in which crowders are only present in the bulk solution, we find that at some conditions presence of crowding agents can enhance specific-DNA binding. Finally, we make use of structure-based techniques to look at the impact of the presence of crowders on the folding a protein. We find that polymeric crowders have stronger effects on protein stability than spherical crowders. The strength of this effect increases as the polymeric crowders become longer. The methods we propose here are general and can also be applied to more complicated systems.