Universität Stuttgart

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    Investigating superconductivity by tunneling spectroscopy using oxide heterostructures
    (2017) Fillis-Tsirakis, Evangelos; Mannhart, Jochen (Prof. Dr.)
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    Nonlinear optical microspectroscopy with few-cycle laser pulses
    (2017) Wan, Hui; Wrachtrup, Jörg (Prof. Dr.)
    Nonlinear optical (NLO) microscopy is a powerful tool in physics, chemistry, and material science it probes intrinsic optical properties of the sample without the need of labeling. In order to investigate the ultrafast processes in nonlinear materials with high spatial resolution, we need to combine both ultrashort pulses and techniques focusing them to the diffraction limit. Previously, few-cycle laser pulses have often been tightly focused using conventional microscope objectives. However, the propagation of an ultrashort pulse in optical materials, particularly in the glass of a high numerical aperture (N.A.) microscope objective, results in spatial and temporal distortions of the pulse electric field, which can severely affect its quality in the focus. By purely passive group delay dispersion (GDD) and third-order dispersion (TOD) management, in this thesis, we experimentally demonstrate in-focus diffraction-limited and bandwidth-limited few-cycle pulses by using high N.A. objectives. Based on these achievements, the performance of a novel few-cycle NLO microscope for both second-harmonic generation (SHG) imaging and microspectroscopy in the frequency- and time-domains was characterized. The inverse linear dependence of SHG intensity on the in-focus pulse duration was demonstrated down to 7.1 fs for the first time. The application of shorter in-focus pulses for the enhancement of SHG image contrast was successfully demonstrated on a single collagen (type-I) fibril as a biological model system for studying protein assemblies under physiological conditions. Beyond imaging, a collagen fibril has been found to act as a purely non-resonant χ(2) soft matter under the present excitation conditions, and its ratio of forward- to epi-detected SHG intensities allowed for the estimation of the fibril thickness, which corresponds well with atomic force microscopy (AFM) measurements. The ultrafast dephasing of the localized surface plasmon resonance (LSPR) in the metallic nanoparticles, that only occurs on a time scale of a few femtoseconds, has gained a lot of attraction in the field of nanoplasmonics. This thesis is the first systematic experimental demonstration of time-resolving ultrashort plasmon dephasing in single gold nanoparticles by using interferometric SHG spectroscopy with in-focus 7.3 fs excitation pulses in combination with linear scattering spectroscopy performed on the same nanoparticle. For nanorods, nanodisks, and nanorectangles, strong plasmon resonance enhanced SHG is observed, where the SHG intensity strongly depends on the spectral overlap between the LSPR band and the excitation laser spectrum. For single nanorods and nanorectangles, the polarization dependence of the SHG intensity was found to follow second-order dipole scattering, and the effect of size and shape on the LSPR properties was directly observed in the time-domain. Good agreement between experimental and simulated values of dephasing times and resonance wavelengths is obtained, which confirms that a common driven damped harmonic oscillator model for the LSPR in the nanoparticle can qualitatively explain both the linear scattering spectra in the frequency-domain and the SHG response in the time-domain. Resonance bands in linear transmission and scattering spectra have also been observed for nanoholes with sizes smaller than the wavelength of the incident light in a metal film, which are assigned to LSPR modes of the electric field distribution around the nanohole with qualitatively similar resonance properties as a nanoparticle. The polarization-resolved nonlinear optical properties of the single nanoholes with different shapes and symmetries were also reported. The objective of this thesis has been systematic SHG studies of the size effect in the LSPR of single nanoholes in metal films and of their ultrafast dephasing dynamics. Although, enhancement of both the forward- and epi-detected SHG emissions from single rectangular nanoholes are observed,however,no ultrafast dephasing dynamics of LSPRs in rectangular nanoholes could be time-resolved with our in-focus 7.3 fs excitation laser pulses, which indicates that contributions from LSPR enhanced SHG to the detected SHG signal are negligible. More work needs to be done in order to overcome the current experimental limitations. However, in this thesis, the polarization dependence of the forward- and epi-detected SHG intensity from the single rectangular nanohole was found to follow that of a second-order dipole pattern. While the SHG dipole pattern observed for rectangular nanoparticles is oriented parallel to its long-axis, the SHG dipole pattern of its complementary rectangular nanohole is oriented perpendicular to its long-axis. This observation represents the first experimental demonstration of Babinet’s principle in second-order nonlinear scattering of a single rectangular nanohole in a gold film.
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    Long-term stability of capped and buffered palladium-nickel thin films and nanostructures for plasmonic hydrogen sensing applications
    (2013) Strohfeldt, Nikolai; Tittl, Andreas; Giessen, Harald
    One of the main challenges in optical hydrogen sensing is the stability of the sensor material. We found and studied an optimized material combination for fast and reliable optical palladium-based hydrogen sensing devices. It consists of a palladium-nickel alloy that is buffered by calcium fluoride and capped with a very thin layer of platinum. Our system shows response times below 10 s and almost no short-term aging effects. Furthermore, we successfully incorporated this optimized material system into plasmonic nanostructures, laying the foundation for a stable and sensitive hydrogen detector.
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    From Hermitian to non-Hermitian topological phases of matter
    (2019) Rui, Wenbin; Metzner, Walter (Prof. Dr.)
    The focus of this thesis lies on extending the theory of topological phases of matter from the Hermitian to the non-Hermitian regime. This includes not only the extension of conventional concepts such as topological invariants and topological boundary states in the theory of Hermitian topological phases, but also the exploration and characterization of entirely new topological phases unique to non-Hermitian systems.
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    Structure and electronic properties of epitaxial monolayer WSe2
    (2019) Mohammed, Avaise; Takagi, Hidenori (Prof. Dr.)
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    Berücksichtigung der Mondrotation beim Asteroideneinfang an Lagrangepunkten
    (2019) Zatsch, Jonas Christian Jörg
    In der vorliegenden Arbeit wird das Verhalten und die Stabilität von Asteroiden nahe des zweiten Sonne-Erde-Lagrangepunkts L2 und der Einfluss des Erdmonds hierauf untersucht. Dafür wird die Transition State Theory, die sich zur Beschreibung der Dynamik an Rang-1-Sätteln eignet, angewendet.
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    Bose-Einstein condensates with balanced gain and loss beyond mean-field theory
    (2017) Dast, Dennis; Wunner, Günter (Prof. Dr.)
    Most of the work done in the field of Bose-Einstein condensates with balanced gain and loss has been performed in the mean-field approximation using the non-Hermitian PT-symmetric Gross-Pitaevskii equation. However, the exchange of particles with the environment plays a crucial role in such systems which in general leads to deviations from the mean-field behavior. Thus, it is not clear whether a mean-field approach is appropriate. It is the purpose of this work to formulate and study a many-particle description of a Bose-Einstein condensate with balanced gain and loss. This is achieved by using a quantum master equation describing a double well where the incoupling of particles in one well and the outcoupling from the other are implemented with Lindblad superoperators. The in- and outcoupling rates are adjusted in an appropriate manner such that balanced gain and loss is achieved. It is shown that the mean-field limit of this master equation yields a PT-symmetric Gross-Pitaevskii equation. Furthermore the master equation supports the characteristic dynamical properties of PT-symmetric systems. There are, however, fundamental differences compared with the mean-field description revealing a new generic feature of PT-symmetric Bose-Einstein condensates. It is shown that the purity of the condensate periodically drops to small values but then is nearly completely restored, when the particles oscillate in the double well. Since in the mean-field limit a completely pure condensate is assumed, this effect cannot be covered by the Gross-Pitaevskii equation. These purity oscillations have a direct impact on the average contrast in interference experiments. In particular it is found that the extrema of the purity can be precisely measured since the average contrast at these points is not reduced by an imbalance of the particle distribution. To gain a detailed understanding of the purity oscillations, analytic solutions for the dynamics in the non-interacting limit are presented and the Bogoliubov backreaction method is used to discuss the influence of the on-site interaction. A central result is that the strength of the purity revivals does neither depend on the amount of particles in the system nor the interaction strength, but is almost exclusively determined by the strength of the in- and outcoupling processes. However, the strong revivals are shifted towards longer times for larger particle numbers. Without interaction this would make the purity oscillations unobservable for a realistic particle number, but by adjusting the interaction strength the strong revivals again occur earlier.
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    Optical and magneto-optical investigations on 3D Dirac- and Weyl-semimetals
    (2017) Neubauer, David; Dressel, Martin (Prof. Dr.)
    This work concentrates on optical investigations on 3D Dirac- and Weyl-semimetals with and without applied magnetic fields. Four compounds are extensively discussed, namely the 3D Dirac semimetal Cd3As2, the Weyl semimetals TaAs and NbP, and finally evidence is found for 2D Dirac states in the iron based superconductor FeSe. For the measurements in magnetic fields a novel magneto-optical installation is designed and implemented in the lab. The design principle and characterization of this setup is presented.
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    Efficient algorithms for electrostatic interactions including dielectric contrasts
    (2013) Arnold, Axel; Breitsprecher, Konrad; Fahrenberger, Florian; Kesselheim, Stefan; Lenz, Olaf; Holm, Christian
    Coarse grained models of soft matter are usually combined with implicit solvent models that take the electrostatic polarizability into account via a dielectric background. In biophysical or nanoscale simulations that include water, this constant can vary greatly within the system. Performing molecular dynamics or other simulations that need compute exact electrostatic interactions between charges in those systems is computationally demanding. We review here several algorithms developped by us that perform exactly this task. For planar dielectric surfaces in partial periodic boundary conditions, the arising image charges can be either treated with the MMM2D algorithm in a very efficient and accurate way, or with the ELC term that enables the user to use his favorite 3D periodic Coulomb solver . Arbitrarily shaped interfaces can be dealt with using induced surface charges with the ICC algorithm. Finally, the local electrostatics algorithm MEMD (Maxwell Equations Molecular Dynamics) allows even to employ a smoothly varying dielectric constant in the systems. We introduce the concepts of these three algorithms, and an extension for the inclusion of boundaries that are to be held fixed at constant potential (metal conditions). For each method, we present a showcase application to highlight the importance of dielectric interfaces.