Universität Stuttgart
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Item Open Access Investigating superconductivity by tunneling spectroscopy using oxide heterostructures(2017) Fillis-Tsirakis, Evangelos; Mannhart, Jochen (Prof. Dr.)Item Open Access 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.Item Open Access Molecular solids containing BEDT-TTF and structurally related transition metal complexes(1986) Keller, Heimo J.; Niebl, Roland; Nöthe, Dietrich; Schweitzer, Dieter; Weber, AngelikaThe special physical properties of BEDT-TTF salts, e.g. their two-dimensional behaviour, are caused by the typical geometry of this donor and the arrangement of the cations in the crystal lattice of its salts. In order to extend the range of physical properties produced by BEDT-TTF like compounds, we synthesized sulfur containing transition metal complexes with a molecular structure very similar to BEDT-TTF. The bis(5.6-dihydro-1.4-dithin-2.3-dithiolate)metallates of the nickel triad can be prepared in different oxidation states as anions and in neutral form. The anionic complexes can be reacted with BEDT-TTF cations.Item Open Access Energy gap reduction in superconducting tin films by quasiparticle injection(1977) Fuchs, Jürgen; Epperlein, Peter W.; Welte, Michael; Eisenmenger, WolfgangIn Sn-/-Sn-/-Pb tunneling structures the energy gap ΔSn of Sn is reduced by quasiparticle injection via single-particle tunneling between the Sn films. ΔSn as function of the quasiparticle density is probed by the Pb contact and found in agreement with the theory of Owen and Scalapino. An instability of the energy gap of Sn is observed at the critical gap reduction ratio predicted by this theory for a first-order phase transition.Item Open Access 1,3,5-Tris(dimethylamino)benzol mit Iod und 1,3,5-Tricyanobenzol : eine ungewöhnliche Dimerisierung und ein "normaler" Donor/Akzeptor-Komplex(1988) Keller, Heimo J.; Niebl, Roland; Renner, Gerd; Ruhr, Dorothea von der; Schweitzer, DieterWir sind auf der Suche nach "organischen" Ferromagneten. Als Zielsubstanz haben wir kristallisierte Radikal-Ionen mit bahnentarteten Grundzuständen ausgewählt. Molekulare Festkörper aus planaren organischen Radikalionen zeigen ein breites Spektrum teilweise recht interessanter physikalischer Eigenschaften, die durch kollektives Elektronenverhalten zu erklären sind. In den letzten Jahren wurde vor allem das elektrische Verhalten dieser Substanzen untersucht. Dies führte zur Entdeckung einer Vielzahl "organischer Metalle", von denen einige bei tiefer Temperatur auch supraleitend werden.Item Open Access Zukunft der Optik(1970) Tiziani, Hans J.Die Optik hat in den letzten Jahren neuen Aufschwung genommen. Mitverantwortlich für diese Entwicklung sind sowohl die Verwendung von leistungsfähigen Computern als auch die Nachfrage nach immer besserer Auflösung und Bildqualität. Besonders positiv haben sich die Entwicklungen des Laser (1960) und der Holographie ausgewirkt. Immer neue Applikationen des gebündelten, kohärenten Laserlichtes werden erschlossen, doch will ich mich in diesem Zusammenhang auf die mögliche Weiterentwlckung der erwähnten Gebiete beschränken.Item Open Access Exploring the growth of refractory metal and sapphire films by thermal laser epitaxy(2024) Majer, Lena N.; Mannhart, Jochen (Prof. Dr.)Item Open Access Zero bias anomalies in point-contact characteristics of αt-(BEDT-TTF)2I3(1994) Ernst, Gabriele; Nowack, Andreas; Weger, Meir; Schweitzer, DieterThe zero-bias anomaly in point-contact characteristics of the organic superconductor α-(BEDT-TTF)2I3 is investigated as a function of temperature and magnetic field. It is found that the zero-bias anomaly is insensitive to magnetic fields up to 5 T. In contrast, a structure at 5 meV, conventionally designated as the superconducting gap - but which is 4 times larger than the expected BCS gap - is strongly affected by magnetic fields above 1 T.Item Open Access Microscopic calculation of line tensions(2008) Merath, Rolf-Jürgen Christian; Dietrich, Siegfried (Prof. Dr.)In this work the line tension has been determinded with molecular resolution, which in this context marks the forefront of research. A semi-microscopic line tension theory based on the sharp-kink approximation has been further developed. The sharp-kink results concerning wetting and line tension behavior deviate considerably from the fully microscopic results. A hybrid line tension theory has been introduced, which employs an improved effective interface potential for the SK line tension calculation. For most of the studied cases the results from this hybrid method describe the fully microscopic line tension values semi-quantitatively. However, for a tailored system with relatively strong spatial variations of the substrate potential and of the solid-liquid interfacial density the hybrid method fails and does not predict the correct order of magnitude of the line tension values. Hence in general the fully microscopic approach is required, if one is interested in quantitatively reliable line tension values or/and if the validity of the hybrid method for the considered system has not been checked. The calculation of the line tension of a liquid wedge is an important contribution for understanding the shape of very small droplets (below the micrometer range). Furthermore a proposal is given, how axisymmetric sessile droplets can be addressed efficiently within DFT.Item Open Access Reflection of high-frequency phonons at silicon-solid interfaces(1981) Marx, Dieter; Eisenmenger, WolfgangIn reflection experiments with phonons of frequencies above 280 GHz propagating along (110) directions we observed large deviations from the acoustic mismatch theory for silicon-metal, silicon-condensed gas, and silicon-liquid helium interfaces.