Universität Stuttgart
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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 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 Nanoscale magnetic resonance spectroscopy with nitrogen-vacancy centers in diamond(2021) Paone, Domenico; Wrachtrup, Jörg (Prof. Dr.)Stickstoff-Fehlstellen (NV-Zentren) in Diamant bilden interessante Quantensysteme, welche für Quanten-Sensing Protokolle genutzt werden können. In der vorliegenden Arbeit, werden NV-Zentren genutzt, um einzelne Molekülsysteme auszulesen und supraleitende Proben lokal zu charakterisieren. Zusätzlich werden Methoden entwickelt, um die Spineigenschaften der NV-Zentren zu optimieren, welche dann Einfluss auf das Sensorikverhalten des Systems haben.Item Open Access Microwave conductivity in polycrystalline (BEDT-TTF)2I3 material(1991) Müller, Gerhard; Helberg, Hans W.; Schweitzer, Dieter; Keller, Heimo J.Polycrystalline material of the α-phase of (BEDT-TTF)2I3 was compressed to small samples (4-mm x 1mm, thickness 0.3 mm typically) at a pressure of 10 kbar. Annealing at 70°C yields the superconducting αt-phase. Microwaves (10,2 GHz) enable the measurements of the conductivity for stepwise annealing after every annealing step in always the same sample. For annealing times 10 min all conductivity versus temperature curves are intersecting in an isosbestlc point at 190 K. This behaviour can be described by a conductivity relation for a two component system, from which was determined the volume fraction of the new grown αt-phase in dependence of the annealing time. Starting annealing (annealing times < 10 min) shows another unexpected phase transformation. After 2 min annealing the conductivity at 200 K increases by more than one order of magnitude, but then decreases of further annealing (5-10 min) down to the value for the unannealed sample.Item Open Access Fluoreszenzdetektiertes Schalten im optischen Nahfeld(2018) Heilig, Mark; Wrachtrup, Jörg (Prof. Dr.)In dieser Abhandlung wird ein neuer Ansatz für hochdichte optische Speichersysteme auf Basis isolierter, dicht gepackter, photochromer Nanostrukturen (Dots) überprüft und weiterentwickelt. Zum Nachweis der dicht gepackten Fulgid-Nanostrukturen mit Strukturabständen weit unterhalb des Beugungslimits über deren Fluoreszenemission wurde ein multifunktionales Raster-Mikroskopiesystem (Konfokal, AFM, SNOM) entwickelt und aufgebaut. Als Sonde werden geätzte Glasfaserspitzen verwendet. Die Fluoreszenzeigenschaften der verwendeten Fulgide bei Raumtemperatur werden bestimmt. Die Korrelation zwischen Schaltzustand und Fluoreszenzemission des C-Isomer der Fulgide wird nachgewiesen. Schaltexperimente an unregelmäßig strukturierten Fulgid-Schichten zeigen die prinzipielle Eignung des Konzepts. An regelmäßig angeordneten Strukturen werde in programmgesteuerten Speicherversuchen Informationen reversibel in die einzelnen Speicherzellen geschrieben, gelesen und gelöscht. Für kleinste Fulgid-Strukturen in hexagonaler Anordnung mit einem Strukturabstand von 0.100µm ergibt sich eine Speicherdichte von 173GBit=in². Aufgrund der Anordnung treten in hochauflösenden SNOM-Messungen Überlagerungseffekte auf. Diese werden mit Hilfe der FEM in der Simulation untersucht, analysiert und erklärt. Eine Alternative zu Apertur-Sitzen im SNOM stellen lokal emittierende Lichtquellen dar. Ein Nanodiamant mit Stickstoff-Defekt-Zelle eignet sich als Emitter. Die Wechselwirkung mit einer Gold-Struktur wird in der FEM simuliert und experimentell bestätigt.Item Open Access Resonant Raman scattering from superconducting single crystals of (BEDT-TTF)2I3(1993) Pokhodnia, Konstantin I.; Graja, Andrzej; Weger, Meir; Schweitzer, DieterA study of low energetic resonant Raman scattering of (BEDT-TTF)2I3 superconducors was performed. The vanishing of phonon bands accompanied by a decrease of the electronic background was observed below Tc. We propose a theoretical explanation for this novel effect in terms of the Balseiro-Falicov model of phonon-superconducting amplitude mode interaction.Item Open Access Quantifying quantum heterodyne and non-linear spectroscopy for nanoscale magnetic resonance(2022) Meinel, Jonas; Wrachtrup, Jörg (Prof. Dr.)Item Open Access Resonant Raman scattering from superconducting gap excitations in single crystals of (BEDT-TTF)2I3(1993) Graja, Andrzej; Pokhodnia, Konstantin I.; Weger, Meir; Schweitzer, DieterA study of low-energetic resonant Raman scattering of αt- and βH-(BEDT-TTF)2I3 superconductor was performed. The softening and weakening of the low frequency optical phonons at about 30 cm-1 in the superconducting state of both αt- and βH-phases were observed below Tc.Item Open Access Structural and electronic characterization of single crystals of ambipolar organic semiconductors : diindenoperylene and diphenylanthracene(2008) Tripathi, Ashutosh Kumar; Wrachtrup, Jörg (Prof. Dr.)In the present work, structural and electronic characterizations of the chemically stable ambipolar organic semiconductor molecules diindenoperylene (DIP) and 9,10 diphenylanthracene (DPA) have been performed. As proposed by Clar's sextet rule these molecules exhibit a strong resistivity against photo-oxidation due to their molecular configuration. This was verified by Ultraviolet-visible (UV-Vis) spectroscopy. Crystals of high quality were grown by sublimation (DIP and DPA) as well as Bridgman growth (DPA) techniques. Different polymorphs of these crystals were analytically characterized and the corresponding crystal structures were obtained using temperature dependent X-ray diffraction and single crystal diffractometry. DIP crystals undergo an enantiotropic phase transition at 403 K. The low temperature (T < 403 K) phase consists of a triclinic crystal structure which changes to the higher symmetry monoclinic crystal structure for temperatures above 403 K. The enthalpy of the phase transition estimated by differential scanning calorimetry (DSC) amounts to 1 ± 0.2 kJ/mol and the corresponding entropy of 2.4 ± 0.5 J/(mol K) is in good agreement with theoretical calculations of the entropy change of 2.88 J/(mol K) due to the change in symmetry. Time of Flight (TOF) measurements were performed along out-of-plane (c') direction of DIP crystals. Both electron and hole transport were observed. This reflects the chemical stability of the DIP molecule. Room temperature mobilities for electrons and holes amount to 0.02 cm^2/Vs and 0.003 cm^2/Vs respectively. As expected, both electrons and holes exhibit a thermally activated transport because of the structural defects, caused by the phase transition, which break the translational symmetry. The Effects of the structural phase transition were observed on both electrons and holes transport. Further, field effect transistors (FETs) were fabricated on DIP crystals to study the charge transport in the (ab)- plane. At room temperature a FET mobility of ~ 2*10^-4 cm^2/Vs in the (ab)-plane was estimated. The FET mobility is more sensitive on the phase transition due to the stronger intermolecular interactions in the (ab)-plane. Two monotropic polymorphs were observed in DPA crystals which depend delicately on the growth technique (i.e. from vapor phase or from the melt). Bridgman grown crystals show a typical band-like transport along c'-direction with a room temperature hole mobility of ~ 3.7 cm^2/Vs and a temperature dependence of T^-2.3. The exponent 2.3 in the power law indicates a band-like transport with scattering by acoustic as well as optical phonons. Sublimation grown crystals grow with their surface normal along the b-direction. Both electrons and holes transport was observed by TOF technique in these crystals. Room temperature mobilities for electrons and holes amount to 4.8 cm^2/Vs and 6.6 cm^2/Vs respectively. Both electrons and holes exhibit a band-like transport with a temperature dependence of the mobility of T^-1.4 and T^-1.5 respectively. The exponent ~1.5 characterizes band-like transport with scattering by acoustic phonons. High mobilities in DPA crystals can be attributed to the phenyl-phenyl group overlap along the transport directions.Item Open Access Organic metals from chiral BEDT-TTF donors(1991) Chen, Ben-ming; Deilacher, Frank; Hoch, Matthias; Keller, Heimo J.; Wu, Pei-ji; Gärtner, Stephan; Kahlich, Siegfried; Schweitzer, DieterWe have shown that is is possible to obtain organic metals from chiral molecules. The X-ray results prove an oxidation number of + 1.5 for the radical cations in at least two cases. To our best knowledge. these are: the first examples of BEDT-TTF-related radical cation salts with this oxidation number. As expected, we obtained statistically disordered crystals, containing the two different enantiomers in a "racemic" mixture. The broad smeared-out phase transitions are probably due to this disorder, or may be caused by the three-dimensional interactions which have been observed, so far, only once in a BEDT-TTF radical salt. We will crystallize the metallic compounds using "optically pure" isomers, in the hope to be able to isolate chiral metals.