@phdthesis{Niehoerster2022, author = {Nieh{\"o}rster, Thomas}, title = {Spektral aufgel{\"o}ste Fluoreszenzlebensdauer-Mikroskopie mit vielen Farben}, doi = {10.25972/OPUS-29657}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-296573}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {Die Fluoreszenzmikroskopie ist eine vielseitig einsetzbare Untersuchungsmethode f{\"u}r biologische Proben, bei der Biomolek{\"u}le selektiv mit Fluoreszenzfarbstoffen markiert werden, um sie dann mit sehr gutem Kontrast abzubilden. Dies ist auch mit mehreren verschiedenartigen Zielmolek{\"u}len gleichzeitig m{\"o}glich, wobei {\"u}blicherweise verschiedene Farbstoffe eingesetzt werden, die {\"u}ber ihre Spektren unterschieden werden k{\"o}nnen. Um die Anzahl gleichzeitig verwendbarer F{\"a}rbungen zu maximieren, wird in dieser Arbeit zus{\"a}tzlich zur spektralen Information auch das zeitliche Abklingverhalten der Fluoreszenzfarbstoffe mittels spektral aufgel{\"o}ster Fluoreszenzlebensdauer-Mikroskopie (spectrally resolved fluorescence lifetime imaging microscopy, sFLIM) vermessen. Dazu wird die Probe in einem Konfokalmikroskop von drei abwechselnd gepulsten Lasern mit Wellenl{\"a}ngen von 485 nm, 532nm und 640nm angeregt. Die Detektion des Fluoreszenzlichtes erfolgt mit einer hohen spektralen Aufl{\"o}sung von 32 Kan{\"a}len und gleichzeitig mit sehr hoher zeitlicher Aufl{\"o}sung von einigen Picosekunden. Damit wird zu jedem detektierten Fluoreszenzphoton der Anregungslaser, der spektrale Kanal und die Ankunftszeit registriert. Diese detaillierte multidimensionale Information wird von einem Pattern-Matching-Algorithmus ausgewertet, der das Fluoreszenzsignal mit zuvor erstellten Referenzpattern der einzelnen Farbstoffe vergleicht. Der Algorithmus bestimmt so f{\"u}r jedes Pixel die Beitr{\"a}ge der einzelnen Farbstoffe. Mit dieser Technik konnten pro Anregungslaser f{\"u}nf verschiedene F{\"a}rbungen gleichzeitig dargestellt werden, also theoretisch insgesamt 15 F{\"a}rbungen. In der Praxis konnten mit allen drei Lasern zusammen insgesamt neun F{\"a}rbungen abgebildet werden, wobei die Anzahl der Farben vor allem durch die anspruchsvolle Probenvorbereitung limitiert war. In anderen Versuchen konnte die sehr hohe Sensitivit{\"a}t des sFLIM-Systems genutzt werden, um verschiedene Zielmolek{\"u}le voneinander zu unterscheiden, obwohl sie alle mit demselben Farbstoff markiert waren. Dies war m{\"o}glich, weil sich die Fluoreszenzeigenschaften eines Farbstoffmolek{\"u}ls geringf{\"u}gig in Abh{\"a}ngigkeit von seiner Umgebung {\"a}ndern. Weiterhin konnte die sFLIM-Technik mit der hochaufl{\"o}senden STED-Mikroskopie (STED: stimulated emission depletion) kombiniert werden, um so hochaufgel{\"o}ste zweifarbige Bilder zu erzeugen, wobei nur ein einziger gemeinsamer STED-Laser ben{\"o}tigt wurde. Die gleichzeitige Erfassung von mehreren photophysikalischen Messgr{\"o}ßen sowie deren Auswertung durch den Pattern-Matching-Algorithmus erm{\"o}glichten somit die Entwicklung von neuen Methoden der Fluoreszenzmikroskopie f{\"u}r Mehrfachf{\"a}rbungen.}, subject = {Fluoreszenzmikroskopie}, language = {de} } @phdthesis{Gruene2022, author = {Gr{\"u}ne, Jeannine}, title = {Spin States and Efficiency-Limiting Pathways in Optoelectronic Materials and Devices}, doi = {10.25972/OPUS-29340}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-293405}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {This thesis addresses the identification and characterization of spin states in optoelectronic materials and devices using multiple spin-sensitive techniques. For this purpose, a systematic study focussing on triplet states as well as associated loss pathways and excited state kinetics was carried out. The research was based on comparing a range of donor:acceptor systems, reaching from organic light emitting diodes (OLEDs) based on thermally activated delayed fluorescence (TADF) to organic photovoltaics (OPV) employing fullerene and multiple non-fullerene acceptors (NFAs). By developing new strategies, e.g., appropriate modeling, new magnetic resonance techniques and experimental frameworks, the influence of spin states in the fundamental processes of organic semiconductors has been investigated. Thereby, the combination of techniques based on the principle of electron paramagnetic resonance (EPR), in particular transient EPR (trEPR) and optically detected magnetic resonance (ODMR), with all-optical methods, such as transient electroluminescence (trEL) and transient absorption (TA), has been employed. As a result, excited spin states, especially molecular and charge transfer (CT) states, were investigated in terms of kinetic behavior and associated pathways, which revealed a significant impact of triplet states on efficiency-limiting processes in both optoelectronic applications.}, subject = {Elektronenspinresonanz}, language = {en} } @phdthesis{Hajer2022, author = {Hajer, Jan}, title = {Mercury Telluride Nanowires for Topological Quantum Transport}, doi = {10.25972/OPUS-29322}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-293222}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {Novel appraches to the molecular beam epitaxy of core-shell nanowires in the group II telluride material system were explored in this work. Significant advances in growth spurred the development of a flexible and reliable platform for a charge transport characterization of the topological insulator HgTe in a tubular nanowire geometry. The transport results presented provide an important basis for the design of future studies that strive for the experimental realization of topological charge transport in the quantum wire limit.}, subject = {Quecksilbertellurid}, language = {en} } @phdthesis{Schmitt2022, author = {Schmitt, Fabian Bernhard}, title = {Transport properties of the three-dimensional topological insulator mercury telluride}, doi = {10.25972/OPUS-29173}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-291731}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {The subject of this thesis is the investigation of the transport properties of topological and massive surface states in the three-dimensional topological insulator Hg(Mn)Te. These surface states give rise to a variety of extraordinary transport phenomena, making this material system of great interest for research and technological applications. In this connection, many physical properties of the topological insulator Hg(Mn)Te still require in-depth exploration. The overall aim of this thesis is to analyze the quantum transport of HgTe-based devices ranging from hundreds of micrometers (macroscopic) down to a few micrometers in size (microscopic) in order to extend the overall understanding of surface states and the possibilities of their manipulation. In order to exploit the full potential of our high-quality heterostructures, it was necessary to revise and improve the existing lithographic fabrication process of macroscopic three-dimensional Hg(Mn)Te samples. A novel lithographic standard recipe for the fabrication of the HgTe-based macrostructures was developed. This recipe includes the use of an optimized Hall bar design and wet etching instead of etching with high-energy \(\mathrm{{Ar^{+}}}\)-ions, which can damage the samples. Further, a hafnium oxide insulator is applied replacing the SiO\(_{2}\)/Si\(_{3}\)N\(_{4}\) dielectric in order to reduce thermal load. Moreover, the devices are metallized under an alternating angle to avoid discontinuities of the metal layers over the mesa edges. It was revealed that the application of gate-dielectric and top-gate metals results in n-type doping of the devices. This phenomenon could be attributed to quasi-free electrons tunneling from the trap states, which form at the interface cap layer/insulator, through the cap into the active layer. This finding led to the development of a new procedure to characterize wafer materials. It was found that the optimized lithographic processing steps do not unintentionally react chemically with our heterostructures, thus avoiding a degradation of the quality of the Hg(Mn)Te layer. The implementation of new contact structures Ti/Au, In/Ti/Au, and Al/Ti/Au did not result in any improvement compared to the standard structure AuGe/Au. However, a novel sample recipe could be developed, resulting in an intermixing of the contact metals (AuGe and Au) and fingering of metal into the mesa. The extent of the quality of the ohmic contacts obtained through this process has yet to be fully established. This thesis further deals with the lithographic realization of three-dimensional HgTe-based microstructures measuring only a few micrometer in size. Thus, these structures are in the order of the mean free path and the spin relaxation length of topological surface state electrons. A lithographic process was developed enabling the fabrication of nearly any desired microscopic device structure. In this context, two techniques suitable for etching microscopic samples were realized, namely wet etching and the newly established inductively coupled plasma etching. While wet etching was found to preserve the crystal quality of the active layer best, inductively coupled plasma etching is characterized by high reproducibility and excellent structural fidelity. Hence, the etching technique employed depends on the envisaged type of experiment. Magneto-transport measurements were carried out on the macroscopic HgTe-based devices fabricated by means of improved lithographic processing with respect to the transport properties of topological and massive surface states. It was revealed that due to the low charge carrier density present in the leads to the ohmic contacts, these regions can exhibit an insulating behavior at high magnetic fields and extremely low temperatures. As soon as the filling factor of the lowest Landau levels dropped below a critical value (\(\nu_{\mathrm{{c}}}\approx0.8\)), the conductance of the leads decreased significantly. It was demonstrated that the carrier density in the leads can be increased by the growth of modulation doping layers, a back-gate-electrode, light-emitting diode illumination, and by the application of an overlapping top-gate layout. This overlapping top-gate and a back-gate made it possible to manipulate the carrier density of the surface states on both sides of the Hg(Mn)Te layer independently. With this setup, it was identified that topological and massive surface states contribute to transport simultaneously in 3D Hg(Mn)Te. A model could be developed allowing the charge carrier systems populated in the sample to be determined unambiguously. Based on this model, the process of the re-entrant quantum Hall effect observed for the first time in three-dimensional topological insulators could be explained by an interplay of n-type topological and p-type massive surface states. A well-pronounced \(\nu=-1\rightarrow\nu=-2\rightarrow\nu=-1\) sequence of quantum Hall plateaus was found in manganese-doped HgTe-based samples. It is postulated that this is the condensed-matter realization of the parity anomaly in three-dimensional topological insulators. The actual nature of this phenomenon can be the subject of further research. In addition, the measurements have shown that inter-scattering occurs between counter-propagating quantum Hall edge states. The good quantization of the Hall conductance despite this inter-scattering indicates that only the unpaired edge states determine the transport properties of the system as a whole. The underlying inter-scattering mechanism is the topic of a publication in preparation. Furthermore, three-dimensional HgTe-based microstructures shaped like the capital letter "H" were investigated regarding spin transport phenomena. The non-local voltage signals occurring in the measurements could be attributed to a current-induced spin polarization of the topological surface states due to electrons obeying spin-momentum locking. It was shown that the strength of this non-local signal is directly connected to the magnitude of the spin polarization and can be manipulated by the applied top-gate voltage. It was found that in these microstructures, the massive surface and bulk states, unlike the topological surface states, cannot contribute to this spin-associated phenomenon. On the contrary, it was demonstrated that the population of massive states results in a reduction of the spin polarization, either due to the possible inter-scattering of massive and topological surface states or due to the addition of an unpolarized electron background. The evidence of spin transport controllable by a top-gate-electrode makes the three-dimensional material system mercury telluride a promising candidate for further research in the field of spintronics.}, subject = {Topologischer Isolator}, language = {en} } @phdthesis{Fijalkowski2022, author = {Fijalkowski, Kajetan Maciej}, title = {Electronic Transport in a Magnetic Topological Insulator (V,Bi,Sb)\(_2\)Te\(_3\)}, doi = {10.25972/OPUS-28230}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-282303}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {This thesis focuses on investigating magneto-transport properties of a ferromagnetic topological insulator (V,Bi,Sb)2Te3. This material is most famously known for exhibiting the quantum anomalous Hall effect, a novel quantum state of matter that has opened up possibilities for potential applications in quantum metrology as a quantum standard of resistance, as well as for academic investigations into unusual magnetic properties and axion electrodynamics. All of those aspects are investigated in the thesis.}, subject = {Topologischer Isolator}, language = {en} } @phdthesis{Uenzelmann2022, author = {{\"U}nzelmann, Maximilian}, title = {Interplay of Inversion Symmetry Breaking and Spin-Orbit Coupling - From the Rashba Effect to Weyl Semimetals}, doi = {10.25972/OPUS-28310}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-283104}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {Breaking inversion symmetry in crystalline solids enables the formation of spin-polarized electronic states by spin-orbit coupling without the need for magnetism. A variety of interesting physical phenomena related to this effect have been intensively investigated in recent years, including the Rashba effect, topological insulators and Weyl semimetals. In this work, the interplay of inversion symmetry breaking and spin-orbit coupling and, in particular their general influence on the character of electronic states, i.e., on the spin and orbital degrees of freedom, is investigated experimentally. Two different types of suitable model systems are studied: two-dimensional surface states for which the Rashba effect arises from the inherently broken inversion symmetry at the surface, and a Weyl semimetal, for which inversion symmetry is broken in the three-dimensional crystal structure. Angle-resolved photoelectron spectroscopy provides momentum-resolved access to the spin polarization and the orbital composition of electronic states by means of photoelectron spin detection and dichroism with polarized light. The experimental results shown in this work are also complemented and supported by ab-initio density functional theory calculations and simple model considerations. Altogether, it is shown that the breaking of inversion symmetry has a decisive influence on the Bloch wave function, namely, the formation of an orbital angular momentum. This mechanism is, in turn, of fundamental importance both for the physics of the surface Rashba effect and the topology of the Weyl semimetal TaAs.}, subject = {Rashba-Effekt}, language = {en} } @phdthesis{GraetzgebDittmann2022, author = {Graetz [geb. Dittmann], Jonas}, title = {X-Ray Dark-Field Tensor Tomography : a Hitchhiker's Guide to Tomographic Reconstruction and Talbot Imaging}, doi = {10.25972/OPUS-28143}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-281437}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {X-ray dark-field imaging allows to resolve the conflict between the demand for centimeter scaled fields of view and the spatial resolution required for the characterization of fibrous materials structured on the micrometer scale. It draws on the ability of X-ray Talbot interferometers to provide full field images of a sample's ultra small angle scattering properties, bridging a gap of multiple orders of magnitude between the imaging resolution and the contrasted structure scale. The correspondence between shape anisotropy and oriented scattering thereby allows to infer orientations within a sample's microstructure below the imaging resolution. First demonstrations have shown the general feasibility of doing so in a tomographic fashion, based on various heuristic signal models and reconstruction approaches. Here, both a verified model of the signal anisotropy and a reconstruction technique practicable for general imaging geometries and large tensor valued volumes is developed based on in-depth reviews of dark-field imaging and tomographic reconstruction techniques. To this end, a wide interdisciplinary field of imaging and reconstruction methodologies is revisited. To begin with, a novel introduction to the mathematical description of perspective projections provides essential insights into the relations between the tangible real space properties of cone beam imaging geometries and their technically relevant description in terms of homogeneous coordinates and projection matrices. Based on these fundamentals, a novel auto-calibration approach is developed, facilitating the practical determination of perspective imaging geometries with minimal experimental constraints. A corresponding generalized formulation of the widely employed Feldkamp algorithm is given, allowing fast and flexible volume reconstructions from arbitrary tomographic imaging geometries. Iterative reconstruction techniques are likewise introduced for general projection geometries, with a particular focus on the efficient evaluation of the forward problem associated with tomographic imaging. A highly performant 3D generalization of Joseph's classic linearly interpolating ray casting algorithm is developed to this end and compared to typical alternatives. With regard to the anisotropic imaging modality required for tensor tomography, X-ray dark-field contrast is extensively reviewed. Previous literature is brought into a joint context and nomenclature and supplemented by original work completing a consistent picture of the theory of dark-field origination. Key results are explicitly validated by experimental data with a special focus on tomography as well as the properties of anisotropic fibrous scatterers. In order to address the pronounced susceptibility of interferometric images to subtle mechanical imprecisions, an efficient optimization based evaluation strategy for the raw data provided by Talbot interferometers is developed. Finally, the fitness of linear tensor models with respect to the derived anisotropy properties of dark-field contrast is evaluated, and an iterative scheme for the reconstruction of tensor valued volumes from projection images is proposed. The derived methods are efficiently implemented and applied to fiber reinforced plastic samples, imaged at the ID19 imaging beamline of the European Synchrotron Radiation Facility. The results represent unprecedented demonstrations of X-ray dark-field tensor tomography at a field of view of 3-4cm, revealing local fiber orientations of both complex shaped and low-contrast samples at a spatial resolution of 0.1mm in 3D. The results are confirmed by an independent micro CT based fiber analysis.}, subject = {Dreidimensionale Rekonstruktion}, language = {en} } @phdthesis{Iff2022, author = {Iff, Oliver}, title = {Implementierung und Charakterisierung von Einzelphotonenquellen in zweidimensionalen Übergangsmetall-Dichalkogeniden und deren Kopplung an optische Resonatoren}, doi = {10.25972/OPUS-28140}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-281404}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {Schon heute bilden Einzelphotonenquellen einen wichtigen Baustein in der Photonik und Quanteninformation. Der Fokus der Forschung liegt entsprechend auf dem Finden und Charakterisieren daf{\"u}r geeigneter Materialsysteme. Konkret beschäftigt sich die vorliegende Arbeit vorwiegend mit dem Übergangsmetall-Dichalkogenid (TMDC1 ) Wolframdiselenid und seinen Eigenschaften. Diese Wahl ist durch den direkte Zugang zu Einzelphotonenquellen begr{\"u}ndet, die sich in dessen Monolagen ausbilden können. Diese Lichtquellen können {\"u}ber eine Modulation der Verspannung der Monolage gezielt aktiviert werden. Durch die, verglichen mit ihrem Volumen, riesige Kontaktfläche lassen sich Monolagen zudem mit Hilfe des Substrats, auf das sie transferiert wurden, wesentlich beeinflussen. Im Rahmen dieser Arbeit wurden Monolagen von WSe2 in unterschiedlichen Bauteilen wie zirkulare Bragg-Gittern oder vorstrukturierten, metallischen Oberflächen implementiert und die Photolumineszenz des TMDCs untersucht. Diese Arbeit belegt die Möglichkeit, Einzelphotonenquellen basierend aufWSe2 -Monolagen auf verschiedenste Weise modulieren zu können. Dank ihrer zwei- dimensionalen Geometrie lassen sie sich einfach in bestehende Strukturen integrieren oder auch in der Zukunft mit weiteren 2D-Materialien kombinieren.}, subject = {Einzelphotonenemission}, language = {de} } @phdthesis{Kissner2022, author = {Kißner, Katharina}, title = {Manipulation of electronic properties in strongly correlated Cerium-based surface alloys}, doi = {10.25972/OPUS-27306}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-273067}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {Photoelectron spectroscopy proves as a versatile tool for investigating various aspects of the electronic structure in strongly correlated electron systems. Influencing the manifestation of strong correlation in Ce-based surface alloys is the main task of this work. It is shown, that the manifestation of the Kondo ground state is influenced by a multitude of parameters such as the choice of the metal binding partner in binary Ce compounds, the surface alloy layer thickness and accompanying variations in the lattice structure as well as the interfaces to substrate or vacuum. Gaining access to these parameters allows to directly influence essential state variables, such as the f level occupancy nf or the Kondo temperature TK. The center of this work are the intermetallic thin films of CePt5/Pt(111) and CeAgx/Ag(111). By utilizing different excitation energies, photoemission spectroscopy provides access to characteristic features of Kondo physics in the valence band, such as the Kondo resonance and its spin-orbit partner at the Fermi level, as well as the multiplet structure of the Ce 3d core levels. In this work both approaches are applied to CePt5/Pt(111) to determine nf and TK for a variety of surface alloy layer thicknesses. A temperature dependent study of the Ce 3d core levels allows to determine the systems TK for the different layer thicknesses. This leads to TK ≈200-270K in the thin layer thickness regime and TK >280K for larger layer thicknesses. These results are confirmed by fitting the Ce 3d multiplet based on the Gunnarsson-Sch{\"o}nhammer formalism for core level spectroscopy and additionally by valence band photoemission spectra of the respective Kondo resonances. The influence of varying layer thickness on the manifestation of strong correlation is subsequently studied for the surface alloy CeAgx/Ag(111). Furthermore, the heavy element Bi is added, to investigate the effects of strong spin-orbit coupling on the electronic structure of the surface alloy.}, subject = {Korrelation}, language = {en} } @phdthesis{Strunz2022, author = {Strunz, Jonas}, title = {Quantum point contacts in HgTe quantum wells}, doi = {10.25972/OPUS-27459}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-274594}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {Quantenpunktkontakte (englisch: quantum point contacts, QPCs) sind eindimensionale Engstellen in einem ansonsten zweidimensionalen Elektronen- oder Lochsystem. Seit der erstmaligen Realisierung in GaAs-basierten zweidimensionalen Elektronengasen sind QPCs sukzessive zu einem Grundbestandteil mesoskopischer Physik geworden und erfahren in einer Vielzahl von Experimenten Anwendung. Jedoch ist es bis zur Anfertigung der vorliegenden Arbeit nicht gelungen, QPCs in der neuen Materialklasse der zweidimensionalen topologischen Isolatoren zu realisieren. In diesen Materialien tritt der sogenannte Quanten-Spin-Hall-Effekt (QSH-Effekt) auf, welcher sich durch die Ausbildung von leitf{\"a}higen, eindimensionalen sowie gleichermaßen spinpolarisierten Zust{\"a}nden an der Bauteilkante auszeichnet, w{\"a}hrend die restlichen Bereiche der Probe isolierend sind. Ein in einem zweidimensionalen topologischen Isolator realisierter QPC kann demgem{\"a}ß daf{\"u}r benutzt werden, die sich stets an der Bauteilkante befindlichen QSH-Randkan{\"a}le einander r{\"a}umlich anzun{\"a}hern, was beispielsweise die Untersuchung potentieller Wechselwirkungseffekte zwischen ebenjenen Randkan{\"a}len erm{\"o}glicht. Die vorliegende Arbeit beschreibt die erstmalig erfolgreich durchgef{\"u}hrte Implementierung einer QPC-Technologie in einem QSH-System. {\"U}berdies werden die neuartigen Bauteile experimentell charakterisiert sowie analysiert. Nach einer in Kapitel 1 erfolgten Einleitung der Arbeit besch{\"a}ftigt sich das nachfolgende Kapitel 2 zun{\"a}chst mit der besonderen Bandstruktur von HgTe. In diesem Kontext wird die Ausbildung der QSH-Phase f{\"u}r HgTe-Quantentr{\"o}ge mit einer invertierten Bandstruktur erl{\"a}utert, welche f{\"u}r deren Auftreten eine Mindesttrogdicke von d_QW > d_c = 6.3 nm aufweisen m{\"u}ssen. Im Anschluss wird das Konzept eines QPCs allgemein eingef{\"u}hrt sowie das zugeh{\"o}rige Transportverhalten analytisch beschrieben. {\"U}berdies werden die Einschr{\"a}nkungen und Randbedingungen diskutiert, welche bei der Realisierung eines QPCs in einem QSH-System Ber{\"u}cksichtigung finden m{\"u}ssen. Darauf folgt die Pr{\"a}sentation des eigens zur QPC-Herstellung entwickelten Lithographieprozesses, welcher auf einer mehrstufigen Anwendung eines f{\"u}r HgTe-Quantentrogstrukturen geeigneten nasschemischen {\"A}tzverfahrens beruht. Die im Nachgang diskutierten Transportmessungen exemplarischer Proben zeigen die erwartete Leitwertquantisierung in Schritten von ΔG ≈ 2e^2/h im Bereich des Leitungsbandes -- sowohl f{\"u}r eine topologische als auch f{\"u}r eine triviale (d_QW < d_c) QPC-Probe. Mit dem Erreichen der Bandl{\"u}cke saturiert der Leitwert f{\"u}r den topologischen QPC um G_QSH ≈ 2e^2/h, wohingegen ebenjener f{\"u}r den Fall des trivialen Bauteils auf G ≈ 0 abf{\"a}llt. Dar{\"u}ber hinaus belegen durchgef{\"u}hrte Messungen des differentiellen Leitwertes einer invertierten QPC-Probe in Abh{\"a}ngigkeit einer Biasspannung die stabile Koexistenz von topologischen und trivialen Transportmoden. Gegenstand von Kapitel 3 ist die Beschreibung der Ausbildung eines QSH-Interferometers in QPCs mit geringer Weite, welche unter Verwendung von Quantentr{\"o}gen mit einer Trogdicke von d_QW = 7 nm hergestellt werden. Die Diskussion von Bandstrukturrechnungen legt dar, dass die r{\"a}umliche Ausdehnung der Randkan{\"a}le von der jeweiligen Position der Fermi-Energie im Bereich der Bandl{\"u}cke abh{\"a}ngt. Hieraus resultiert eine Transportsituation, in welcher -- unter bestimmten Voraussetzungen -- Reservoir-Elektronen mit randomisiertem Spin an beide QSH-Randkan{\"a}le mit gleicher Wahrscheinlichkeit koppeln, was in der Ausbildung eines QSH-Rings resultiert. Diese Ringbildung wird im Rahmen eines durch Plausibilit{\"a}ts{\"u}berpr{\"u}fung getesteten Modells erkl{\"a}rt und spezifiziert. Danach erfolgt eine theoretische Einf{\"u}hrung von drei relevanten Quantenphasen, deren Akkumulation in der Folge f{\"u}r mehrere geeignete QPC-Proben nachgewiesen wird. Es handelt sich hierbei um die Aharonov-Bohm-Phase, um die dynamische Aharonov-Casher-Phase sowie um eine Spin-Bahn-Berry-Phase mit einem Wert von π. Diese experimentellen Ergebnisse stehen dar{\"u}ber hinaus im Einklang mit analytischen Modellbetrachtungen. Das anschließende Kapitel 4 stellt den letzten Teil der Arbeit dar und besch{\"a}ftigt sich mit der Beobachtung einer anomalen Leitwertsignatur, welche f{\"u}r QPC-Proben basierend auf einer Quantentrogdicke von d_QW = 10.5 nm auftritt. Diese Proben zeigen neben der durch die QSH-Phase bedingten Leitwertquantisierung von G_QSH ≈ 2e^2/h ein weiteres Leitwertplateau mit einem Wert von G ≈ e^2/h = 0.5 x G_QSH. Diese sogenannte 0.5-Anomalie ist nur f{\"u}r ein kleines Intervall von QPC-Weiten beobachtbar und wird mit zunehmender Bauteilweite abgeschw{\"a}cht. Weiterf{\"u}hrende Untersuchungen in Abh{\"a}ngigkeit der Temperatur sowie einer angelegten Biasspannung deuten dar{\"u}ber hinaus darauf hin, dass das Auftreten der 0.5-Anomalie mit einem modifizierten topologischen Zustand einhergeht. {\"U}berdies wird eine zus{\"a}tzliche sowie vervollst{\"a}ndigende Charakterisierung dieses Transportregimes durch die Realisierung eines neuartigen Bauteilkonzeptes m{\"o}glich, welches einen QPC in eine standardisierte Hall-Bar-Geometrie integriert. Das Ergebnis der experimentellen Analyse einer solchen Probe verkn{\"u}pft das Auftreten der 0.5-Anomalie mit der R{\"u}ckstreuung eines QSH-Randkanals. Demgem{\"a}ß wird aus Sicht des Einteilchenbildes geschlussfolgert, dass im Kontext der 0.5-Anomalie lediglich ein Randkanal transmittiert wird. Zudem werden zwei theoretische Modelle basierend auf Elektron-Elektron-Wechselwirkungen diskutiert, welche beide jeweils als urs{\"a}chlicher Mechanismus f{\"u}r das Auftreten der 0.5-Anomalie in Frage kommen. Abschließend ist zu deduzieren, dass die Implementierung einer QPC-Technologie in einem QSH-System eine bedeutende Entwicklung im Bereich der Erforschung von zweidimensionalen topologischen Isolatoren darstellt, welche eine Vielzahl zuk{\"u}nftiger Experimente erm{\"o}glicht. So existieren beispielsweise theoretische Vorhersagen, dass QPCs in einem QSH-System die Detektion von Majorana- sowie Para-Fermionen erm{\"o}glichen. {\"U}berdies ist die nachgewiesene Ausbildung eines QSH-Interferometers in geeigneten QPC-Proben eine Beobachtung von großer Folgewirkung. So erm{\"o}glicht die beobachtete dynamische Aharonov-Casher-Phase im QSH-Regime die kontrollierbare Modulation des topologischen Leitwertes, was die konzeptionelle Grundlage eines topologischen Transistors darstellt. Eine weitere Anwendungsm{\"o}glichkeit wird durch die Widerstandsf{\"a}higkeit geometrischer Phasen gegen{\"u}ber Dephasierung er{\"o}ffnet, wodurch die nachgewiesene Spin-Bahn-Berry-Phase mit einem Wert von π im Kontext potentieller Quantencomputerkonzepte von Interesse ist. Dar{\"u}ber hinaus ist die Transmission von nur einem QSH-Randkanal im Zuge des Auftretens der 0.5-Anomalie {\"a}quivalent zu 100 \% Spinpolarisierung, was einen Faktor essentieller Relevanz f{\"u}r die Realisierung spintronischer Anwendungen darstellt. Demgem{\"a}ß beinhaltet die vorliegende Arbeit den experimentellen Nachweis von drei unterschiedlichen Effekten, von welchen jedem einzelnen eine fundamentale Rolle im Rahmen der Entwicklung neuer Generationen logischer Bauelemente zukommen kann -- erm{\"o}glicht durch die Realisierung von QPCs in topologischen HgTe-Quantentr{\"o}gen.}, subject = {Topologischer Isolator}, language = {en} } @phdthesis{Gottscholl2022, author = {Gottscholl, Andreas Paul}, title = {Optical Accessible Spin Defects in Hexagonal Boron Nitride: Identification, Control and Application of the Negatively Charged Boron Vacancy VB-}, doi = {10.25972/OPUS-27432}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-274326}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {In this work, a bridge was built between the so-far separate fields of spin defects and 2D systems: for the first time, an optically addressable spin defect (VB-) in a van der Waals material (hexagonal boron nitride) was identified and exploited. The results of this thesis are divided into three topics as follows: 1.) Identification of VB-: In the scope of this chapter, the defect ,the negatively charged boron vacancy VB-, is identified and characterized. An initialization and readout of the spin state can be demonstrated optically at room temperature and its spin Hamiltonian contributions can be quantified. 2.) Coherent Control of VB-: A coherent control is required for the defect to be utilized for quantum applications, which}, subject = {Bornitrid}, language = {en} } @phdthesis{Suchomel2022, author = {Suchomel, Holger Maximilian}, title = {Entwicklung elektrooptischer Bauteile auf der Basis von Exziton-Polaritonen in Halbleiter-Mikroresonatoren}, doi = {10.25972/OPUS-27163}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-271630}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {Exziton-Polaritonen (Polaritonen), hybride Quasiteilchen, die durch die starke Kopplung von Quantenfilm-Exzitonen mit Kavit{\"a}tsphotonen entstehen, stellen auf Grund ihrer vielseitigen und kontrollierbaren Eigenschaften einen vielversprechenden Kandidaten f{\"u}r die Entwicklung einer neuen Generation von nichtlinearen und integrierten elektrooptischen Bauteilen dar. Die vorliegende Arbeit besch{\"a}ftigt sich mit der Entwicklung und Untersuchung kompakter elektrooptischer Bauelemente auf der Basis von Exziton-Polaritonen in Halbleitermikrokavit{\"a}ten. Als erstes wird die Implementierung einer elektrisch angeregten, oberfl{\"a}chenemittierenden Polariton-Laserdiode vorgestellt, die ohne ein externes Magnetfeld arbeiten kann. Daf{\"u}r wird der Schichtaufbau, der Q-Faktor, das Dotierprofil und die RabiAufspaltung der Polariton-Laserdiode optimiert. Der Q-Faktor des finalen Aufbaus bel{\"a}uft sich auf Q ~ 16.000, w{\"a}hrend die Rabi-Aufspaltung im Bereich von ~ 11,0 meV liegt. Darauf aufbauend werden Signaturen der Polariton-Kondensation unter elektrischer Anregung, wie ein nichtlinearer Anstieg der Intensit{\"a}t, die Reduktion der Linienbreite und eine fortgesetzte Verschiebung der Emission zu h{\"o}heren Energien oberhalb der ersten Schwelle, demonstriert. Ferner werden die Koh{\"a}renzeigenschaften des Polariton-Kondensats mittels Interferenzspektroskopie untersucht. Basierend auf den optimierten Halbleiter-Mikroresonatoren wird eine Kontaktplattform f{\"u}r die elektrische Anregung ein- und zweidimensionaler Gitterstrukturen entwickelt. Dazu wird die Bandstrukturbildung eines Quadrat- und Graphen-Gitters unter elektrischer Anregung im linearen Regime untersucht und mit den Ergebnissen der optischen Charakterisierung verglichen. Die erhaltenen Dispersionen lassen sich durch das zugeh{\"o}rige Tight-Binding-Modell beschreiben. Ferner wird auch eine elektrisch induzierte Nichtlinearit{\"a}t in der Emission demonstriert. Die untersuchte Laser-Mode liegt auf der H{\"o}he des unteren Flachbandes und an der Position der Γ-Punkte in der zweiten Brillouin-Zone. Die zugeh{\"o}rige Modenstruktur weist die erwartete Kagome-Symmetrie auf. Abschließend wird die Bandstrukturbildung eines SSH-Gitters mit eingebautem Defekt unter elektrischer Anregung untersucht und einige Eigenschaften des topologisch gesch{\"u}tzten Defektzustandes gezeigt. Dazu geh{\"o}rt vor allem die Ausbildung der lokalisierten Defektmode in der Mitte der S-Bandl{\"u}cke. Die erhaltenen Ergebnisse stellen einen wichtigen Schritt in der Realisierung eines elektrisch betriebenen topologischen Polariton-Lasers dar. Abschließend wird ein elektrooptisches Bauteil auf der Basis von Polaritonen in einem Mikrodrahtresonator vorgestellt, in dem sich die Propagation eines PolaritonKondensats mittels eines elektrostatischen Feldes kontrollieren l{\"a}sst. Das Funktionsprinzip des Polariton-Schalters beruht auf der Kombination einer elektrostatischen Potentialsenke unterhalb des Kontaktes und der damit verbundenen erh{\"o}hten ExzitonIonisationsrate. Der Schaltvorgang wird sowohl qualitativ als auch quantitativ analysiert und die Erhaltenen Ergebnisse durch die Modellierung des Systems {\"u}ber die GrossPitaevskii-Gleichung beschrieben. Zus{\"a}tzlich wird ein negativer differentieller Widerstand und ein bistabiles Verhalten in der Strom-Spannungs-Charakteristik in Abh{\"a}ngigkeit von der Ladungstr{\"a}gerdichte im Kontaktbereich beobachtet. Dieses Verhalten wird auf gegenseitig konkurrierende Kondensats-Zust{\"a}nde innerhalb der Potentialsenke und deren Besetzung und damit direkt auf den r{\"a}umlichen Freiheitsgrad der PolaritonZust{\"a}nde zur{\"u}ckgef{\"u}hrt.}, subject = {Drei-F{\"u}nf-Halbleiter}, language = {de} } @phdthesis{Heinrich2022, author = {Heinrich, Robert}, title = {Multi-species gas detection based on an external-cavity quantum cascade laser spectrometer in the mid-infrared fingerprint region}, doi = {10.25972/OPUS-26864}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-268640}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {Laser spectroscopic gas sensing has been applied for decades for several applications as atmospheric monitoring, industrial combustion gas analysis or fundamental research. The availability of new laser sources in the mid-infrared opens the spectral fingerprint range to the technology where multiple molecules possess their fundamental ro-vibrational absorption features that allow very sensitive detection and accurate discrimination of the species. The increasing maturity of quantum cascade lasers that cover this highly interesting spectral range motivated this research to gain fundamental knowledge about the spectra of hydrocarbon gases in pure composition and in complex mixtures as they occur in the petro-chemical industry. The long-term target of developing accurate and fast hydrocarbon gas analyzers, capable of real-time operation while enabling feedback-loops, would lead to a paradigm change in this industry. This thesis aims to contribute to a higher accuracy and more comprehensive understanding of the sensing of hydrocarbon gas mixtures. This includes the acquisition of yet unavailable high resolution and high accuracy reference spectra of the respective gases, the investigation of their spectral behavior in mixtures due to collisional broadening of their transitions and the verification of the feasibility to quantitatively discriminate the spectra when several overlapping species are simultaneously measured in gas mixtures. To achieve this knowledge a new laboratory environment was planned and built up to allow for the supply of the individual gases and their arbitrary mixing. The main element was the development of a broadly tunable external-cavity quantum cascade laser based spectrometer to record the required spectra. This also included the development of a new measurement method to obtain highly resolved and nearly gap-less spectral coverage as well as a sophisticated signal post-processing that was crucial to achieve the high accuracy of the measurements. The spectroscopic setup was used for a thorough investigation of the spectra of the first seven alkanes as of their mixtures. Measurements were realized that achieved a spectral resolution of 0.001 cm-1 in the range of 6-11 µm while ensuring an accuracy of 0.001 cm-1 of the spectra and attaining a transmission sensitivity of 2.5 x 10-4 for long-time averaging of the acquired spectra. These spectral measurements accomplish a quality that compares to state-of-the art spectral databases and revealed so far undocumented details of several of the investigated gases that have not been measured with this high resolution before at the chosen measurement conditions. The results demonstrate the first laser spectroscopic discrimination of a seven component gas mixture with absolute accuracies below 0.5 vol.\% in the mid-infrared provided that a sufficiently broad spectral range is covered in the measurements. Remaining challenges for obtaining improved spectral models of the gases and limitations of the measurement accuracy and technology are discussed.}, subject = {Quantenkaskadenlaser}, language = {en} } @phdthesis{Betzold2022, author = {Betzold, Simon}, title = {Starke Licht-Materie-Wechselwirkung und Polaritonkondensation in hemisph{\"a}rischen Mikrokavit{\"a}ten mit eingebetteten organischen Halbleitern}, doi = {10.25972/OPUS-26665}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-266654}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {Kavit{\"a}ts-Exziton-Polaritonen (Polaritonen) sind hybride Quasiteilchen, die sich aufgrund starker Kopplung von Halbleiter-Exzitonen mit Kavit{\"a}tsphotonen ausbilden. Diese Quasiteilchen weisen eine Reihe interessanter Eigenschaften auf, was sie einerseits f{\"u}r die Grundlagenforschung, andererseits auch f{\"u}r die Entwicklung neuartiger Bauteile sehr vielversprechend macht. Bei Erreichen einer ausreichend großen Teilchendichte geht das System in den Exziton-Polariton-Kondensationszustand {\"u}ber, was zur Emission von laserartigem Licht f{\"u}hrt. Organische Halbleiter als aktives Emittermaterial zeigen in diesem Kontext großes Potential, da deren Exzitonen neben großen Oszillatorst{\"a}rken auch hohe Bindungsenergien aufweisen. Deshalb ist es m{\"o}glich, unter Verwendung organischer Halbleiter selbst bei Umgebungsbedingungen {\"a}ußerst stabile Polaritonen zu erzeugen. Eine wichtige Voraussetzung zur Umsetzung von integrierten opto-elektronischen Bauteilen basierend auf Polaritonen ist der kontrollierte r{\"a}umliche Einschluss sowie die Realisierung von frei konfigurierbaren Potentiallandschaften. Diese Arbeit besch{\"a}ftigt sich mit der Entwicklung und der Untersuchung geeigneter Plattformen zur Erzeugung von Exziton-Polaritonen und Polaritonkondensaten in hemisph{\"a}rischen Mikrokavit{\"a}ten, in die organische Halbleiter eingebettet sind.}, subject = {Exziton-Polariton}, language = {de} } @phdthesis{Schmitt2022, author = {Schmitt, Matthias}, title = {High Energy Spin- and Momentum-Resolved Photoelectron Spectroscopy of Complex Oxides}, doi = {10.25972/OPUS-26475}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-264757}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {Spin- and \(k\)-resolved hard X-ray photoelectron spectroscopy (HAXPES) is a powerful tool to probe bulk electronic properties of complex metal oxides. Due to the low efficiency of common spin detectors of about \(10^{-4}\), such experiments have been rarely performed within the hard X-ray regime since the notoriously low photoionization cross sections further lower the performance tremendously. This thesis is about a new type of spin detector, which employs an imaging spin-filter with multichannel electron recording. This increases the efficiency by a factor of \(10^4\) and makes spin- and \(k\)-resolved photoemission at high excitation energies possible. Two different technical approaches were pursued in this thesis: One using a hemispherical deflection analyzer (HDA) and a separate external spin detector chamber, the other one resorting to a momentum- or \(k\)-space microscope with time-of-flight (TOF) energy recording and an integrated spin-filter crystal. The latter exhibits significantly higher count rates and - since it was designed for this purpose from scratch - the integrated spin-filter option found out to be more viable than the subsequent upgrade of an existing setup with an HDA. This instrumental development is followed by the investigation of the complex metal oxides (CMOs) KTaO\(_3\) by angle-resolved HAXPES (HARPES) and Fe\(_3\)O\(_4\) by spin-resolved HAXPES (spin-HAXPES), respectively. KTaO\(_3\) (KTO) is a band insulator with a valence-electron configuration of Ta 5\(d^0\). By angle- and spin-integrated HAXPES it is shown that at the buried interface of LaAlO\(_3\)/KTO - by the generation of oxygen vacancies and hence effective electron doping - a conducting electron system forms in KTO. Further investigations using the momentum-resolution of the \(k\)-space TOF microscope show that these states are confined to the surface in KTO and intensity is only obtained from the center or the Gamma-point of each Brillouin zone (BZ). These BZs are furthermore square-like arranged reflecting the three-dimensional cubic crystal structure of KTO. However, from a comparison to calculations it is found that the band structure deviates from that of electron-doped bulk KTaO\(_3\) due to the confinement to the interface. There is broad consensus that Fe\(_3\)O\(_4\) is a promising material for spintronics applications due to its high degree of spin polarization at the Fermi level. However, previous attempts to measure the spin polarization by spin-resolved photoemission spectroscopy have been hampered by the use of low photon energies resulting in high surface sensitivity. The surfaces of magnetite, though, tend to reconstruct due to their polar nature, and thus their magnetic and electronic properties may strongly deviate from each other and from the bulk, dependent on their orientation and specific preparation. In this work, the intrinsic bulk spin polarization of magnetite at the Fermi level (\(E_F\)) by spin-resolved photoelectron spectroscopy, is determined by spin-HAXPES on (111)-oriented thin films, epitaxially grown on ZnO(0001) to be \(P(E_F) = -80^{+10}_{-20}\) \%.}, subject = {Elektronenkorrelation}, language = {en} } @phdthesis{Reis2022, author = {Reis, Felix}, title = {Realization and Spectroscopy of the Quantum Spin Hall Insulator Bismuthene on Silicon Carbide}, doi = {10.25972/OPUS-25825}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-258250}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {Topological matter is one of the most vibrant research fields of contemporary solid state physics since the theoretical prediction of the quantum spin Hall effect in graphene in 2005. Quantum spin Hall insulators possess a vanishing bulk conductivity but symmetry-protected, helical edge states that give rise to dissipationless charge transport. The experimental verification of this exotic state of matter in 2007 lead to a boost of research activity in this field, inspired by possible ground-breaking future applications. However, the use of the quantum spin Hall materials available to date is limited to cryogenic temperatures owing to their comparably small bulk band gaps. In this thesis, we follow a novel approach to realize a quantum spin Hall material with a large energy gap and epitaxially grow bismuthene, i.e., Bi atoms adopting a honeycomb lattice, in a \((\sqrt{3}\times\sqrt{3})\) reconstruction on the semiconductor SiC(0001). In this way, we profit both from the honeycomb symmetry as well as the large spin-orbit coupling of Bi, which, in combination, give rise to a topologically non-trivial band gap on the order of one electronvolt. An in-depth theoretical analysis demonstrates that the covalent bond between the Si and Bi atoms is not only stabilizing the Bi film but is pivotal to attain the quantum spin Hall phase. The preparation of high-quality, unreconstructed SiC(0001) substrates sets the basis for the formation of bismuthene and requires an extensive procedure in ultra-pure dry H\(_2\) gas. Scanning tunneling microscopy measurements unveil the (\(1\times1\)) surface periodicity and smooth terrace planes, which are suitable for the growth of single Bi layers by means of molecular beam epitaxy. The chemical configuration of the resulting Bi film and its oxidation upon exposure to ambient atmosphere are inspected with X-ray photoelectron spectroscopy. Angle-resolved photoelectron spectroscopy reveals the excellent agreement of probed and calculated band structure. In particular, it evidences a characteristic Rashba-splitting of the valence bands at the K point. Scanning tunneling spectroscopy probes signatures of this splitting, as well, and allows to determine the full band gap with a magnitude of \(E_\text{gap}\approx0.8\,\text{eV}\). Constant-current images and local-density-of-state maps confirm the presence of a planar honeycomb lattice, which forms several domains due to different, yet equivalent, nucleation sites of the (\(\sqrt{3}\times\sqrt{3}\))-Bi reconstruction. Differential conductivity measurements demonstrate that bismuthene edge states evolve at atomic steps of the SiC substrate. The probed, metallic local density of states is in agreement with the density of states expected from the edge state's energy dispersion found in density functional theory calculations - besides a pronounced dip at the Fermi level. By means of temperature- and energy-dependent tunneling spectroscopy it is shown that the spectral properties of this suppressed density of states are successfully captured in the framework of the Tomonaga-Luttinger liquid theory and most likely originate from enhanced electronic correlations in the edge channel.}, subject = {Zweidimensionales Material}, language = {en} } @phdthesis{Mueller2022, author = {M{\"u}ller, Valentin Leander}, title = {Transport signatures of topological and trivial states in the three-dimensional topological insulator HgTe}, doi = {10.25972/OPUS-25952}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-259521}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {The thesis at hand is concerned with improving our understanding of and our control over transport properties of the three-dimensional topological insulator HgTe. Topological insulators are characterized by an insulating bulk and symmetry-protected metallic surface states. These topological surface states hold great promise for research and technology; at the same time, many properties of experimentally accessible topological insulator materials still need to be explored thoroughly. The overall aim of this thesis was to experimentally investigate micrometer-sized HgTe transport devices to observe the ballistic transport regime as well as intercarrier scattering and possibly identify special properties of the topological surface states. Part I of the thesis presents lithographic developments concerned with etching small HgTe devices. The aim was to replace existing processes which relied on dry etching with high-energy \(\text{Ar}^+\) ions and an organic etch mask. This etching method is known to degrade the HgTe crystal quality. In addition, the etch mask turned out to be not durable for long etching processes and difficult to remove completely after etching. First, \(\text{BaF}_2\) was introduced as a new etch mask for dry etching to replace the organic etch mask. With common surface characterization techniques like SEM and XPS it was shown that \(\text{BaF}_2\) etch masks are easy to deposit, highly durable in common dry etching processes for \(\text{Hg}_{1-x}\text{Cd}_x\text{Te}\), and easy to remove in deionized water. Transport results of HgTe devices fabricated with the new etch mask are comparable to results obtained with the old process. At the same time, the new etch mask can withstand longer etching times and does not cause problems due to incomplete removal. Second, a new inductively coupled plasma dry etching process based on \(\text{CH}_4\) and Ar was introduced. This etching process is compatible with \(\text{BaF}_2\) etch masks and yields highly reproducible results. Transport results indicate that the new etching process does not degrade the crystal quality and is suitable to produce high-quality transport devices even in the micrometer range. A comparison with wet-etched samples shows that inductively coupled plasma etching introduces a pronounced edge roughness. This - usually undesirable - property is actually beneficial for some of the experiments in this study and mostly irrelevant for others. Therefore, most samples appearing in this thesis were fabricated with the new process. Part II of the thesis details the advancements made in identifying topological and trivial states which contribute to transport in HgTe three-dimensional topological insulators. To this end, macroscopic Hall bar samples were fabricated from high-quality tensilely strained HgTe layers by means of the improved lithographic processes. All samples were equipped with a top gate electrode, and some also with a modulation doping layer or a back gate electrode to modify the carrier density of the surface states on both sides of the HgTe layer. Due to the high sample quality, Landau levels could be well-resolved in standard transport measurements down to magnetic fields of less than 0.5T. High-resolution measurements of the Landau level dispersion with gate voltage and magnetic field allowed disentangling different transport channels. The main result here is that the upper (electron) branches of the two topological surface states contribute to transport in all experimentally relevant density regimes, while the hole branch is not accessible. Far in n-regime bulk conduction band states give a minor contribution to transport. More importantly, trivial bulk valence band holes come into play close to the charge neutrality point. Further in p-regime, the strong applied gate voltage leads to the formation of two-dimensional, massive hole states at the HgTe surface. The interplay of different states gives rise to rich physics: Top gate-back gate maps revealed that an anticrossing of Landau levels from the two topological surface states occurs at equal filling. A possible explanation for this effect is a weak hybridization of the surface states; however, future studies need to further clarify this point. Furthermore, the superposition of n-type topological and p-type trivial surface states leads to an intriguing Landau level dispersion. The good quantization of the Hall conductance in this situation indicates that the counterpropagating edge states interact with each other. The nature of this interaction will be the topic of further research. Part III of the thesis is focused on HgTe microstructures. These "channel samples" have a typical width of 0.5 to 4µm and a typical length of 5 to 80µm. The quality of these devices benefits particularly from the improved lithographic processes. As a result, the impurity mean free path of the topological surface state electrons is on the order of the device width and transport becomes semiballistic. This was verified by measuring the channel resistance in small magnetic fields in n-regime. The deflection of carriers towards the dissipative channel walls results in a pronounced peak in the magnetoresistance, which scales in a predictable manner with the channel width. To investigate transport effects due to mutual scattering of charge carriers, the differential resistance of channel samples was measured as a function of carrier temperature. Selective heating of the charge carriers - but not the lattice - was achieved by passing a heating current through the channel. Increasing the carrier temperature has two pronounced effects when the Fermi level is situated in proximity to the bulk valence band maximum where the density of states is large. First, when both topological surface state electrons and bulk holes are present, electron-hole scattering leads to a pronounced increase in resistance with increasing carrier temperature. Second, a thermally induced increase of the electron and hole carrier densities reduces the resistance again at higher temperatures. A model considering these two effects was developed, which can well reproduce the experimental results. Current heating experiments in zero-gap HgTe quantum wells and compressively strained HgTe layers are consistent with this model. These observations raise the question as to how electron-hole scattering may affect other transport properties of HgTe-based three-dimensional topological insulators, which is briefly discussed in the outlook.}, subject = {Topologischer Isolator}, language = {en} } @phdthesis{Hoecker2022, author = {H{\"o}cker, Julian Harald}, title = {High-quality Organolead Trihalide Perovskite Crystals: Growth, Characterisation, and Photovoltaic Applications}, doi = {10.25972/OPUS-25859}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-258590}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {Overview of the Organolead Trihalide Perovskite Crystal Area Studies of perovskite single crystals with high crystallographic quality is an important technological area of the perovskite research, which enables to estimate their full optoelectronic potential, and thus to boost their future applications [26]. It was therefore essential to grow high-quality single crystals with lowest structural as well as chemical defect densities and with a stoichiometry relevant for their thin-film counterparts [26]. Optoelectronic devices, e.g. solar cells, are highly complex systems in which the properties of the active layer (absorber) are strongly influenced by the adjacent layers, so it is not always easy to define the targeted properties and elaborate the design rules for the active layer. Currently, organolead trihalide perovskite (OLTP) single crystals with the structure ABX3 are one of the most studied crystalline systems. These hybrid crystals are solids composed of an organic cation such as methylammonium (A = MA+) or formamidinium (A = FA+) to form a three-dimensional periodic lattice together with the lead cation (B = Pb2+) and a halogen anion such as chloride, bromide or iodide (X = Cl-, Br- or I-) [23]. Among them are methylammonium lead tribromide (MAPbBr3), methylammonium lead triiodide (MAPbI3), as well as methylammonium lead trichloride (MAPbCl3) [62, 63]. Important representatives with the larger cation FA+ are formamidinium lead tribromide (FAPbBr3) and formamidinium lead triiodide (FAPbI3) [23, 64]. Besides the exchange of cations as well as anions, it was possible to grow crystals containing two halogens to obtain mixed crystals with different proportions of chlorine to bromine and bromine to iodine, as it is shown in Figure 70. By varying the mixing ratio of the halogens, it was therefore possible to vary the colour and thus the absorption properties of the crystals [85], as it can be done with thin polycrystalline perovskite films. In addition, since a few years it is also doable to grow complex crystals that contain several cations as well as anions [26, 80, 81]. These include the perovskites double cation - double halide formamidinium lead triiodide - methylammonium lead tribromide (FAPbI3)0.9(MAPbBr3)0.1 (FAMA) [26, 80] and formamidinium lead triiodide - methylammonium lead tribromide - caesium lead tribromide (FAPbI3)0.9(MAPbBr3)0.05(CsPbBr3)0.05 (CsFAMA) [81], which have made a significant contribution to increase the power conversion efficiency (PCE) in thin-film photovoltaics [47, 79, 182]. The growth of crystals to this day is performed exclusively from solution [23, 26, 56, 62]. Important preparation methods are the cooling acid-based precursor solution crystallisation [22], the inverse temperature crystallisation (ITC) [62], and the antisolvent vapour-assistant crystallisation (AVC) [137]. In the cooling crystallisation, the precursor salts AX and PbX2 are dissolved in an aqueous halogen-containing acid at high temperatures [56]. Controlled and slow cooling finally results in a supersaturated precursor solution, which leads to spontaneous nucleation of crystal nuclei, followed by subsequent crystal growth. The ITC method is based on the inverse or retrograde solubility of a dissociated perovskite in an organic solvent [23, 64]. With increasing temperature, the solubility of the perovskite decreases and mm-sized crystals can be grown within a few hours [23]. In the AVC method, the precursors are also dissolved in an organic solvent as well [137]. By slow evaporation of a so-called antisolvent [137], the solubility of the perovskite in the now present solvent mixture decreases and it finally precipitates. In addition, there are many other methods with the goal of growing high quality and large crystals in a short period of time [60, 61, 233, 310].}, subject = {Perowskit}, language = {en} } @phdthesis{Harder2022, author = {Harder, Tristan H.}, title = {Topological Modes and Flatbands in Microcavity Exciton-Polariton Lattices}, doi = {10.25972/OPUS-25900}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-259008}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {The fascination of microcavity exciton-polaritons (polaritons) rests upon the combination of advanced technological control over both the III-V semiconductor material platform as well as the precise spectroscopic access to polaritonic states, which provide access to the investigation of open questions and complex phenomena due to the inherent nonlinearity and direct spectroscopic observables such as energy-resolved real and Fourier space information, pseudospin and coherence. The focus of this work was to advance the research area of polariton lattice simulators with a particular emphasis on their lasing properties. Following the brief introduction into the fundamental physics of polariton lattices in chapter 2, important aspects of the sample fabrication as well as the Fourier spectroscopy techniques used to investigate various features of these lattices were summarized in chapter 3. Here, the implementation of a spatial light modulator for advanced excitation schemes was presented. At the foundation of this work is the capability to confine polaritons into micropillars or microtraps resulting in discrete energy levels. By arranging these pillars or traps into various lattice geometries and ensuring coupling between neighbouring sites, polaritonic band structures were engineered. In chapter 4, the formation of a band structure was visualised in detail by investigating ribbons of honeycomb lattices. Here, the transition of the discrete energy levels of a single chain of microtraps to the fully developed band structure of a honeycomb lattice was observed. This study allows to design the size of individual domains in more complicated lattice geometries such that a description using band structures becomes feasible, as it revealed that a width of just six unit cells is sufficient to reproduce all characteristic features of the S band of a honeycomb lattice. In particular in the context of potential technological applications in the realms of lasing, the laser-like, coherent emission from polariton microcavities that can be achieved through the excitation of polariton condensates is intriguing. The condensation process is significantly altered in a lattice potential environment when compared to a planar microcavity. Therefore, an investigation of the polariton condensation process in a lattice with respect to the characteristics of the excitation laser, the exciton-photon detuning as well as the reduced trap distance that represents a key design parameter for polaritonic lattices was performed. Based on the demonstration of polariton condensation into multiple bands, the preferred condensation into a desired band was achieved by selecting the appropriate detuning. Additionally, a decreased condensation threshold in confined systems compared to a planar microcavity was revealed. In chapter 5, the influence of the peculiar feature of flatbands arising in certain lattice geometries, such as the Lieb and Kagome lattices, on polaritons and polariton condensates was investigated. Deviations from a lattice simulator described by a tight binding model that is solely based on nearest neighbour coupling cause a remaining dispersiveness of the flatbands along certain directions of the Brillouin zone. Therefore, the influence of the reduced trap distance on the dispersiveness of the flatbands was investigated and precise technological control over the flatbands was demonstrated. As next-nearest neighbour coupling is reduced drastically by increasing the distance between the corresponding traps, increasing the reduced trap distance enables to tune the S flatbands of both Lieb and Kagome lattices from dispersive bands to flatbands with a bandwidth on the order of the polariton linewidth. Additionally to technological control over the band structures, the controlled excitation of large condensates, single compact localized state (CLS) condensates as well as the resonant excitation of polaritons in a Lieb flatband were demonstrated. Furthermore, selective condensation into flatbands was realised. This combination of technological and spectroscopic control illustrates the capabilities of polariton lattice simulators and was used to study the coherence of flatband polariton condensates. Here, the ability to tune the dispersiveness from a dispersive band to an almost perfect flatband in combination with the selectivity of the excitation is particularly valuable. By exciting large flatband condensates, the increasing degree of localisation to a CLS with decreasing dispersiveness was demonstrated by measurements of first order spatial coherence. Furthermore, the first order temporal coherence of CLS condensates was increased from τ = 68 ps for a dispersive flatband, a value typically achieved in high-quality microcavity samples, to a remarkable τ = 459 ps in a flatband with a dispersiveness below the polarion linewidth. Corresponding to this drastic increase of the first order coherence time, a decrease of the second order temporal coherence function from g(2)(τ =0) = 1.062 to g(2)(0) = 1.035 was observed. Next to laser-like, coherent emission, polariton condensates can form vortex lattices. In this work, two distinct vortex lattices that can form in polariton condensates in Kagome flatbands were revealed. Furthermore, chiral, superfluid edge transport was realised by breaking the spatial symmetry through a localised excitation spot. This chirality was related to a change in the vortex orientation at the edge of the lattice and thus opens the path towards further investigations of symmetry breaking and chiral superfluid transport in Kagome lattices. Arguably the most influential concept in solid-state physics of the recent decades is the idea of topological order that has also provided a new degree of freedom to control the propagation of light. Therefore, in chapter 6, the interplay of topologically non-trivial band structures with polaritons, polariton condensates and lasing was emphasised. Firstly, a two-dimensional exciton-polariton topological insulator based on a honeycomb lattice was realised. Here, a topologically non-trivial band gap was opened at the Dirac points through a combination of TE-TM splitting of the photonic mode and Zeeman splitting of the excitonic mode. While the band gap is too small compared to the linewidth to be observed in the linear regime, the excitation of polariton condensates allowed to observe the characteristic, topologically protected, chiral edge modes that are robust against scattering at defects as well as lattice corners. This result represents a valuable step towards the investigation of non-linear and non-Hermitian topological physics, based on the inherent gain and loss of microcavities as well as the ability of polaritons to interact with each other. Apart from fundamental interest, the field of topological photonics is driven by the search of potential technological applications, where one direction is to advance the development of lasers. In this work, the starting point towards studying topological lasing was the Su-Schrieffer-Heeger (SSH) model, since it combines a simple and well-understood geometry with a large topological gap. The coherence properties of the topological edge defect of an SSH chain was studied in detail, revealing a promising degree of second order temporal coherence of g(2)(0) = 1.07 for a microlaser with a diameter of only d = 3.5 µm. In the context of topological lasing, the idea of using a propagating, topologically protected mode to ensure coherent coupling of laser arrays is particularly promising. Here, a topologically non-trivial interface mode between the two distinct domains of the crystalline topological insulator (CTI) was realised. After establishing selective lasing from this mode, the coherence properties were studied and coherence of a full, hexagonal interface comprised of 30 vertical-cavity surface-emitting lasers (VCSELs) was demonstrated. This result thus represents the first demonstration of a topological insulator VCSEL array, combining the compact size and convenient light collection of vertically emitting lasers with an in-plane topological protection. Finally, in chapter 7, an approach towards engineering the band structures of Lieb and honeycomb lattices by unbalancing the eigenenergies of the sites within each unit cell was presented. For Lieb lattices, this technique opens up a path towards controlling the coupling of a flatband to dispersive bands and could enable a detailed study of the influence of this coupling on the polariton flatband states. In an unbalanced honeycomb lattice, a quantum valley Hall boundary mode between two distinct, unbalanced honeycomb domains with permuted sites in the unit cells was demonstrated. This boundary mode could serve as the foundation for the realisation of a polariton quantum valley Hall effect with a truly topologically protected spin based on vortex charges. Modifying polariton lattices by unbalancing the eigenenergies of the sites that comprise a unit cell was thus identified as an additional, promising path for the future development of polariton lattice simulators.}, subject = {Exziton-Polariton}, language = {en} } @phdthesis{Youssef2022, author = {Youssef, Almoatazbellah}, title = {Fabrication of Micro-Engineered Scaffolds for Biomedical Application}, doi = {10.25972/OPUS-23545}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-235457}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2022}, abstract = {Thermoplastic polymers have a history of decades of safe and effective use in the clinic as implantable medical devices. In recent years additive manufacturing (AM) saw increased clinical interest for the fabrication of customizable and implantable medical devices and training models using the patients' own radiological data. However, approval from the various regulatory bodies remains a significant hurdle. A possible solution is to fabricate the AM scaffolds using materials and techniques with a clinical safety record, e.g. melt processing of polymers. Melt Electrowriting (MEW) is a novel, high resolution AM technique which uses thermoplastic polymers. MEW produces scaffolds with microscale fibers and precise fiber placement, allowing the control of the scaffold microarchitecture. Additionally, MEW can process medical-grade thermoplastic polymers, without the use of solvents paving the way for the production of medical devices for clinical applications. This pathway is investigated in this thesis, where the layout is designed to resemble the journey of a medical device produced via MEW from conception to early in vivo experiments. To do so, first, a brief history of the development of medical implants and the regenerative capability of the human body is given in Chapter 1. In Chapter 2, a review of the use of thermoplastic polymers in medicine, with a focus on poly(ε-caprolactone) (PCL), is illustrated, as this is the polymer used in the rest of the thesis. This review is followed by a comparison of the state of the art, regarding in vivo and clinical experiments, of three polymer melt AM technologies: melt-extrusion, selective laser sintering and MEW. The first two techniques already saw successful translation to the bedside, producing patient-specific, regulatory-approved AM implants. To follow in the footsteps of these two technologies, the MEW device parameters need to be optimized. The MEW process parameters and their interplay are further discussed in Chapter 3 focusing on the importance of a steady mass flow rate of the polymer during printing. MEW reaches a balance between polymer flow, the stabilizing electric field and moving collector to produce reproducible, high-resolution scaffolds. An imbalance creates phenomena like fiber pulsing or arcing which result in defective scaffolds and potential printer damage. Chapter 4 shows the use of X-ray microtomography (µCT) as a non-destructive method to characterize the pore-related features: total porosity and the pore size distribution. MEW scaffolds are three-dimensional (3D) constructs but have long been treated in the literature as two-dimensional (2D) ones and characterized mainly by microscopy, including stereo- and scanning electron microscopy, where pore size was simply reported as the distance between the fibers in a single layer. These methods, together with the trend of producing scaffolds with symmetrical pores in the 0/90° and 0/60/120° laydown patterns, disregarded the lateral connections between pores and the potential of MEW to be used for more complex 3D structures, mimicking the extracellular matrix. Here we characterized scaffolds in the aforementioned symmetrical laydown patterns, along with the more complex 0/45/90/135° and 0/30/60/90/120/150° ones. A 2D pore size estimation was done first using stereomicroscopy, followed by and compared to µCT scanning. The scaffolds with symmetrical laydown patterns resulted in the predominance of one pore size, while those with more complex patterns had a broader distribution, which could be better shown by µCT scans. Moreover, in the symmetrical scaffolds, the size of 3D pores was not able to reach the value of the fiber spacing due to a flattening effect of the scaffold, where the thickness of the scaffold was less than the fiber spacing, further restricting the pore size distribution in such scaffolds. This method could be used for quality assurance of fabricated scaffolds prior to use in in vitro or in vivo experiments and would be important for a clinical translation. Chapter 5 illustrates a proof of principle subcutaneous implantation in vivo experiment. MEW scaffolds were already featured in small animal in vivo experiments, but to date, no analysis of the foreign body reaction (FBR) to such implants was performed. FBR is an immune reaction to implanted foreign materials, including medical devices, aimed at protecting the host from potential adverse effects and can interfere with the function of some medical implants. Medical-grade PCL was used to melt electrowrite scaffolds with 50 and 60 µm fiber spacing for the 0/90° and 0/60/120° laydown patterns, respectively. These implants were implanted subcutaneously in immunocompetent, outbred mice, with appropriate controls, and explanted after 2, 4, 7 and 14 days. A thorough characterization of the scaffolds before implantation was done, followed by a full histopathological analysis of the FBR to the implants after excision. The scaffolds, irrespective of their pore geometry, induced an extensive FBR in the form of accumulation of foreign body giant cells around the fiber walls, in a manner that almost occluded available pore spaces with little to no neovascularization. This reaction was not induced by the material itself, as the same reaction failed to develop in the PCL solid film controls. A discussion of the results was given with special regard to the literature available on flat surgical meshes, as well as other hydrogel-based porous scaffolds with similar pore sizes. Finally, a general summary of the thesis in Chapter 6 recapitulates the most important points with a focus on future directions for MEW.}, language = {en} }