Techn. Hochsch., Diss., 2004--Aachen.

In this PhD thesis, the fingerprints of geometry and topology on low dimensional mesoscopic systems are investigated. In particular, holographic non-equilibrium transport properties of the quantum spin Hall phase, a two dimensional time reversal symmetric bulk insulating phase featuring one dimensional gapless helical edge modes are studied. In these metallic helical edge states, the spin and the direction of motion of the charge carriers are locked to each other and counter-propagating states at the same energy are conjugated by time reversal symmetry. This phenomenology entails a so called topological protection against elastic single particle backscattering by time reversal symmetry. We investigate the limitations of this topological protection by studying the influence of inelastic processes as induced by the interplay of phonons and extrinsic spin orbit interaction and by taking into account multi electron processes due to electron-electron interaction, respectively. Furthermore, we propose possible spintronics applications that rely on a spin charge duality that is uniquely associated with the quantum spin Hall phase. This duality is present in the composite system of two helical edge states with opposite helicity as realized on the two opposite edges of a quantum spin Hall sample with ribbon geometry. More conceptually speaking, the quantum spin Hall phase is the first experimentally realized example of a symmetry protected topological state of matter, a non-interacting insulating band structure which preserves an anti-unitary symmetry and is topologically distinct from a trivial insulator in the same symmetry class with totally localized and hence independent atomic orbitals. In the first part of this thesis, the reader is provided with a fairly self-contained introduction into the theoretical concepts underlying the timely research field of topological states of matter. In this context, the topological invariants characterizing these novel states are viewed as global analogues of the geometric phase associated with a cyclic adiabatic evolution. Whereas the detailed discussion of the topological invariants is necessary to gain deeper insight into the nature of the quantum spin Hall effect and related physical phenomena, the non-Abelian version of the local geometric phase is employed in a proposal for holonomic quantum computing with spin qubits in quantum dots. / In dieser Doktorarbeit wird der Zusammenhang zwischen den mathematischen Bereichen der modernen Differentialgeometrie sowie der Topologie und den physikalischen Eigenschaften niedrigdimensionaler mesoskopischer Systeme erläutert. Insbesondere werden Phänomene des holographischen Quantentransportes in Quanten Spin Hall Systemen fernab des thermodynamischen Gleichgewichtes untersucht. Die Quanten Spin Hall Phase ist ein zweidimensionaler, zeitumkehrsymmetrischer elektrisch isolierender Zustand, dessen charakteristische Eigenschaft eindimensionale metallische Randzustände sind. Diese im Englischen als “helical edge states” bezeichneten Randkanäle zeichnen sic h dadurch aus, dass Spin und Bewegungsrichtung der Ladungsträger fest miteinander verknüpft sind und zwei Zustände mit gleicher Energie aber unterschiedlicher Bewegungsrichtung stets durch die Symmetrieoperation der Zeitumkehr zusammenhängen. Diese Phänomenologie bedingt einen sogenannten topologischen Schutz durch Zeitumkehrsymmetrie gegen elastische Einteilchenrückstreuung. Wir beschäftigen uns mit den Grenzen dieses Schutzes, indem wir inelastische Rückstreuprozesse in Betracht ziehen, wie sie etwa durch das Wechselspiel von extrinsischer Spin-Bahn Kopplung und Gitterschwingungen induziert werden können, oder aber indem wir Mehrteilchen-Streuprozesse untersuchen, welche die Coulomb-Wechselwirkung ermöglicht. Desweiteren werden Anwendungen aus dem Gebiet der Spintronik vorgeschlagen, welche auf einer dem Quanten Spin Hall Effekt eigenen Dualität zwischen dem Spin und dem Ladungsfreiheitsgrad beruhen. Diese Dualität existiert in einem aus zwei Randzuständen mit entgegengesetzter Helizität zusammengesetzten System, wie etwa durch zwei gegenüberliegende Ränder einer streifenförmigen Probe im Quanten Spin Hall Zustand realisiert. Konzeptionell gesehen ist der Quanten Spin Hall Zustand das erste experimentell nachgewiesene Beispiel eines symmetriegeschützten topologischen Zustandes nichtwechselwirkender Materie, also eines Bandisolators, welcher eine antiunitäre Symmetrie besitzt und sich von einem trivialen Isolator mit gleicher Symmetrie aber ausschliesslich lokalisierten und daher voneinander unabhängigen atomaren Orbitalen topologisch unterscheidet. Im ersten Teil dieser Dissertation geben wir eine Einführung in die theoretischen Konzepte, welche dem Forschungsgebiet der nichtwechselwirkenden topologischen Zustände zugrunde liegen. In diesem Zusammenhang werden die topologischen Invarianten, welche diese neuartigen Zustände charakterisieren, als globales Analogon zur lokalen geometrischen Phase dargestellt, welche mit einer zyklischen adiabatischen Entwicklung eines physikalischen Systems verknüpft ist. Während die ausführliche Diskussion der globalen Invarianten einem tieferen Verständnis des Quanten Spin Hall Effektes und damit verwandten physikalischen Phänomenen dienen soll, wird die nicht-Abelsche Variante der lokalen geometrischen Phase für einen Vorschlag zur Realisierung von holonomiebasierter Quanteninformationsverarbeitung genutzt. Das Quantenbit der von uns vorgeschlagenen Architektur ist ein in einem Quantenpunkt eingesperrter Spinfreiheitsgrad.

Stuttgart, Univ., Diss., 2007.

Stuttgart, Univ., Diss., 2001.

Techn. University, Diss., 2004--Berlin.

Magnetism is a phenomenon ubiquitously found in everyday life. Yet, together with superconductivity and superfluidity, it is among the few macroscopically realized quantum states. Although well-understood on a quasi-classical level, its microscopic description is still far from being solved. The interplay of strong interactions present in magnetic condensed-matter systems and the non-trivial commutator structure governing the underlying spin algebra prevents most conventional approaches in solid-state theory to be applied. On the other hand, the quantum limit of magnetic systems is fertile land for the development of exotic phases of matter called spin-liquids. In these states, quantum fluctuations inhibit the formation of magnetic long-range order down to the lowest temperatures. From a theoretical point of view, spin-liquids open up the possibility to study their exotic properties, such as fractionalized excitations and emergent gauge fields. However, despite huge theoretical and experimental efforts, no material realizing spin-liquid properties has been unambiguously identified with a three-dimensional crystal structure. The search for such a realization is hindered by the inherent difficulty even for model calculations. As most numerical techniques are not applicable due to the interaction structure and dimensionality of these systems, a methodological gap has to be filled. In this thesis, to fill this void, we employ the pseudo-fermion functional renormalization group (PFFRG), which provides a scheme to investigate ground state properties of quantum magnetic systems even in three spatial dimensions. We report the status quo of this established method and extend it by alleviating some of its inherent approximations. To this end, we develop a multi-loop formulation of PFFRG, including hitherto neglected terms in the underlying flow equations consistently, rendering the outcome equivalent to a parquet approximation. As a necessary prerequisite, we also significantly improve the numerical accuracy of our implementation of the method by switching to a formulation respecting the asymptotic behavior of the vertex functions as well as employing state-of-the-art numerical algorithms tailored towards PFFRG. The resulting codebase was made publicly accessible in the open-source code PFFRGSolver.jl. We subsequently apply the technique to both model systems and real materials. Augmented by a classical analysis of the respective models, we scan the phase diagram of the three-dimensional body-centered cubic lattice up to third-nearest neighbor coupling and the Pyrochlore lattice up to second-nearest neighbor. In both systems, we uncover in addition to the classically ordered phases, an extended parameter regime, where a quantum paramagnetic phase appears, giving rise to the possibility of a quantum spin liquid. Additionally, we also use the nearest-neighbor antiferromagnet on the Pyrochlore lattice as well as the simple cubic lattice with first- and third-nearest neighbor couplings as a testbed for multi-loop PFFRG, demonstrating, that the inclusion of higher loop orders has quantitative effects in paramagnetic regimes and that the onset of order can be signaled by a lack of loop convergence. Turning towards material realizations, we investigate the diamond lattice compound MnSc\(_2\)S\(_4\), explaining on grounds of ab initio couplings the emergence of a spiral spin liquid at low temperatures, but above the ordering transition. In the Pyrochlore compound Lu\(_2\)Mo\(_2\)O\(_5\)N\(_2\), which is known to not magnetically order down to lowest temperatures, we predict a spin liquid state displaying a characteristic gearwheel pattern in the spin structure factor. / Das Phänomen des Magnetismus ist allgegenwärtig im täglichen Leben und doch ist es, zusammen mit der Supraleitung und -fluidität, eines der wenigen makroskopisch realisierten Quantenphänomene. Auf quasi-klassischer Ebene ist Magnetismus gut verstanden, doch seine mikroskopische Beschreibung ist noch weit davon entfernt, als gelöst bezeichnet zu werden. Das Zusammenspiel von starken Wechselwirkungen, die in magnetischer kondensierte Materie am Werke sind, und der nicht-trivialen Kommutatorstruktur, die die zugrunde liegende Spin-Algebra bestimmt, verhindert, dass konventionelle Herangehensweisen der Festkörpertheorie angewendet werden können. Andererseits ist der quantenmechanische Grenzfall magnetischer Systeme ein fruchtbarer Boden für die Herausbildung exotischer Phasen der Materie, die als Spin-Flüssigkeiten bezeichnet werden. In diesen Zuständen verhindern Quantenfluktuationen die Ausbildung einer langreichweitigen magnetischen Ordnung auch bei niedrigsten Temperaturen. Aus theoretischer Sicht eröffnen Spinflüssigkeiten die Möglichkeit, exotische Eigenschaften, wie fraktionalisierte Anregungen und emergente Eichfelder, zu studieren. Großen theoretischen und experimentellen Anstrengungen zum Trotz wurde jedoch bisher kein Material mit dreidimensionaler Kristallstruktur identifiziert, das unzweifelhaft die Eigenschaften von Spinflüssigkeiten aufweist. Die Suche nach einer solchen Realisierung wird von der Komplexität behindert, die sogar einfachen Modellrechnungen inhärent ist. Da die meisten numerischen Verfahren aufgrund der Wechselwirkungsstruktur und Dimensionalität der Systeme nicht anwendbar sind, bleibt eine methodische Lücke bestehen. In dieser Arbeit benutzen wir die pseudo-fermionische funktionale Renormierungsgruppe (PFFRG), um diese zu füllen. Mit ihr realisieren wir ein Verfahren, um die Grundzustandseigenschaften von quantenmagnetischen Systemen in drei Raumdimensionen zu studieren, Wir fassen den Status quo dieser bereits etablierten Methode zusammen und erweitern sie, indem wir einige ihrer inhärenten Näherungen abmildern. Dafür entwickeln wir eine Mehrschleifen-Formulierung der PFFRG, die bisher vernachlässigte Terme der zugrunde liegenden Flussgleichungen konsistent berücksichtigt und damit die PFFRG äquivalent zur Parquet-Näherung macht. Um dies zu erreichen, verbessern wir außerdem die numerische Genauigkeit der Methode signifikant, indem wir einerseits zu einer Formulierung wechseln, welche die Asymptotiken der Vertex-Funktionen explizit berücksichtigt und andererseits moderne Algorithmen, maßgeschneidert für die PFFRG, nutzt. Der daraus resultierenden Computercode wurde im Open-Source Paket PFFRGSolver.jl öffentlich zugänglich gemacht. Im Anschluss wenden wir die Methode sowohl auf Modellsysteme, als auch echte Materialien an. Vor dem Hintergrund klassischer Analysen scannen wir die Phasendiagramme des dreidimensionalen raumzentrierten kubischen und des Pyrochlorgitters, wobei wir Wechselwirkungen bis zu drittnächsten beziehungsweise übernächsten Nachbarn berücksichtigen. In beiden Systemen finden wir, neben den klassisch geordneten Phasen, einen ausgedehnten Parameterraum, in dem eine quantenparamagnetische Phase im Phasendiagramm erscheint, welche die Möglichkeit einer Quantenspinflüssigkeitsphase eröffnet. Wir nutzen außerdem den Nächstnachbarantiferromagnet auf dem Pyrochlorgitter und das kubische Gitter mit Nächst- und Drittnächstnachbarwechselwirkung als einen Prüfstand für die Vielschleifen-PFFRG, indem wir zeigen, dass die Berücksichtigung höherer Schleifenordnungen quantitative Auswirkungen in den paramagnetischen Regimen hat und außerdem magnetische Ordnung durch ein Fehlen der Schleifenkonvergenz signalisiert werden kann. Abschließend wenden wir uns den echten Materialien zu und untersuchen MnSc\(_2\)S\(_4\), welches eine Diamantgitterstruktur aufweist. Basierend auf ab intio Kopplungsstärken erklären wir das Auftreten einer Spiralspinflüssigkeit bei niedrigen Temperaturen, aber oberhalb des Ordnungsübergangs. Zudem sagen wir im Pyrochlormaterial Lu\(_2\)Mo\(_2\)O\(_5\)N\(_2\), welches in Experimenten auch bei niedrigsten Temperaturen nicht magnetisch ordnet, einen Spinflüssigkeitszustand voraus, der sich durch ein charakteristisches Zahnradmuster im Spinstrukturfaktor auszeichnet.

The last years have witnessed an exciting scientific quest for intriguing topological phenomena in time-dependent quantum systems. A key to many manifestations of topology in dynamical systems relies on the effective dimensional extension by time-periodic drives. An archetypal example is provided by the Thouless pump in one spatial dimension, where a robust and quantized charge transport can be described in terms of an integer quantum Hall effect upon interpreting time as an extra dimension. Generalizing this fundamental concept to multifrequency driving, a variety of higher-dimensional topological models can be engineered in dynamical synthetic dimensions, where the underlying topological classification leads to quantized pumping effects in the associated lower-dimensional time-dependent systems. In this Thesis, we explore how correlations profoundly impact the topological features of dynamical synthetic quantum materials. More precisely, we demonstrate that the interplay of interaction and dynamical synthetic dimension gives rise to striking topological phenomena that go beyond noninteracting implementations. As a starting point, we exploit the Floquet counterpart of an integer quantum Hall scenario, namely a two-level system driven by two incommensurate frequencies. In this model, the topologically quantized response translates into a process in which photons of different frequencies are exchanged between the external modes, referred to as topological frequency conversion. We extend this prototypical setup to an interacting version, focusing on the minimal case of two correlated spins equally exposed to the external drives. We show that the topological invariant determining the frequency conversion can be changed by odd integers, something explicitly forbidden in the noninteracting limit of two identical spins. This correlated topological feature may, in turn, result in an enhancement of the quantized response. Robust response signals, such as those predicted for the topological frequency converter, are of fundamental interest for potential technological applications of topological quantum matter. Based on an open quantum system implementation of the frequency converter, we propose a novel mechanism of topological quantization coined ''topological burning glass effect''. Remarkably, this mechanism amplifies the local response of the driven two-level system by an integer that is proportional to the number of environmental degrees of freedom to which the system is strongly coupled. Specifically, our findings are illustrated by the extension of the frequency converter to a central spin model. There, the local energy transfer mediated exclusively by the central spin is significantly enhanced by the collective motion of the surrounding spins. In this sense, the central spin adopts the topological nature of the total system in its non-unitary dynamics, taking into account the correlations with the environment. / In den letzten Jahren hat sich eine spannende Suche nach faszinierenden topologischen Phänomenen in zeitabhängigen Quantensystemen entwickelt. Ein Schlüssel zu zahlreichen Ausprägungen der Topologie in dynamischen Systemen beruht auf der effektiven Dimensionserweiterung durch zeitlich-periodische Antriebe. Ein Beispiel ist die Thouless-Pumpe in einer räumlichen Dimension, in der ein robuster und quantisierter Ladungstransport mittels eines Quanten-Hall-Effekts beschrieben werden kann, sofern Zeit als zusätzliche Dimension interpretiert wird. Durch Verallgemeinerung dieses Grundkonzepts auf Multifrequenzantriebe kann eine Vielzahl höherdimensionaler topologischer Modelle in zeitlich synthetischen Dimensionen konstruiert werden, bei denen die zugrunde liegende topologische Klassifikation zu quantisierten Pumpeffekten in den zugehörigen niederdimensionalen zeitabhängigen Systemen führt. In dieser Dissertation wird untersucht, wie Korrelationen die topologischen Eigenschaften von zeitlich synthetischen Quantenmaterialen maßgeblich beeinflussen. Konkret wird gezeigt, dass das Zusammenspiel von Wechselwirkung und zeitlicher synthetischer Dimension zu erstaunlichen topologischen Phänomenen führt, die über nicht-wechselwirkende Realisierungen hinausgehen. Als Ausgangspunkt wird das Floquet-Gegenstück eines Quanten-Hall-Szenarios genutzt, ein Zwei-Niveau-System, das von zwei inkommensurablen Frequenzen getrieben wird. In diesem Modell spiegelt sich die topologisch quantisierte Antwort in einen Prozess wider, bei dem Photonen verschiedener Frequenzen zwischen den externen Moden ausgetauscht werden, auch bekannt als topologische Frequenzumwandlung. Wir erweitern dieses prototypische Setup auf eine interagierende Version, indem wir uns auf den Minimalfall zweier korrelierter Spins konzentrieren, die gleichermaßen den externen Antrieben ausgesetzt sind. Wir zeigen, dass die topologische Invariante, die die Frequenzumwandlung bestimmt, durch ungerade ganze Zahlen verändert werden kann. Ein Zustand, der im nicht-wechselwirkenden Fall ausdrücklich verboten ist. Dieses korrelierte topologische Verhalten kann wiederum zu einer Verstärkung der quantisierten Antwort führen. Robuste Antwortsignale, wie sie für den topologischen Frequenzumwandler vorhergesagt werden, sind von grundlegendem Interesse für potentielle technologische Anwendungen der topologischen Quantenmaterie. Basierend auf einer offenen Quantensystem-Realisierung des Frequenzumwandlers schlagen wir einen neuartigen Mechanismus der topologischen Quantisierung vor, den wir als ''topologischen Brennglaseffekt'' bezeichnen. Dieser Mechanismus verstärkt die lokale Antwort des getriebenen Zwei-Niveau-Systems um eine ganze Zahl, die proportional zur Anzahl der Freiheitsgrade der Umgebung ist, an die das System koppelt. Konkret werden unsere Erkenntnisse durch die Erweiterung des Frequenzumwandlers auf ein Zentralspinmodell veranschaulicht. Der lokale Energietransfer, der ausschließlich durch den zentralen Spin vermittelt wird, wird durch die kollektive Bewegung der umgebenden Spins maßgeblich verstärkt. In diesem Sinne erbt der Zentralspin die topologische Natur des Gesamtsystems in seiner nicht-unitären Dynamik, die die Korrelationen mit der Umgebung berücksichtigt.

Solid state physics comprises many interesting physical phenomena driven by the complex interplay of the crystal structure, magnetic and orbital degrees of freedom, quantum fluctuations and correlation. The discovery of materials which exhibit exotic phenomena like low dimensional magnetism, superconductivity, thermoelectricity or multiferroic behavior leads to various applications which even directly influence our daily live. For such technical applications and the purposive modification of materials, the understanding of the underlying mechanisms in solids is a precondition. Nowadays DFT based band structure programs become broadly available with the possibility to calculate systems with several hundreds of atoms in reasonable time scales and high accuracy using standard computers due to the rapid technical and conceptional development in the last decades. These improvements allow to study physical properties of solids from their crystal structure and support the search for underlying mechanisms of different phenomena from microscopic grounds. This thesis focuses on the theoretical description of low dimensional magnets and intermetallic compounds. We combine DFT based electronic structure and model calculations to develop the magnetic properties of the compounds from microscopic grounds. The developed, intuitive pictures were challenged by model simulations with various experiments, probing microscopic and macroscopic properties, such as thermodynamic measurements, high field magnetization, nuclear magnetic resonance or electron spin resonance experiments. This combined approach allows to investigate the close interplay of the crystal structure and the magnetic properties of complex materials in close collaboration with experimentalists. In turn, the systematic variation of intrinsic parameters by substitution or of extrinsic factors, like magnetic field, temperature or pressure is an efficient way to probe the derived models. Especially pressure allows a continuous change of the crystal structure on a rather large energy scale without the chemical complexity of substitution, thus being an ideal tool to consistently alter the electronic structure in a controlled way. Our theoretical results not only provide reliable descriptions of real materials, exhibiting disorder, partial site occupation and/or strong correlations, but also predict fascinating phenomena upon extreme conditions. In parts this theoretical predictions were already confirmed by own experiments on large scale facilities. Whereas in the first part of this work the main purpose was to develop reliable magnetic models of low dimensional magnets, in the second part we unraveled the underlying mechanism for different phase transitions upon pressure. In more detail, the first part of this thesis is focused on the magnetic ground states of spin 1/2 transition metal compounds which show fascinating phase diagrams with many unusual ground states, including various types of magnetic order, like helical states exhibiting different pitch angles, driven by the intimate interplay of structural details and quantum fluctuations. The exact arrangement and the connection of the magnetically active building blocks within these materials determine the hybridization, orbital occupation, and orbital orientation, this way altering the exchange paths and strengths of magnetic interaction within the system and consequently being crucial for the formation of the respective ground states. The spin 1/2 transition metal compounds, which have been investigated in this work, illustrate the great variety of exciting phenomena fueling the huge interest in this class of materials. We focused on cuprates with magnetically active CuO4 plaquettes, mainly arranged into edge sharing geometries. The influence of structural peculiarities, as distortion, folding, changed bonding angles, substitution or exchanged ligands has been studied with respect to their relevance for the magnetic ground state. Besides the detailed description of the magnetic ground states of selected compounds, we attempted to unravel the origin for the formation of a particular magnetic ground state by deriving general trends and relations for this class of compounds. The details of the treatment of the correlation and influence of structural peculiarities like distortion or the bond angles are evaluated carefully. In the second part of this work we presented the results of joint theoretical and experimental studies for intermetallic compounds, all exhibiting an isostructural phase transition upon pressure. Many different driving forces for such phase transitions are known like quantum fluctuations, valence instabilities or magnetic ordering. The combination of extensive computational studies and high pressure XRD, XAS and XMCD experiments using synchrotron radiation reveals completely different underlying mechanism for the onset of the phase transitions in YCo5, SrFe2As2 and EuPd3Bx. This thesis demonstrates on a series of complex compounds that the combination of ab-initio electronic structure calculations with numerical simulations and with various experimental techniques is an extremely powerful tool for a successful description of the intriguing quantum phenomena in solids. This approach is able to reduce the complex behavior of real materials to simple but appropriate models, this way providing a deep understanding for the underlying mechanisms and an intuitive picture for many phenomena. In addition, the close interaction of theory and experiment stimulates the improvement and refinement of the methods in both areas, pioneering the grounds for more and more precise descriptions. Further pushing the limits of these mighty techniques will not only be a precondition for the success of fundamental research at the frontier between physics and chemistry, but also enables an advanced material design on computational grounds.

Solid state physics comprises many interesting physical phenomena driven by the complex interplay of the crystal structure, magnetic and orbital degrees of freedom, quantum fluctuations and correlation. The discovery of materials which exhibit exotic phenomena like low dimensional magnetism, superconductivity, thermoelectricity or multiferroic behavior leads to various applications which even directly influence our daily live. For such technical applications and the purposive modification of materials, the understanding of the underlying mechanisms in solids is a precondition. Nowadays DFT based band structure programs become broadly available with the possibility to calculate systems with several hundreds of atoms in reasonable time scales and high accuracy using standard computers due to the rapid technical and conceptional development in the last decades. These improvements allow to study physical properties of solids from their crystal structure and support the search for underlying mechanisms of different phenomena from microscopic grounds. This thesis focuses on the theoretical description of low dimensional magnets and intermetallic compounds. We combine DFT based electronic structure and model calculations to develop the magnetic properties of the compounds from microscopic grounds. The developed, intuitive pictures were challenged by model simulations with various experiments, probing microscopic and macroscopic properties, such as thermodynamic measurements, high field magnetization, nuclear magnetic resonance or electron spin resonance experiments. This combined approach allows to investigate the close interplay of the crystal structure and the magnetic properties of complex materials in close collaboration with experimentalists. In turn, the systematic variation of intrinsic parameters by substitution or of extrinsic factors, like magnetic field, temperature or pressure is an efficient way to probe the derived models. Especially pressure allows a continuous change of the crystal structure on a rather large energy scale without the chemical complexity of substitution, thus being an ideal tool to consistently alter the electronic structure in a controlled way. Our theoretical results not only provide reliable descriptions of real materials, exhibiting disorder, partial site occupation and/or strong correlations, but also predict fascinating phenomena upon extreme conditions. In parts this theoretical predictions were already confirmed by own experiments on large scale facilities. Whereas in the first part of this work the main purpose was to develop reliable magnetic models of low dimensional magnets, in the second part we unraveled the underlying mechanism for different phase transitions upon pressure. In more detail, the first part of this thesis is focused on the magnetic ground states of spin 1/2 transition metal compounds which show fascinating phase diagrams with many unusual ground states, including various types of magnetic order, like helical states exhibiting different pitch angles, driven by the intimate interplay of structural details and quantum fluctuations. The exact arrangement and the connection of the magnetically active building blocks within these materials determine the hybridization, orbital occupation, and orbital orientation, this way altering the exchange paths and strengths of magnetic interaction within the system and consequently being crucial for the formation of the respective ground states. The spin 1/2 transition metal compounds, which have been investigated in this work, illustrate the great variety of exciting phenomena fueling the huge interest in this class of materials. We focused on cuprates with magnetically active CuO4 plaquettes, mainly arranged into edge sharing geometries. The influence of structural peculiarities, as distortion, folding, changed bonding angles, substitution or exchanged ligands has been studied with respect to their relevance for the magnetic ground state. Besides the detailed description of the magnetic ground states of selected compounds, we attempted to unravel the origin for the formation of a particular magnetic ground state by deriving general trends and relations for this class of compounds. The details of the treatment of the correlation and influence of structural peculiarities like distortion or the bond angles are evaluated carefully. In the second part of this work we presented the results of joint theoretical and experimental studies for intermetallic compounds, all exhibiting an isostructural phase transition upon pressure. Many different driving forces for such phase transitions are known like quantum fluctuations, valence instabilities or magnetic ordering. The combination of extensive computational studies and high pressure XRD, XAS and XMCD experiments using synchrotron radiation reveals completely different underlying mechanism for the onset of the phase transitions in YCo5, SrFe2As2 and EuPd3Bx. This thesis demonstrates on a series of complex compounds that the combination of ab-initio electronic structure calculations with numerical simulations and with various experimental techniques is an extremely powerful tool for a successful description of the intriguing quantum phenomena in solids. This approach is able to reduce the complex behavior of real materials to simple but appropriate models, this way providing a deep understanding for the underlying mechanisms and an intuitive picture for many phenomena. In addition, the close interaction of theory and experiment stimulates the improvement and refinement of the methods in both areas, pioneering the grounds for more and more precise descriptions. Further pushing the limits of these mighty techniques will not only be a precondition for the success of fundamental research at the frontier between physics and chemistry, but also enables an advanced material design on computational grounds.:Contents List of abbreviations 1. Introduction 2. Methods 2.1. Electronic structure and magnetic models for real compounds 2.1.1. Describing a solid 2.1.2. Basic exchange and correlation functionals 2.1.3. Strong correlations 2.1.4. Band structure codes 2.1.5. Disorder and vacancies 2.1.6. Models on top of DFT 2.2. X-ray diffraction and x-ray absorption at extreme conditions 2.2.1. Diamond anvil cells 2.2.2. ID09 - XRD under pressure 2.2.3. ID24 - XAS and XMCD under pressure 3. Low dimensional magnets 3.1. Materials 3.1.1 AgCuVO4 - a model compound between two archetypes of Cu-O chains 3.1.2 Li2ZrCuO4 - in close vicinity to a quantum critical point 3.1.3 PbCuSO4(OH)2 -magnetic exchange ruled by H 3.1.4 CuCl2 and CuBr2 - flipping magnetic orbitals by crystal water 3.1.5 Na3Cu2SbO6 and Na2Cu2TeO6 - alternating chain systems 3.1.6 Cu2(PO3)2CH2 - magnetic vs. structural dimers 3.1.7 Cu2PO4OH - orbital order between dimers and chains 3.1.8 A2CuEO6 - an new family of spin 1/2 square lattice compounds 3.2. General trends and relations 3.2.1. Approximation for the treatment of strong correlation 3.2.2. Structural elements 4. Magnetic intermetallic compounds under extreme conditions 115 4.1. Itinerant magnets 4.1.1. YCo5 - a direct proof for a magneto elastic transition by XMCD 4.1.2. SrFe2As2 - symmetry-preserving lattice collapse 4.2. Localized magnets 4.2.1. EuPd3Bx - valence transition under doping and pressure 5. Summary and outlook A. Technical details B. Crystal Structures C. Supporting Material Bibliography List of Publications Acknowledgments