This thesis presents the theoretical studies of chiral magnetic structures, which exist or are affected by antisymmetric Dzyaloshinskii-Moriya interactions. The theoretical approach is based on the phenomenological model of ferromagnetic materials lacking inversion symmetry. Equilibrium magnetic states are described as static structures in the micromagnetic low temperature limit with a fixed magnitude of the magnetization. The studies are focused on two cases: (i) magnetization structures that are affected by chiral exchange so that a particular chirality of these structures is selected, and (ii) novel solitonic states that are called chiral Skyrmions and only exist because of the chiral exchange. Vortex states in magnetic nanodisks provide the simplest example of a handed magnetization structure, where effects of the chiral couplings may become noticeable. A chiral exchange here favours one chirality of such a vortex state over the other. This effect can stem from surface-induced or other defect-related chiral Dzyaloshinskii-Moriya exchange. The different chiral versions of the vortex states are shown to display strong dependencies on the materials properties of such nanodisks. Within a micromagnetic model for these effects, numerical calculations of the shape, size, and stability of the vortices in equilibrium as functions of magnetic field and the material and geometrical parameters provide a general analysis of the influence of the broken mirror symmetry caused by the surface/interfaces or structural defect on their properties. The Dzyaloshinskii-Moriya interactions impose differences in the energies and sizes of vortices with different chirality: these couplings can considerably increase sizes of vortices with one sense of rotation and suppress vortices with opposite sense of rotation. Torsions related to lattice defects can cause similar to the surface-induced chiral couplings. A general phenomenological magneto-elastic formulation for this torsional chirality selection is given. It is applied to calculate similar effects on vortex states in magnetic disks with a screw dislocation at their center. In systems with strong chiral exchange the magnetic equilibrium states themselves become chiral twisted structures. The most interesting structures in this context are the two-dimensional solitonic states that are now known as chiral Skyrmions. The properties and stability of multiply twisted states composed of these particle-like units are the subject of the second part of this thesis. These states compete with the well known onedimensionally modulated helical states in non-centrosymmetric magnetic systems. Studies of modulated states in cubic helimagnets have shown, that in absence of additional effects, the only thermodynamically stable state is a cone helix. Uniaxial distortions, that can be caused by uniaxial stresses in the bulk samples or arise due to surface effects in thin films, suppress the helical states and stabilize Skyrmion lattices in a broad range of thermodynamical parameters. Using the phenomenological theory for modulated and localized states in chiral magnets, the equilibrium parameters of the Skyrmion and helical states have been derived as functions of applied magnetic field and induced uniaxial anisotropy. These results show that due to a combined effect of induced uniaxial anisotropy and an applied magnetic field, Skyrmion lattices can be formed as thermodynamically stable states. The theoretical results provide a comprehensive description of the evolution of modulated states in an applied magnetic field depending on type of anisotropy. The cases of a uniaxial anisotropy of easy axis and easy plane type with fields applied along its axis are investigated in detail. Existence of Skyrmion-lattice states in the easy axis case as thermodynamic field-induced phase is demonstrated. The results explain recent observation of Skyrmion lattices by magnetic Lorentz microscopy in thin foils of cubic chiral magnets. In systems with easy plane type of anisotropy, Skyrmion states do not form thermodynamic phases in applied fields along the axis. However, distorted Skyrmion phases can exist in fields applied perpendicularly to the axis. In this configuration of anisotropy axis and fields, both the helical states and the Skyrmions display elliptical distortions. The investigated micromagnetic model maps out the basic helical and Skyrmionic states expected to exist in cubic and nearly cubic chiral magnets.

Die magnetischen Eigenschaften von Li2CuO2 sind seit mehr als zwei Jahrzehnten Gegenstand theoretischen und experimentellen Interesses. Über die genaue Natur der magnetischen Wechselwirkungen in diesem Isolator konnte jedoch keine Einigkeit erzielt werden. Während das Material von Seiten theoretischer Untersuchungen als quasi-eindimensionaler Magnet mit starken ferromagnetischen Kopplungen entlang der Kette verstanden wurde, legten experimentelle Studien dominierende dreidimensionale Zwischenkettenkopplungen nahe. Im Rahmen dieser Dissertation werden auf der Grundlage von Untersuchungen des magnetischen Anregungsspektrums mittels inelastischer Neutronenstreuung und dessen Analyse innerhalb eines Spinwellenmodels die führenden magnetischen Wechselwirkungen in Li2CuO2 bestimmt. Es wird zweifelsfrei nachgewiesen, dass das Material eine quasi-eindimensionale Spinkettenverbindung darstellt. Insbesondere kann die Konkurrenz von ferro- und antiferromagnetischen Wechselwirkungen entlang der Ketten nachgewiesen werden. Die Anwendbarkeit einer Spinwellenanalyse dieses niedrigdimensionalen Spin-1=2 Systems wird gezeigt. Das magnetische Phasendiagramm wird mittels Messungen von spezifischer Wärme, thermischer Ausdehnung und Magnetostriktion sowie der Magnetisierung in statischen und gepulsten Magnetfeldern untersucht und im Bezug auf die Austauschwechselwirkungen diskutiert. Aufgrund seiner einfachen kristallographischen und magnetischen Struktur stellt Li2CuO2 ein potentiell wertvolles Modellsystem in der Klasse der Spinkettenverbindungen mit konkurrierenden ferro- und antiferromagnetischen Wechselwirkungen dar. / The magnetic properties of Li2CuO2 have attracted interest since more than two decades, both in theory and experiment. Despite these efforts, the precise nature of the magnetic interactions in this insulator remained an issue of controversial debate. From theoretical studies, the compound was understood as a quasi-one-dimensional magnet with strong ferromagnetic interactions along the chain, while in contrast, experimentally studies suggested dominant three-dimensional inter-chain interactions. In this thesis, the leading magnetic exchange interactions of Li2CuO2 are determined on the basis of a detailed inelastic neutron scattering study of the magnetic excitation spectrum, analyzed within spin-wave theory. It is unequivocally shown, that the material represents a quasi-one-dimensional spin-chain compound. In particular, the competition of ferro- and antiferromagnetic interactions in the chain has been evidenced. The applicability of a spin-wave model for analysis of this low-dimensional spin-1=2 system is shown. The magnetic phase diagram of Li2CuO2 is studied by specific heat, thermal expansion and magnetostriction measurements as well as magnetization measurements in both static and pulsed magnetic fifields. The phase diagram is discussed with respect to the exchange interactions. With its simple crystallographic and magnetic structure, Li2CuO2 may serve as a worthwhile model system in the class of spin-chain compounds with competing ferromagnetic and antiferromagnetic interactions.

The present work addresses in-depth magnetic films with magnonic surface patterning of variable size. Two different kinds of such structures referred to as surface-modulated magnonic crystals were investigated: Ion-irradiated magnonic crystals and structurally etched magnonic crystals. To achieve that, two different experimental approaches were pursued. On the one hand, the magnetic moment at the surface of lithographically patterned permalloy (Ni80Fe20) films was periodically reduced by means of ion irradiation. On the other hand, structural trenches were introduced at the surface of a pre-patterned thin film by sequential ion milling. The goal is the acquisition of a fundamental understanding of the behavior of spin-wave modes in the transition from a continuous magnetic thin film to a full magnonic crystal, i.e. separated periodic magnetic structures. In the framework of this thesis, the spin-wave eigen-modes of such magnonic crystals were mainly investigated spectroscopically by means of ferromagnetic resonance. Thereby, the “Two-magnon scattering perturbation theory” and the “plane-wave method” were employed as the theoretical methodologies to understand the complex dynamics of such systems. The first is a reliable method to calculate the dynamic response of surface-modulated magnonic crystals where the modulation is of a perturbation character, i.e. small compared to the film thickness. The latter is a quasi-analytical approach to calculate the dynamic eigen-modes of magnonic crystals consisting of different components with significantly varying properties. Moreover, numerical methods were employed to get further insight into the spin dynamics of these structures. In such systems, the spin-wave behavior follows the well-known dispersion relation of flat magnetic thin films as long as the surface-modulation is small compared to the film thickness. In this work, it was shown that this circumstance can be exploited for a parameter-free determination of the exchange constant A, which is not experimentally accessible for magnetic thin films in a straightforward manner. However, once the modulation height is of significant magnitude, the dynamics of surface-modulated magnonic crystals become substantially more complex. A straightforward understanding of such kind of system is hampered by the complex interplay of different effects. On the one hand, the internal demagnetizing field reveals an alternating character and depends itself on the modulation height and the field angle. On the other hand, the dynamic eigen-modes are hybridized, i.e., they reveal different characteristics in different regions of the magnonic crystal and, in addition, they couple to each other. Here, the approach is particularly favorable to investigate the spin dynamics of surface-modulated magnonic crystals by systematically altering the modulation height of the same sample. This is mainly due to two reasons. First, the two edge cases, namely the thin film and the full magnonic crystal, are already well understood and, second, other magnetic and structural parameters remain constant. With the help of the measurement results and the simulations, the quasi-analytical theory was validated. Subsequently, the mode profiles were calculated by theory and simulation in order to analyze the mode character in the transition from a thin film to a full magnonic crystal. Two kinds of dynamic eigen-modes were identified, namely hybridized modes and localized modes. For both types, simple formulae were derived describing their characteristic dynamic behavior. Besides, transition rules were found connecting the mode number n of film modes with the mode number m of modes in the full magnonic crystal. In order to correlate the symmetry and magnitude of the demagnetizing field with the spin-wave eigen-modes, the internal fields of a strongly surface-modulated magnonic crystal were reconstructed by electron holography measurements. By reemploying the measurement results for micromagnetic simulations, the dynamics of the whole system could be reproduced. This strategy allowed for a better understanding of the link between the demagnetizing field and the spin-wave mode characteristics. Based on these results, a simplified model for the analytical description of the inplane angular dependence was found. The acquired understanding of such systems led to the elaboration of specific applications, such as the spin-wave channelization. It should be noted that the coupling of uniform to non-uniform spin-wave phenomena, which is an intrinsic property of these structures, holds out the prospect of several applications in the future.

A very important step in the art of cooking up models for the study of natural phenomena is the identification of the relevant ingredients. Taking into account too many details will lead to an overly complicated model, not at all useful to work with, but neglecting some crucial elements will lead to an equally useless model. So it is often the case that the actual experimental situation presents unavoidable sources of local randomness, whilst the analysed phenomenon does not really rely on presence/absence of such imperfections. For some other set of phenomena, however, disorder can play a crucial role, and must be carefully taken into account. Such is for example the case in certain phases of matter, the spin-glass phase, or the many-body localised phase. In this thesis we explore disorder in both of these situations and also as a theoretical means of testing the regime of liquidity in certain two-dimensional highly frustrated magnetic models. The focus here is placed on classical Heisenberg models defined on lattices consisting of clusters all sites of which interact mutually pairwise. This natural way to introduce frustration has been known in the literature to lead to so-called Coulomb spin-liquids, the single class of classical spin-liquids acknowledged to exist so far in Heisenberg models. Here we show that in fact two different classes of classical spin-liquids can be obtained from similarly defined frustrated models. In one of these, algebraic correlations exist at $T=0$, similar to the Coulomb phase, but the system exhibits a rather different low$-T$ effective action from the Coulomb phase. In the other class, the spin-liquid has spin correlations that decay exponentially with distance, with a correlation length smaller than a lattice spacing even at $T=0$. One special effect of disorder in these models, considered in the form of dilution by non-magnetic impurities, is to nucleate local degrees of freedom, so-called orphans, which express the concomitant spin-liquid phase through their non-trivial fractionalisation. When the associated spin-liquid exhibit algebraic correlations, it is also possible to find new effective spin-glass models as an effective $T=0$ description for interactions between the orphans, leading to so-called `random Coulomb magnets'. One part of this thesis is devoted to the first study of these new models. This investigation consists mainly of Monte Carlo simulations and numerical solution of the relevant large$-n$ equations ($n$ being the number of spin components). A clear spin-glass transition for infinitely large coupling strength is determined for the case of spins with an infinite number of components. The results presented on the situation for a finite number of spin components are more of an exploratory character, and large-scale simulations with further optimization schemes to ensure equilibration are still required to locate the transition. The final investigation treated in this thesis deals with the dynamics in a quantum model with disorder displaying the many-body localized phase, where in addition a periodic drive is applied. For a certain range of driving frequencies and amplitudes, it was found recently that the many-body localized phase is robust. These pioneering studies restricted themselves to an analysis of the stability of such a phase in the long time limit, while very little was known about the dynamics towards the asymptotic fate. Our study focuses on this aspect, and analyses the different dynamical behaviors as one varies the driving parameters, so that the many-body localized phase survives or is destroyed by the driving. We discover that on the border between these two asymptotic fates, a new dynamical behavior emerges, where the system heats up at a very slow, logarithmic in time, rate. / Die Bestimmung der wichtigsten Bestandteile stellt einen sehr wichtigen Schritt in der Kunst des Erstellens von Modellen dar. Die Annahme von zu vielen Details ergibt ein sehr kompliziertes, zu nichts zu gebrauchendes Modell, doch die Vernachlässigung von bedeutenden Zusammenhängen führt ebenfalls zu einem unbrauchbaren Ergebnis. Es ist so z.B. häufig der Fall, dass ein Experiment unter dem Einfluss von unvermeindlichen lokalen Zufälligkeiten steht, die allerdings kaum einen Einfluss auf ein beobachtetes Phänomen haben. Für gewisse Phänomene spielt Unordnung jedoch eine wesentliche Rolle und sie muss sehr genau in Betracht gezogen werden. Das ist für bestimmte Phasen, wie beispielsweise Spinglas oder die Vielteilchen-Lokalisation, der Fall. In dieser Dissertation untersuchen wir ungeordnete Systeme, die solche Phasen aufweisen. Außerdem verwenden wir Unordnung als ein theoretisches Werkzeug für die Analyse von bestimmten `Spinflüssigkeiten' in zweidimensionalen Spinmodellen. Der Fokus liegt hierbei auf klassischen Heisenberg Modellen definiert auf Gittern, die aus einer Anordnung von Clustern bestehen, sodass jede einzelne paarweise Heisenberg-Wechselwirkung innerhalb eines Clusters stattfindet. Dadurch weist das System geometrische Frustration auf und in mehreren Fällen tritt eine sogennante Coulomb Spinflüssigkeit ---die bislang einzig bekannte Klasse von klassischen Spinflüssigkeit in Heisenberg Modellen--- auf. Wir zeigen, dass mindestens zwei weitere Arten von klassischen Spinflüssigkeiten in solchen Modellen zu finden sind. Für die eine Klasse sind Spinkorrelationen zu erwarten, die algebraisch mit der Entfernung bei $T=0$ abnehmen, ähnlich wie für eine Coulomb Phase. Diese neu entdeckte Spinflüssigkeit lässt sich jedoch von der Coulomb Phase durch eine neue effektive Tieftemperatur-Theorie unterscheiden. Für die andere Klasse von Spinflüssigkeiten sind die Spinkorrelationen kurzreichweitig, und selbst bei $T=0$ nehmen sie exponentiell ab, mit einer Korrelationslänge, die kleiner als ein Gitterabstand ist. Unordnung, in der Form von nicht-magnetischen Störstellen, kann lokale Freiheitsgrade entstehen lassen (diese werden in der Literatur auch als `Orphans', Waisen, bezeichnet). Die Orphans verweisen durch ihre `Fraktionierung' eindeutig auf die nicht trivialen Korrelationen der spinflüssigen Phase. Falls die Spinflüssigkeit algebraische Korrelationen aufweist, findet man auch langreichweitige Wechselwirkungen zwischen den Orphans bei $T=0$. Dies führt zu neuen Spinglasmodellen, sogenannten `Random Coulomb Magnets'. Ein Teil dieser Dissertation ist der Untersuchung solcher Modelle gewidmet. Diese Untersuchung besteht hauptsächlich aus Monte Carlo Simulationen und numerischer Lösung der relevanten Large-$n$ Gleichungen (wobei $n$ hier auf die Anzahl an Spinkomponenten hinweist). In dem Fall von Spins mit unendlich vielen Spinkomponenten können wir einen eindeutigen Spinglas Phasenübergang für eine unendlich große Kopplungsstärke bestimmen. Die entsprechenden Ergebnisse für den Fall von Spins mit einer endlichen Anzahl an Spinkomponenten sind von einem exploratorischen Charakter. Zusätzliche Simulationen, die möglicherweise weitere Optimierungsschema verwenden um Äquilibrium zu gewährleisten, sind noch von nöten um eine eindeutige Aussage über den Übergang in solchen Fällen zu treffen. Der letzte Teil dieser Dissertation widmet sich der Untersuchung der Dynamik eines ungeordneten Quantenmodells. Das ausgewählte Modell weist die sogennante Vielteilchen-lokalisierte Phase auf, und wir untersuchen insbesondere den Effekt eines periodischen Antriebs auf die Dynamik des Systems. Für eine bestimmte Auswahl der Antriebs-frequenz und -amplitude, wurde es bereits vor kurzem bewiesen, dass die Vielteilchen-lokalisierte Phase diese Störung übersteht. Unsere Studie ist darauf ausgelegt, wie sich die Dynamik des Systems durch Variation der Antriebsparameter ändert, so dass die Vielteilchen-lokalisierte Phase für lange Zeit entweder den Antrieb übersteht oder von ihm zerstört wird. Wir konnten dadurch entdecken, dass an der Grenze zwischen diesen beiden Fällen ein neues dynamisches Verhalten entsteht, bei der das System eine sehr langsame, logarithmisch mit der Zeit, Erwärmung aufweist.

Since the last few decades frustrated spin systems have attracted much interest. These studies are motivated by the rich variety of their unusual magnetic properties and potential applications. In this thesis, excitation spectra of the weakly coupled dimer system Ba3Cr2O8, the spin-1/2 chain material with distorted diamond structure Cu3(CO3)2(OH)2 (natural mineral azurite), and the quasi-twodimensional antiferromagnet with triangle spin structure Cs2CuBr4 have been studied by means of high-field electron spin resonance. Two pairs of gapped modes corresponding to transitions from a spin-singlet ground state to the first excited triplet state with zero-field energy gaps, of 19.1 and 27 K were observed in Ba3Cr2O8. The observation of ground-state excitations clearly indicates the presence of a non-secular term allowing these transitions. Our findings are of crucial importance for the interpretation of the field-induced transitions in this material (with critical fields Hc1 = 12.5 T and Hc2 = 23.6 T) in terms of the magnon Bose-Einstein condensation. The natural mineral azurite, Cu3(CO3)2(OH)2, has been studied in magnetic fields up to 50 T, revealing several modes not observed previously. Based on the obtained data, all three critical fields were identified. A substantial zero-field energy gap, Δ = 9.6 K, has been observed in Cs2CuBr4 above the ordering temperature. It is argued that contrary to the case for the isostructural Cs2CuCl4, the size of the gap can not be explained solely by the uniform Dzyaloshinskii-Moriya interaction, but it is rather the result of the geometrical frustration stabilizing the spin-disordered state in Cs2CuBr4 in the close vicinity of the quantum phase transition between a spiral magnetically ordered state and a 2D quantum spin liquid.

Die komplizierte Struktur der Energielandschaft wurde am Beispiel des +/- J Spinglas-Modells untersucht. Sie ist in glasartigen Systemen der Schlüssel zum Verständnis einer verlangsamten Dynamik. Es wurde ein enger Zusammenhang zwischen der Dynamik und der Energielandschaft nachgewiesen. Die Energielandschaft wird in +/- J Spinglas Modellsystemen durch Cluster charakterisiert, die infolge ihrer Konnektivität größere Objekte (z.B. Täler) bilden. Einzelne Cluster, aber auch ganze Täler, sind miteinander durch sogenannten Sattelcluster verknüpft. Die physikalischen Eigenschaften werden durch die Strukturen der Verknüpfungen und durch die innere Struktur der Cluster geprägt. Zur Beschreibung der Energielandschaften wurde die genaue Kenntnis der Zustände benutzt. Auf der Grundlage des "branch-and-bound" Verfahrens war es möglich, für kleine Systeme alle Zustände bis zu der dritten Anregung zu bestimmen. Danach wurden die Konfigurationen so sortiert, dass die Beziehungen zwischen ihnen, wie z.B. Nachbarschaften und Clusterzugehörigkeiten, einfach zu finden waren. Es gelang, die exakte Landschaft für Systeme bis L=6 aufzubauen. Für größere Systeme ist es zur Zeit unmöglich, alle niederenergetischen Zustände zu finden. Eine alternative Möglichkeit, die Struktur zu beschreiben, erhält man durch Untersuchung der Verteilung der Overlap. An der Gestalt der Verteilung erkennt man, ob die niederenergetische Struktur kompliziert oder einfach ist. Bei genaueren Untersuchungen ist es sogar möglich, die Anzahl der existierenden Täler abzuschätzen. Die Untersuchungen der Overlap bei 8555 3D Systemen (L=4) weisen darauf hin, dass bei kleineren Grundzustandsenergien die Struktur durch zwei spiegelsymmetrische Täler geprägt ist. Mit wachsender Grundzustandsenergie wird die Struktur der Systeme immer komplizierter. Eine weitere wichtige Komponente der Energielandschaft ist die innere Struktur der Sattelcluster. Ein Sattelcluster besteht aus wenigstens drei Gruppen von Konfigurationen. Zwei Gruppen enthalten Konfigurationen, die mit den Grundzustandsclustern verbunden sind, und die dritte Gruppe verbindet die beiden. Es passiert oft, dass die Konfigurationsgruppen, die verschiedene Grundzustandscluster verbinden, weit voneinander entfernt liegen. Dies wurde als ein wichtiger Aspekt erkannt, der zu einer Verlangsamung dynamischer Prozesse führt. Der andere Aspekt der Energielandschaft ist ihr Zusammenhang mit dem Realraumbild. Das Realraumbild ist als die Lage der Spins auf dem Gitter zu verstehen. Spins kann man zu verschiedenen Spindomänen zusammenfassen, die dann auf natürliche Weise die Struktur der Energielandschaft generieren. Für die Größe der einzelnen Cluster sind die freien Spins verantwortlich. Es wurde bestätigt, dass die Existenz einzelner Täler durch Spindomänen erklärt werden kann. Dabei wird durch das kollektive Umdrehen aller Spins in einer solcher Domäne ein anderer Cluster in einem anderen Tal erzeugt. Neben dem Zusammenhang von Spindomänen und Energielandschaft konnte der Einfluss von bestimmten zusammenhängenden Strukturen freier Spins genauer aufgeklärt werden. Hier ergeben sich Ansatzpunkte für weitergehende Untersuchungen.

Within the last decades low-dimensional frustrated quantum spin systems have attracted great interest in the field of modern research. In these systems a competition of various magnetic interactions takes place, leading to an energetically degenerated magnetic ground state, and thus to the occurrence of exotic, unconventional physical properties at low temperatures. This thesis focuses on the quasi one-dimensional frustrated spin chain system linarite, PbCuSO4(OH)2. In this compound the basic building blocks are CuO4 plaquettes which are connected to each other along one crystallographic direction, analogue to a chain. The frustration in linarite is established due to the competition between the magnetic interactions. The nearest-neighbor magnetic spins are coupled ferromagnetically along the chain via a coupling constant J1, while the next-nearest neighbors are coupled antiferromagnetically via a coupling constant J2. For this configuration it is not possible to satisfy all magnetic couplings simultaneously, hence the system is magnetically frustrated. In this work, comprehensive thermodynamic and nuclear magnetic resonance (NMR) studies demonstrate that linarite is one of the richest and most fascinating compounds in the class of low-dimensional frustrated magnets. By means of susceptibility, magnetization, specific heat, magnetocaloric effect, magnetostriction, and thermal-expansion measurements a rich magnetic phase diagram could be mapped out below a temperature of 2.8 K. The phase diagram contains five different magnetic regions/phases for an external magnetic field pointing along the chain direction. Based on the thermodynamic studies it was possible to calculate the exchange integrals within the frustrated J1-J2 model and extensions of it by using various theoretical approaches. The magnetic microscopic nature of the different long-range magnetic phases present in linarite were investigated by NMR measurements and by collaborative neutron scattering experiments. The ground state (phase I) is identified as an incommensurate elliptical helical structure. Via a theoretical modelling the 1H-NMR spectrum of the ground state could be explained, revealing a rearrangement of the zero-field structure in an external magnetic field of 2.0 T used for the NMR studies. By further increasing the external field the system undergoes a complex spin flop transition in two steps (phase I - phase III - phase IV). In phase III a phase separation takes place where one part of the spins form a circular spiral structure while the remaining fraction form a simple antiferromagnetic structure. In phase IV the remaining circular spiral structure vanishes, so that all spins collectively form the antiferromagnetic collinear phase. The most peculiar physical properties studied in this thesis take place in region V at high fields, showing only tiny features in the thermodynamic properties. The magnetic spins in region V form a sine-wave modulated spin-density structure as identified via NMR and neutron investigations. It is discussed whether region V is related to a multipolar phase or if the spin-density wave structure could possibly coexist with such a phase.

In the vast realm of inorganic materials, the Cu2+-containing cuprates form one of the richest classes. Due to the combined effect of crystal-field, covalency and strong correlations, all undoped cuprates are magnetic insulators with well-localized spins S=1/2, whereas the charge and orbital degrees of freedom are frozen out. The combination of the spin-only nature of their magnetism with the unique structural diversity renders cuprates as excellent model systems. The experimental studies, boosted by the discovery of high-temperature superconductivity in doped La2CuO4, revealed a fascinating variety of magnetic behaviors observed in cuprates. A digest of prominent examples should include the spin-Peierls transition in CuGeO3, the Bose-Einstein condensation of magnons in BaCuSi2O6, and the quantum critical behavior of Li2ZrCuO4. The magnetism of cuprates originates from short-range (typically, well below 1 nm) exchange interactions between pairs of spins Si and Sj, localized on Cu atoms i and j. Especially in low-dimensional compounds, these interactions are strongly anisotropic: even for similar interatomic distances |Rij|, the respective magnetic couplings Jij can vary by several orders of magnitude. On the other hand, there is an empirical evidence for the isotropic nature of this interaction in the spin space: different components of Si are coupled equally strong. Thus, the magnetism of cuprates is mostly described by a Heisenberg model, comprised of Jij(Si*Sj) terms. Although the applicability of this approach to cuprates is settled, the model parameters Jij are specific to a certain material, or more precisely, to a particular arrangement of the constituent atoms, i.e. the crystal structure. Typically, among the infinite number of Jij terms, only several are physically relevant. These leading exchange couplings constitute the (minimal) microscopic magnetic model. Already at the early stages of real material studies, it became gradually evident that the assignment of model parameters is a highly nontrivial task. In general, the problem can be solved experimentally, using elaborate measurements, such as inelastic neutron scattering on large single crystals, yielding the magnetic excitation spectrum. The measured dispersion is fitted using theoretical models, and in this way, the model parameters are refined. Despite excellent accuracy of this method, the measurements require high-quality samples and can be carried out only at special large-scale facilities. Therefore, less demanding (especially, regarding the sample requirements), yet reliable and accurate procedures are desirable. An alternative way to conjecture a magnetic model is the empirical approach, which typically relies on the Goodenough-Kanamori rules. This approach links the magnetic exchange couplings to the relevant structural parameters, such as bond angles. Despite the unbeatable performance of this approach, it is not universally applicable. Moreover, in certain cases the resulting tentative models are erroneous. The recent developments of computational facilities and techniques, especially for strongly correlated systems, turned density-functional theory (DFT) band structure calculations into an appealing alternative, complementary to the experiment. At present, the state-of-the-art computational methods yield accurate numerical estimates for the leading microscopic exchange couplings Jij (error bars typically do not exceed 10-15%). Although this computational approach is often regarded as ab initio, the actual procedure is not parameter-free. Moreover, the numerical results are dependent on the parameterization of the exchange and correlation potential, the type of the double-counting correction, the Hubbard repulsion U etc., thus an accurate choice of these crucial parameters is a prerequisite. In this work, the optimal parameters for cuprates are carefully evaluated based on extensive band structure calculations and subsequent model simulations. Considering the diversity of crystal structures, and consequently, magnetic behaviors, the evaluation of a microscopic model should be carried out in a systematic way. To this end, a multi-step computational approach is developed. The starting point of this procedure is a consideration of the experimental structural data, used as an input for DFT calculations. Next, a minimal DFT-based microscopic magnetic model is evaluated. This part of the study comprises band structure calculations, the analysis of the relevant bands, supercell calculations, and finally, the evaluation of a microscopic magnetic model. The ground state and the magnetic excitation spectrum of the evaluated model are analyzed using various simulation techniques, such as quantum Monte Carlo, exact diagonalization and density-matrix renormalization groups, while the choice of a particular technique is governed by the dimensionality of the model, and the presence or absence of magnetic frustration. To illustrate the performance of the approach and tune the free parameters, the computational scheme is applied to cuprates featuring rather simple, yet diverse magnetic behaviors: spin chains in CuSe2O5, [NO]Cu(NO3)3, and CaCu2(SeO3)2Cl2; quasi-two-dimensional lattices with dimer-like couplings in alpha-Cu2P2O7 and CdCu2(BO3)2, as well as the 3D magnetic model with pronounced 1D correlations in Cu6Si6O18*6H2O. Finally, the approach is applied to spin liquid candidates --- intricate materials featuring kagome-lattice arrangement of the constituent spins. Based on the DFT calculations, microscopic magnetic models are evaluated for herbertsmithite Cu3(Zn0.85Cu0.15)(OH)6Cl2, kapellasite Cu3Zn(OH)6Cl2 and haydeeite Cu3Mg(OH)6Cl2, as well as for volborthite Cu3[V2O7](OH)2*2H2O. The results of the DFT calculations and model simulations are compared to and challenged with the available experimental data. The advantages of the developed approach should be briefly discussed. First, it allows to distinguish between different microscopic models that yield similar macroscopic behavior. One of the most remarkable example is volborthite Cu3[V2O7](OH)2*2H2O, initially described as an anisotropic kagome lattice. The DFT calculations reveal that this compound features strongly coupled frustrated spin chains, thus a completely different type of magnetic frustration is realized. Second, the developed approach is capable of providing accurate estimates for the leading magnetic couplings, and consequently, reliably parameterize the microscopic Hamiltonian. Dioptase Cu6Si6O18*6H2O is an instructive example showing that the microscopic theoretical approach eliminates possible ambiguity and reliably yields the correct parameterization. Third, DFT calculations yield even better accuracy for the ratios of magnetic exchange couplings. This holds also for small interchain or interplane couplings that can be substantially smaller than the leading exchange. Hence, band structure calculations provide a unique possibility to address the interchain or interplane coupling regime, essential for the magnetic ground state, but hardly perceptible in the experiment due to the different energy scales. Finally, an important advantage specific to magnetically frustrated systems should be mentioned. Numerous theoretical and numerical studies evidence that low-dimensionality and frustration effects are typically entwined, and their disentanglement in the experiment is at best challenging. In contrast, the computational procedure allows to distinguish between these two effects, as demonstrated by studying the long-range magnetic ordering transition in quasi-1D spin chain systems. The computational approach presented in the thesis is a powerful tool that can be directly applied to numerous S=1/2 Heisenberg materials. Moreover, with minor modifications, it can be largely extended to other metallates with higher value of spin. Besides the excellent performance of the computational approach, its relevance should be underscored: for all the systems investigated in this work, the DFT-based studies not only reproduced the experimental data, but instead delivered new valuable information on the magnetic properties for each particular compound. Beyond any doubt, further computational studies will yield new surprising results for known as well as for new, yet unexplored compounds. Such "surprising" outcomes can involve the ferromagnetic nature of the couplings that were previously considered antiferromagnetic, unexpected long-range couplings, or the subtle balance of antiferromagnetic and ferromagnetic contributions that "switches off" the respective magnetic exchange. In this way, dozens of potentially interesting systems can acquire quantitative microscopic magnetic models. The results of this work evidence that elaborate experimental methods and the DFT-based modeling are of comparable reliability and complement each other. In this way, the advantageous combination of theory and experiment can largely advance the research in the field of low-dimensional quantum magnetism. For practical applications, the excellent predictive power of the computational approach can largely alleviate designing materials with specific properties.