A way to obtain materials that show novel phenomena is to explore the interplay between geometry and interactions. When it is not geometrically possible to satisfy all the interactions by a given configuration, then to find the ground state becomes very complicated. This interplay between geometry and interactions defines geometrical frustration. One of the most popular examples of geometrical frustration in magnetism is spin ice. In this system, nearest neighbour ferromagnetic interactions between Ising spins in a pyrochlore structure emulate water ice by showing the same degree of frustration. This is manifested by the same ground state residual entropy. Although the clearest example of spin ice among magnets is shown by Dy₂Ti₂O₇, the behaviour of this material is richer than that of pure spin ice. The large magnetic moments of the rare earth Dy form a spin ice that also interacts via dipolar interactions. These long range interactions give rise to monopolar excitations which dramatically affect the dynamics of the system with respect to the pure spin ice case. In this thesis magnetisation experiments and numerical methods are used to explore the properties of the magnetic insulator Dy₂Ti₂O₇. We study its excitations at low temperature and describe the out-of-equilibrium characteristics of the magnetisation processes, below a temperature where the system freezes out. For temperatures above the freezing temperature, we describe and measure a 3D Kasteleyn transition and the concomitant Dirac strings associated to it, for the field in the [100] crystallographic direction. For temperatures below the freezing temperature, we find new out-of-equilibrium phenomena. Magnetic jumps are measured and their sweep rate dependence analysed. A deflagration theory is proposed and supported by simultaneous magnetisation and sample temperature measurements obtained by a new design of a Faraday magnetometer.

Made available in DSpace on 2015-03-26T13:35:18Z (GMT). No. of bitstreams: 1 texto completo.pdf: 2056393 bytes, checksum: 6c718958e16dde37636b88ed5dbf583f (MD5) Previous issue date: 2012-02-14 / Fundação de Amparo a Pesquisa do Estado de Minas Gerais / We study the magnetic excitations in two-dimensional spin ices on square lattices, by means of computer simulations. These materials are artificially produced by lithographic techniques, using ferromegnetic nano-islands arranged in a lattice especially organized in such a way, that, the lattice geometry together with the dipole-dipole interactions lead to an intrinsic frustration of the system. Our analysis, based only on the dipolar interaction between the islands, correctly reproduces the ground state experimentally observed recently. In addition, we verify the emergence of magnetic excitations that behave like magnetic monopoles, carrying isolated magnetic charge. These quasi-particles interact by means of the Coulomb potential plus a linear confining potential, which is attributed to the emergence of string-like excitations, linking the pair of opposite charges. However, we argue that the string has a configurational entropy, so that the string tension may decrease as the temperature is increased and then, free magnetic monopoles should be found in two-dimensional spin ices at a critical temperature. We also study the case where the artificial spin ice is built with missing nano-island (vacancy). For the case with only one vacancy, we found that the defect modify the potential obtained for the normal lattice. The vacancy behaves like a pair of opposite charges, carrying half charge of the usual magnetic monopole excitation. Our calculations show that when the smallest distance between the charges (or the string) is greater than 2a (a is the lattice spacing), the interaction of the string with the defect is negligible. However, for distances smaller than 2a, the string interacts with the defect more appreciable, in a very complicated way, which depends on the shape and size of the string. Our results indicate that, on each vertex where the string passes, there is an additional quadrupole moment and so the field created by the string decays very quickly. / Nós estudamos as excitações magnéticas que surgem nos gelos de spin bidimensionais, por meio de simulações computacionais em redes quadradas. Esses materiais são produzidos artificialmente, através de técnicas litográficas utilizando nanopartículas ferromagnéticas arranjadas em uma rede especialmente organizada, de modo que a geometria da rede juntamente com a interação dipolo-dipolo leva a uma frustração intríseca do sistema. A análise, baseada somente na interação dipolar entre as nanoilhas, reproduz corretamente o estado fundamental recentemente observado experimentalmente. Foi verificado a emergência de excitações magnéticas que se comportam como monopolo magnético, carregando carga magnética isolada. Essas quasi-partículas interagem via potencial coulombiano adicionado a um potencial confinante linear, atribuído ao aparecimento de excitações do tipo corda, que conectam o par monopolo-antimonopolo. Contudo, verificamos que a corda possui uma entropia configuracional, de modo que a tensão da corda pode diminuir à medida em que a temperatura é aumentada, fazendo com que os monopolos magnéticos possam ser encontrados livres nos gelos de spin bidimensionais em uma temperatura crítica. Também estudamos o caso em que o gelo de spin é construído com uma única ilha faltante em uma dada posição da rede. Foi visto que o defeito pertuba o potencial obtido em uma rede normal. A vacância se comporta como um par de cargas opostas carregando metade da carga do monopolo magnético usual. Nossos cálculos mostram que quando a menor distância entre uma carga e a vacância é maior que 2a (a é o espaçamento de rede), a interação entre a corda e o defeito é negligenciável. Contudo, para distâncias menores que 2a, a corda interage mais apreciavelmente com o defeito, de uma forma muito complicada que depende de seu tamanho e forma. Os resultados indicam que em cada vértice por onde a corda passa, existe um momento de quadrupolo magnético adicional, de forma que o campo criado pela corda decai muito rapidamente.

Cette thèse se concentre sur l'étude de composés magnétiques géométriquement frustrés où les ions magnétiques se situent aux sommets d'un réseau de tétraèdres partageant leurs sommets: les composés pyrochlores. Deux familles de formule chimique R2M2O7, où R est un lanthanide et M= Ti, Sn, sont particulièrement intéressantes puisqu'elles présentent une grande variété d'états magnétiques exotiques. Premièrement, nous avons étudié le champ cristallin agissant au site de la terre rare dans l'approximation de Stevens où uniquement le terme fondamental est considéré. Un jeu unique de paramètres a été déterminé pour chaque famille considérée grâce à une analyse globale incluant des spectres de neutrons inélastiques de plusieurs composés. Ensuite, nous avons caractérisé avec un large éventail de techniques les propriétés physiques à basse température de Nd2Sn2O7. En dessous de la température de transition Tc=0.91 K, ce composé possède un ordre magnétique à longue portée dans la configuration de spins dite "all-in-all-out". Une persistance de la dynamique de spins a été révélée dans la phase ordonnée, attribuée à des excitations unidimensionnelles de spins. Une dynamique de spins anormalement lente est également reportée dans la phase paramagnétique. Enfin, nous avons apporté quelques informations sur les deux états fondamentaux proposés pour le composé très étudié Tb2Ti2O7: premièrement, l'apparition d'une transition Jahn-Teller à basse température est suggérée mais l'absence d'élargissement des pics de Bragg réfute la présence d'une transition structurale. Enfin ce composé pourrait être un exemple d'une glace de spin quantique mais l'existence d'un plateau d'aimantation n'est pas évident jusqu'à T=20 mK. / This Phd thesis focuses on the study of magnetically frustrated compounds where magnetic ions lie at the vertices of a corner-sharing tetrahedra network: the pyrochlore compounds. The two series of chemical formula R2M2O7, where R is a lanthanide and M=Ti, Sn, are of peculiar interest since they display a large variety of exotic magnetic ground states. First, we have studied the crystal-electric-field acting at the rare earth within the Stevens approximation where only the ground state multiplet is considered. A single set of parameters for each families of interest has been determined through a global analysis including several inelastic neutron scattering spectra of various compounds. Then, we have characterised with a large panel of techniques the low temperature physical properties of Nd2Sn2O7. This compound enters a long-range magnetic order at transition temperature Tc=0.91 K with an ``all-in-all-out'' spin configuration. A persistence of spin dynamics has been found in the ordered phase, ascribed to one-dimensional spin loops excitations. Anomalously slow paramagnetic spin fluctuations are also reported. Finally, we have brought information on the two proposed ground states of the widely studied compound Tb2Ti2O7: first, a Jahn-Teller transition is claimed to occur at low temperatures but no broadening of the Bragg peaks is seen down to T=4 K precluding premises of a structural transition. Secondly, this compound could be a realisation of a quantum spin-ice but no definitive evidence of a magnetisation plateau is found down to T=20 mK.

Cette thèse se concentre sur l'étude de composés magnétiques géométriquement frustrés où les ions magnétiques se situent aux sommets d'un réseau de tétraèdres partageant leurs sommets: les composés pyrochlores. Deux familles de formule chimique R2M2O7, où R est un lanthanide et M= Ti, Sn, sont particulièrement intéressantes puisqu'elles présentent une grande variété d'états magnétiques exotiques. Premièrement, nous avons étudié le champ cristallin agissant au site de la terre rare dans l'approximation de Stevens où uniquement le terme fondamental est considéré. Un jeu unique de paramètres a été déterminé pour chaque famille considérée grâce à une analyse globale incluant des spectres de neutrons inélastiques de plusieurs composés. Ensuite, nous avons caractérisé avec un large éventail de techniques les propriétés physiques à basse température de Nd2Sn2O7. En dessous de la température de transition Tc=0.91 K, ce composé possède un ordre magnétique à longue portée dans la configuration de spins dite "all-in-all-out". Une persistance de la dynamique de spins a été révélée dans la phase ordonnée, attribuée à des excitations unidimensionnelles de spins. Une dynamique de spins anormalement lente est également reportée dans la phase paramagnétique. Enfin, nous avons apporté quelques informations sur les deux états fondamentaux proposés pour le composé très étudié Tb2Ti2O7: premièrement, l'apparition d'une transition Jahn-Teller à basse température est suggérée mais l'absence d'élargissement des pics de Bragg réfute la présence d'une transition structurale. Enfin ce composé pourrait être un exemple d'une glace de spin quantique mais l'existence d'un plateau d'aimantation n'est pas évident jusqu'à T=20 mK. / This Phd thesis focuses on the study of magnetically frustrated compounds where magnetic ions lie at the vertices of a corner-sharing tetrahedra network: the pyrochlore compounds. The two series of chemical formula R2M2O7, where R is a lanthanide and M=Ti, Sn, are of peculiar interest since they display a large variety of exotic magnetic ground states. First, we have studied the crystal-electric-field acting at the rare earth within the Stevens approximation where only the ground state multiplet is considered. A single set of parameters for each families of interest has been determined through a global analysis including several inelastic neutron scattering spectra of various compounds. Then, we have characterised with a large panel of techniques the low temperature physical properties of Nd2Sn2O7. This compound enters a long-range magnetic order at transition temperature Tc=0.91 K with an ``all-in-all-out'' spin configuration. A persistence of spin dynamics has been found in the ordered phase, ascribed to one-dimensional spin loops excitations. Anomalously slow paramagnetic spin fluctuations are also reported. Finally, we have brought information on the two proposed ground states of the widely studied compound Tb2Ti2O7: first, a Jahn-Teller transition is claimed to occur at low temperatures but no broadening of the Bragg peaks is seen down to T=4 K precluding premises of a structural transition. Secondly, this compound could be a realisation of a quantum spin-ice but no definitive evidence of a magnetisation plateau is found down to T=20 mK.

Neste trabalho estudamos o modelo da rede de Kondo em uma rede kagome, buscando uma maior compreensão dos efeitos da frustração geométrica em sistemas de férmions pesados. Para tanto, fizemos uma aproximação de campo médio no hamiltoniano do sistema que serve para todas as fases do sistema. Analisamos inicialmente o caso não magnético. Obtemos neste limite as energias eletrônicas e as funções de Green necessárias ao cálculo numérico autoconsistente das ocupações e do parâmetro de Kondo. Os resultados encontrados estão em concordância qualitativa com trabalhos publicados em outras geometrias. A seguir analisamos o caso magnético, onde introduzimos uma aproximação suplementar, a qual é compatível com a de campo médio já considerada e, em princípio, existente apenas em sistemas com frustração geométrica. Realizamos cálculos autoconsistentes através de somas sobre as frequências de Matsubara. Os resultados mostram que não há coexistência entre ordem magnética e efeito Kondo, além de haver a supressão do antiferromagnetismo com o aumento de temperatura e variações no preenchimento de bandas. / In this work we study the Kondo Lattice model for the kagome lattice, in order to understand better the effects of geometrical frustration in heavy-fermion systems. In this context, we consider a mean field scheme valid for all the system’s phases. Firstly, we analyzed the nonmagnetic case. In this approximation the electron energies and spectral functions are reachable, then we use the density of states to calculate the occupations selfconsistently. Our results are qualitatively compared with previous works in other geometries. In the second part we introduce an approximation for magnestism, which takes into account the mean field scheme considered and the presence of geometrical frustration. Self-consistent calculations are done through the frequencies summation method. Our results show that the magnetism is supressed when the temperature is increased or the band filling deviates from half-filling. Besides, the coexistence of magnetic order and Kondo effect is not observable.

Neste trabalho estudamos o modelo da rede de Kondo em uma rede kagome, buscando uma maior compreensão dos efeitos da frustração geométrica em sistemas de férmions pesados. Para tanto, fizemos uma aproximação de campo médio no hamiltoniano do sistema que serve para todas as fases do sistema. Analisamos inicialmente o caso não magnético. Obtemos neste limite as energias eletrônicas e as funções de Green necessárias ao cálculo numérico autoconsistente das ocupações e do parâmetro de Kondo. Os resultados encontrados estão em concordância qualitativa com trabalhos publicados em outras geometrias. A seguir analisamos o caso magnético, onde introduzimos uma aproximação suplementar, a qual é compatível com a de campo médio já considerada e, em princípio, existente apenas em sistemas com frustração geométrica. Realizamos cálculos autoconsistentes através de somas sobre as frequências de Matsubara. Os resultados mostram que não há coexistência entre ordem magnética e efeito Kondo, além de haver a supressão do antiferromagnetismo com o aumento de temperatura e variações no preenchimento de bandas. / In this work we study the Kondo Lattice model for the kagome lattice, in order to understand better the effects of geometrical frustration in heavy-fermion systems. In this context, we consider a mean field scheme valid for all the system’s phases. Firstly, we analyzed the nonmagnetic case. In this approximation the electron energies and spectral functions are reachable, then we use the density of states to calculate the occupations selfconsistently. Our results are qualitatively compared with previous works in other geometries. In the second part we introduce an approximation for magnestism, which takes into account the mean field scheme considered and the presence of geometrical frustration. Self-consistent calculations are done through the frequencies summation method. Our results show that the magnetism is supressed when the temperature is increased or the band filling deviates from half-filling. Besides, the coexistence of magnetic order and Kondo effect is not observable.

Neste trabalho estudamos o modelo da rede de Kondo em uma rede kagome, buscando uma maior compreensão dos efeitos da frustração geométrica em sistemas de férmions pesados. Para tanto, fizemos uma aproximação de campo médio no hamiltoniano do sistema que serve para todas as fases do sistema. Analisamos inicialmente o caso não magnético. Obtemos neste limite as energias eletrônicas e as funções de Green necessárias ao cálculo numérico autoconsistente das ocupações e do parâmetro de Kondo. Os resultados encontrados estão em concordância qualitativa com trabalhos publicados em outras geometrias. A seguir analisamos o caso magnético, onde introduzimos uma aproximação suplementar, a qual é compatível com a de campo médio já considerada e, em princípio, existente apenas em sistemas com frustração geométrica. Realizamos cálculos autoconsistentes através de somas sobre as frequências de Matsubara. Os resultados mostram que não há coexistência entre ordem magnética e efeito Kondo, além de haver a supressão do antiferromagnetismo com o aumento de temperatura e variações no preenchimento de bandas. / In this work we study the Kondo Lattice model for the kagome lattice, in order to understand better the effects of geometrical frustration in heavy-fermion systems. In this context, we consider a mean field scheme valid for all the system’s phases. Firstly, we analyzed the nonmagnetic case. In this approximation the electron energies and spectral functions are reachable, then we use the density of states to calculate the occupations selfconsistently. Our results are qualitatively compared with previous works in other geometries. In the second part we introduce an approximation for magnestism, which takes into account the mean field scheme considered and the presence of geometrical frustration. Self-consistent calculations are done through the frequencies summation method. Our results show that the magnetism is supressed when the temperature is increased or the band filling deviates from half-filling. Besides, the coexistence of magnetic order and Kondo effect is not observable.

Submitted by Renata Lopes (renatasil82@gmail.com) on 2017-06-28T14:29:11Z No. of bitstreams: 1 damiaodesousavieirajunior.pdf: 10265456 bytes, checksum: 8b1ceaeb4c4be0e91a46c2d30add7349 (MD5) / Approved for entry into archive by Adriana Oliveira (adriana.oliveira@ufjf.edu.br) on 2017-08-07T21:17:55Z (GMT) No. of bitstreams: 1 damiaodesousavieirajunior.pdf: 10265456 bytes, checksum: 8b1ceaeb4c4be0e91a46c2d30add7349 (MD5) / Made available in DSpace on 2017-08-07T21:17:55Z (GMT). No. of bitstreams: 1 damiaodesousavieirajunior.pdf: 10265456 bytes, checksum: 8b1ceaeb4c4be0e91a46c2d30add7349 (MD5) Previous issue date: 2016-02-03 / CAPES - Coordenação de Aperfeiçoamento de Pessoal de Nível Superior / O contínuo desenvolvimento das técnicas de fabricação de estruturas em escala nanométrica, com considerável precisão e reprodutibilidade, tem permitido e estimulado a investigação científica em torno das propriedades básicas e novas aplicações tecnológicas desses sistemas. Especialmente a partir dos anos 90, é crescente o interesse da comunidade científica no comportamento de sistemas magnéticos nano-estruturados. Nestes, a quebra da simetria espacial devido às pequenas dimensões faz com que exibam comportamentos completamente distintos dos observados em amostras macroscópicas. A anisotropia de forma resultante das interações clássicas entre os dipolos magnéticos permite a formação de estruturas magnéticas exóticas em nanomagnetos como vórtices, skyrmions, paredes de domínio individuais e, até mesmo, excitações topológicas similares a monopolos magnéticos. A compreensão e controle do comportamento magnético estático e dinâmico dessas estruturas é fundamental para o desenvolvimento de novos dispositivos tecnológicos baseados em spintrônica. Neste trabalho foram estudadas nanopartículas planares, alongadas na forma elíptica, de material ferromagnético macio, especificamente o Permalloy-79. Tais nanopartículas tem atraído atenção devido ao seu potencial de aplicação prática no desenvolvimento de novos sensores, dispositivos de lógica, mídias de armazenamento de dados de alta densidade e dispositivos MRAM (Magnetic Random Access Memory). Pelo viés do interesse científico básico, tais nano-ilhas ferromagnéticas são a unidade fundamental em arranjos magnéticos bidimensionais geometricamente frustrados, como sistemas de gelo de spin artificiais. Nestes sistemas o arranjo geométrico das ilhas quebra a degenerescência do estado fundamental da rede, caracterizando um estado de frustração geométrica que permite excitações de comportamento análogo ao de monopólos magnéticos. Sob tais aspectos, é essencial caracterizar as configurações magnéticas no estado fundamental e os processos de reversão da magnetização em nanopartículas individuais. A forma elíptica planar gera uma forte anisotropia magnética, definindo duas configurações fundamentais para a magnetização do estado fundamental das nanopartículas: o estado de vórtice ou o estado alinhado ao longo do maior eixo — estado tipo C. A partir de uma razão de aspecto limite, a magnetização do estado fundamental é confinada no plano e ao longo do eixo maior de cada nano ilha, definindo um nanomagneto monodomínio com dois estados degenerados de magnetização, útil às aplicações previamente descritas. Partindo desse intuito estudamos inicialmente, através de simulação por dinâmica de spin, a competição entre os estados de vórtice e os estados alinhados tipo C como uma função da forma de cada nano-ilha elíptica, construindo um diagrama de fases de estados vórtice - tipo C. Cada nanopartícula magnética é modelada por momentos magnéticos que interagem via interação de troca entre primeiros vizinhos e por interação dipolar clássica de longo alcance. Nossos resultados mostram que é possível fabricar nano-ilhas alongadas com estado fundamental alinhado tipo C em razões de aspecto menores que dois. Este é um resultado interessante do ponto de vista tecnológico, pois permite usar ilhas menores que as atuais em pesquisas com gelos de spin e MRAM. Geralmente, os arranjos experimentais são feitos com nanopartículas de razão de aspecto próximas a três para garantir o estado fundamental alinhado da magnetização. Acrescentando ao modelo um termo de interação Zeeman com um campo magnético externo, estudamos o comportamento da reversão da magnetização nas nanopartículas. Consideramos espessuras diferentes e duas razões de aspecto distintas: uma do tamanho experimental usual e outra menor proposta a partir de nossos resultados. Aplicando campo magnético senoidal em diferentes frequências e em direções distintas no plano das nanoilhas, observou-se a dependência dos processos de reversão em função da espessura das partículas e com a direção e frequência do campo aplicado. Os resultados permitem traçar linhas gerais acerca do comportamento da reversão da magnetização nas nanopartículas individuais sob campo magnético externo. Evidentemente para o desenvolvimento das possíveis aplicações tecnológicas, inclusive o controle de excitações como monopólos magnéticos em gelos de spin, é crucial entender os processos ultra rápidos de reversão da magnetização, o que envolve a aplicação de campo externo de alta frequência em direções cuidadosamente definidas. Com esse objetivo, também estudamos a reversão da magnetização nas nano-ilhas por pulsos curtos de campo magnético (da ordem de nanosegundos) aplicados em diferentes direções. Observamos uma forte dependência da coerência da reversão da magnetização com a direção do campo aplicado e uma significante diferença na dependência angular da coercividade em relação ao observado em trabalhos prévios para campos aplicados na condição quase-estática. Finalmente, baseado em nossos resultados, propomos um método para o controle da reversão coerente da magnetização de nanopartículas individuais em matrizes quadradas de gelos de spin artificiais. Acreditamos que nossos resultados poderão ser úteis no desenvolvimento ulterior de arranjos magnéticos artificiais geometricamente frustrados e no controle das excitações topológicas destes sistemas. / The continuous development of structures fabrication techniques at the nanometer scale with considerable precision and reproducibility has allowed and encouraged scientific research around the basic properties and new technological applications of these systems. Especially from the 90's, there is growing interest of the scientific community in the behavior of nanostructured magnetic systems. In these, the breaking of spatial symmetry due to small dimensionality causes quite different behaviors from those observed in the bulk. The resulting shape anisotropy of the classical interaction between magnetic dipoles allows the formation of exotic magnetic structures in nanomagnets as vortices, skyrmions, single domain walls and even topological excitations similar to magnetic monopoles. The understanding and control of static and dynamic magnetic behavior of these structures is essential for the development of new technological devices based on spintronics. In this work we studied planar elongated nanoparticles in the elliptical shape of soft ferromagnetic material, specifically the Permalloy-79. Such nanoparticles have attracted attention because of their potential to practical application in the development of new sensors, logic devices, high density data storage media and MRAM (Magnetic Random Access Memory) devices. By the bias of basic scientific interest, such ferromagnetic nano-islands are the fundamental unit in two-dimensional magnetic arrangements geometrically frustrated as artificial spin ice systems. In these systems, the geometric arrangement of islands break the degeneracy of the network ground state featuring a state of geometrical frustration that allows excitations with analogous behavior of magnetic monopoles. Under these aspects, it is essential to characterize the magnetic configurations in the ground state and the magnetization reversal processes in individual nanoparticles. The elliptical planar shape generates a strong magnetic anisotropy which defines two basic configurations for the magnetization of the ground state of the nanoparticles: the vortex state or the aligned state along the major axis - type C state. As from an aspect ratio limit value, the magnetization of the ground state is confined in the plane and along the major axis of each nano-island defining mono-domain nanomagnet with two degenerate states of magnetization, useful for the applications previously described. Starting from this purpose we study initially, through simulation by spin dynamics, the competition between the vortex states and aligned type C states as a function of the shape of each elliptical nano-island to build a states diagram. Each magnetic nanoparticle is modeled by magnetic moments that interact by exchange interaction between nearest neighbors and by the classical long-range dipolar interaction. Our theoretical results indicate the possibility to manufacture elongated nano-islands with ground state like aligned C state for aspect ratios less than two. This is an interesting result from the technological point of view because it will be possible to use smaller islands in researches on spin ice and MRAM. Generally, the experimental arrangements are made with nanoparticles of aspect ratio close to three to ensure aligned magnetization in the ground state. Adding to the model a Zeeman interaction term between the magnetic moments and an external magnetic field we study the behavior of the magnetization reversal in nanoparticles. We consider different thickness and two different aspect ratios: one in the usual experimental size and a smaller proposed from our results. Applying sinusoidal magnetic field at different frequencies along the anisotropy axis in directions of ten and forty-five degrees from this, we observed the dependence of the reversal processes on the thickness of the particles and with the direction and frequency of the applied field. The results allow to establish general guidelines about the magnetization reversal behavior of the individual nanoparticles under external magnetic field. Evidently, for the development of possible technological applications, including the control of excitation like magnetic monopoles in spin ice, it is crucial to understand the ultrafast magnetization reversal processes which involves the application of high frequency magnetic fields in carefully defined directions. With this aim, we also studied the magnetization reversal of the nano-islands by short pulses of magnetic field (of the nanosecond order) applied in different directions. We observed a strong dependence on the coherence of the magnetization reversal with the direction of the applied field and a significant difference in the angular dependence of the coercivity compared to those seen in previous studies with applied magnetic fields in quasistatic conditions. Finally, based on our results we propose a method for the control of the coherent magnetization reversal of individual nanoparticles in square artificial spin ice arrays. We believe that our results may be useful in further developments of geometrically frustrated magnetic artificial arrangements and in the control of the topological excitations of these systems.

Uměle vytvořené systémy spinového ledu jsou vhodným nástrojem pro zkoumání neobvyklých jevů, které se v přírodě dají jen těžko pozorovat. Speciálním případem umělého spinového ledu je kagome mřížka, která umožňuje zkoumat kolektivní chování spinů v látce. Tento systém má řadu předpovězených exotických magnetických fází, které zatím nebyly změřeny a prozkoumány v reálném prostoru. V rámci této práce se zabýváme úpravou kagome mřížky tak, aby mohla být využita ke zkoumání exotických stavů v reálném prostoru. Experimenty provedené na naší upravené mřížce ukazují, že jsme schopni detekovat nízko i vysoko energiové stavy, a tedy, že námi navržená úprava kagome mřížky je vhodná pro zkoumání exotických stavů v reálném prostoru.

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.