Das Standart-Modell zur Beschreibung von Observablen magnetischer Moleküle ist das Heisenberg-Modell. In diesem wird der Magnetismus des Superaustausches der Elektronen durch einfache bilineare Spin-Spin-Kopplungen beschrieben. Zur genaueren Approximation experimenteller Ergebnisse können, der jeweiligen Struktur des Moleküls entsprechend, verschiedene Erweiterungen des Heisenberg-Modells verwendet werden. Diese werden, explizit für das 4-Spin-System {Ni4Mo12}, in ihren Auswirkungen auf die Hochtemperatur-Nullfeldsuszeptibilität, die Nullfeldsuszeptibilität und die Hochfeldmagnetisierung betrachtet. Die wesentlichen Erweiterungen sind dabei die Einzelionen-Anisotropie, die Dzyaloshinskii-Moriya-Anisotropie und die allgemeinen Kopplungen zweiter Ordnung. Letztere stellen eine Verallgemeinerung der bekannten biquadratischen Kopplungen dar und werden im Rahmen eines magneto-elastischen Modells hergeleitet. Dabei ergeben sich unterschiedliche Einschränkungen der Kopplungsmatrix zweiter Ordnung für starre und flexible Molekülstrukturen. Speziell für {Ni4Mo12} entsprechen die Ergebnisse numerischer Simulationen von Messwerten einer Strukturänderung im externen Magnetfeld.

Deux mécanismes importants reliant la préparation des couches ultraminces d’oxydes magnétiques à leurs propriétés physiques ont été étudiés dans ce travail. En premier lieu, l’influence de la contrainte épitaxiale sur les propriétés magnéto-optiques de la manganite La₂/₃Sr₁/₃MnO₃ (LSMO) a été étudiée. Les couches ultraminces ont été déposées par ablation laser pulsé sur quatre substrats différents, ce qui a fourni différentes valeurs statiques de la contrainte épitaxiale. Les propriétés magnétiques ont été révélées comme se détériorant avec l’augmentation de la contrainte, ce qui était prévisible à cause de la distorsion grandissante de la maille unitaire ainsi qu’à cause de l’effet de la couche magnétiquement inerte. La combinaison de l’ellipsométrie spectroscopique et de la spectroscopie Kerr magnéto-optique a été utilisée afin de déterminer les spectres des éléments diagonaux et non diagonaux du tenseur de permittivité. L’étude des éléments non-diagonaux a confirmé la présence déjà rapportée de deux transitions électroniques dans les spectres de toutes les couches. De plus, elle a révélé une autre transition électronique autour de l’énergie de 4.3 eV, mais seulement dans les spectres des couches déposées avec une contrainte compressive. Nous avons proposé la classification de cette transition comme une transition paramagnétique du champ cristallin Mn t2g → eg. Cette classification a été confortée par des calculs ab initio. Nous avons ainsi montré le rôle clé de la contrainte dans le contrôle des propriétés magnéto-optiques des couches pérovskites ultraminces. En revanche, l’application dynamique de la contrainte par l’utilisation d’une sous-couche piézoélectrique est restée peu concluante. Le transfert de la contrainte entre la sous-couche piézoélectrique et la couche LSMO nécessite des améliorations ultérieures. En second lieu, l’influence de la désorientation du substrat a été étudiée par rapport à la dynamique de l’aimantation dans l’oxyde SrRuO₃ (SRO). Comme attendu, nous avons trouvé qu’un grand angle de désorientation mène à la suppression de la croissance de plusieurs variants cristallographiques du SRO. Au moyen de la microscopie à force magnétique, nous avons montré que la présence de plusieurs variants de SRO mène à l’augmentation de la densité de défauts agissant comme points d’ancrage ou de nucléation pour les domaines magnétiques. Nous avons donc montré que l’emploi d’un substrat vicinal est important pour la fabrication des couches ultraminces de SRO de haute qualité, avec une faible densité de défauts cristallographiques et d’excellentes propriétés magnétiques. / Two important mechanisms in preparation of ultrathin films of magnetic oxides were systematically investigated in this work. First, influence of epitaxial strain on resulting magneto-optical properties of La₂/₃Sr₁/₃MnO₃ (LSMO) ultrathin films was studied. The investigated films were grown by pulsed laser deposition on four different substrates, providing a broad range of induced epitaxial strains. Magnetic properties were found to deteriorate with increasing value of the epitaxial strain, as expected due to the unit cell distortion increasingly deviating from the bulk and effect of the magnetically inert layer. A combination of spectroscopic ellipsometry and magneto-optical Kerr effect spectroscopy was used to determine spectra of the diagonal and off-diagonal elements of permittivity tensor. The off-diagonal elements confirmed presence of two previously reported electronic transitions in spectra of all films. Moreover, they revealed another electronic transition around 4.3 eV only in spectra of films grown under compressive strain. We proposed classification of this transition as crystal field paramagnetic Mn t2g → eg transition, which was further supported by ab initio calculations. A key role of strain in controlling electronic structure of ultrathin perovskite films was demonstrated. Dynamic application of strain via use of piezoelectric underlayer remained inconclusive, requiring further improvement of the strain transfer from the piezoelectric layer into the LSMO. Second, influence of substrate miscut on magnetization dynamics in SrRuO₃ (SRO) was studied. As expected we found that high miscut angle leads to suppression of multi-variant growth. By means of magnetic force microscopy we showed that presence of multiple SRO variants leads to higher density of defects acting as pinning or nucleation sites for the magnetic domains, which consequently results in deterioration of magnetic properties. We demonstrated that use of vicinal substrate with high miscut angle is important for fabrication of high quality SRO ultrathin films with low density of crystallographic defects and excellent magnetic properties.

The main objective of the thesis was to construct a wide-field Kerr microscope to study all-optical helicity-dependent (AOHDS) switching in FePt nanograins. The wide- field Kerr microscope was successfully implemented into AOHDS experiments, was fully characterized and optimized for maximum image contrast. The real-time imaging and resolution of 2, 5µm enables the study of a wide range of magnetic materials and their dynamics. Moreover, a new light source, the High Lumen Density MODULE from CRY- TUR, spol. s r.o., was tested for future application in Kerr microscopy. The technical solution enabled to form a collimated beam with low divergence required for Kerr mi- croscopy. From the switching experiments on FePt nanograins, we observed a strong non-magnetic contribution to the magnetic signal, not reported in previous works. The experiments have also shown that the switching intensity depends on the laser spot size and total laser power, suggesting that the FePt grains are not entirely isolated. The grains' ensemble exhibits a more complex behavior than anticipated. 1

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We derive the amplitude expansion for a phase-field-crystal (APFC) model that captures the basic physics of magneto-structural interactions. The symmetry breaking due to magnetization is demonstrated, and the characterization of the magnetic anisotropy for a bcc crystal is provided. This model enables a convenient coarse-grained description of crystalline structures, in particular when considering the features of the APFC model combined with numerical methods featuring inhomogeneous spatial resolution. This is shown by addressing the shrinkage of a spherical grainwithin amatrix, chosen as a prototypical system to demonstrate the influence of different magnetizations. These simulations serve as a proof of concept for the modeling of manipulation of dislocation networks and microstructures in ferromagnetic materials within the APFC model.

The dissertation explores a framework for numerically simulating the deformation of the liquid metal wall's free surface in Z-pinch fusion devices. This research is conducted in the context of utilizing liquid metals as plasma-facing components in fusion reactors. In the Z-pinch fusion process, electric current travels through a plasma column and enters into a pool of liquid metal. The current flowing through the liquid metal generates Lorentz force, which deforms the free surface of the liquid metal. Modeling this phenomenon is essential as it offers insights into the feasibility of using liquid metal as an electrode wall in such fusion devices. The conventional magneto-hydrodynamic (MHD) formulation aims at modeling the situation where an external magnetic field is applied to flows involving electrically conducting liquids, with the initial magnetic field is known and then evolved over time through magnetic induction equation. However, in Z-pinch fusion devices, the electric current is directly injected into a conducting liquid. In these situations, an analytical expression for the magnetic field generated by the applied current is not readily available, necessitating numerical calculations. Moreover, the deformation of the liquid metal surface changes the geometry of the current path over time and the resulting magnetic field. By directly solving the Maxwell equations in combination with Navier-Stokes equations, it becomes possible to predict the magnetic field even when the fluid is in motion. In this dissertation, a numerical framework utilizing the Maxwell-Navier-Stokes system is explored to successfully capture the deformation of the liquid metal's free surface due to applied electric current. / Doctor of Philosophy / In this dissertation, a method is described that uses a computer to simulate how the initially stable, flat surface of liquid metal deforms when subjected to electrical currents in Z-pinch fusion devices, a specific type of nuclear fusion technology. Z-pinch fusion devices generate plasma, a hot fluid-like substance, through the nuclear fusion process, triggered and maintained by strong pulsated current. There's a growing interest in using liquid metal as the first layer of material to isolate the hot plasma from the rest of the nuclear fusion reactor body, rather than solid materials, due to its unique benefits. However, the Z-pinch fusion process, by introducing electric currents through the liquid metal layer, induces a Lorentz force that consequently deforms the surface of the liquid metal. Developing a tool to predict this deformation is vital as it aids in evaluating the potential of using liquid metal as a plasma-facing layer over solid materials in these fusion devices. The simulation tools presented in this dissertation are able to successfully captures the dynamics of how the liquid metal surface deforms under the impact of electrical currents.

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