@phdthesis{Kagerer2024, author = {Kagerer, Philipp Thomas}, title = {Two-Dimensional Ferromagnetism and Topology at the Surface of MnBi\(_2\)Te\(_4\) - Bi\(_2\)Te\(_3\) Heterostructures - MBE Growth, Magnetism and Electronic Properties}, doi = {10.25972/OPUS-36012}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-360121}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2024}, abstract = {In this thesis, a model system of a magnetic topological heterostructure is studied, namely a heterosystem consisting of a single ferromagnetic septuple-layer (SL) of \(MnBi_2Te_4\) on the surface of the three-dimensional topological insulator \(Bi_2Te_3\). Using MBE and developing a specialized experimental setup, the first part of this thesis deals with the growth of \(Bi_2Te_3\) and thin films of \(MnBi_2Te_4\) on \(BaF_2\)-substrates by the co-evaporation of its binary constituents. The structural analysis is conducted along several suitable probes such as X-ray diffraction (XRD, XRR), AFM and scanning tunnelling electron microscopy (STEM). It is furthermore found that the growth of a single septuple-layer of \(MnBi_2Te_4\) on the surface of \(Bi_2Te_3\) can be facilitated. By using X-ray absorption and circular magnetic dichroism (XAS, XMCD), the magnetic properties of \(MnBi_2Te_4\) are explored down to the monolayer limit. The layered nature of the vdW crystal and a strong uniaxial magnetocrystalline anisotropy establish stable out-of plane magnetic order at the surface of \(MnBi_2Te_4\), which is stable even down to the 2D limit. Pushing the material system to there, i.e. a single SL \(MnBi_2Te_4\) further allows to study the phase transition of this 2D ferromagnet and extract its critical behaviour with \(T_c \, = \, 14.89~k\) and \(\beta \, = \, 0.484\). Utilizing bulk crystals of the ferromagnetic \(Fe_3GeTe_2\) as substrate allows to influence, enhance and bias the magnetism in the single SL of \(MnBi_2Te_4\). By growing heterostructures of the type \(MnBi_2Te_4\) -- n layer \(Bi_2Te_3\) -- \(Fe_3GeTe_2\)for n between 0 and 2, it is shown, that a considerable magnetic coupling can be introduced between the \(MnBi_2Te_4\) top-layer and the substrate. Finally the interplay between topology and magnetism in the ferromagnetic extension is studied directly by angle-resolved photoemission spectroscopy. The heterostructure is found to host a linearly dispersing TSS at the centre of the Brillouin zone. Using low temperature and high-resolution ARPES a large magnetic gap opening of \(\sim\) 35 meV is found at the Dirac point of the TSS. By following its temperature evolution, it is apparent that the scaling behaviour coincides with the magnetic order parameter of the modified surface.}, subject = {Molekularstrahlepitaxie}, language = {en} } @phdthesis{Trabel2019, author = {Trabel, Mirko}, title = {Growth and Characterization of Epitaxial Manganese Silicide Thin Films}, doi = {10.25972/OPUS-18472}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-184720}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2019}, abstract = {This thesis describes the growth and characterization of epitaxial MnSi thin films on Si substrates. The interest in this material system stems from the rich magnetic phase diagram resulting from the noncentrosymmetric B20 crystal structure. Here neighboring spins prefer a tilted relative arrangement in contrast to ferro- and antiferromagnets, which leads to a helical ground state where crystal and spin helix chirality are linked [IEM+85]. This link makes the characterization and control of the crystal chirality the main goal of this thesis. After a brief description of the material properties and applied methods, the thesis itself is divided into four main parts. In the first part the advancement of the MBE growth process of MnSi on Si\((111)\) substrate as well as the fundamental structural characterization are described. Here the improvement of the substrate interface by an adjusted substrate preparation process is demonstrated, which is the basis for well ordered flat MnSi layers. On this foundation the influence of Mn/Si flux ratio and substrate temperature on the MnSi layer growth is investigated via XRD and clear boundaries to identify the optimal growth conditions are determined. The nonstoichiometric phases outside of this optimal growth window are identified as HMS and Mn\(_5\)Si\(_3\). Additionally, a regime at high substrate temperatures and low Mn flux is discovered, where MnSi islands are growing incorporated in a Si layer, which could be interesting for further investigations as a size confinement can change the magnetic phase diagram [DBS+18]. XRD measurements demonstrate the homogeneity of the grown MnSi layers over most of the 3 inch wafer diameter and a small \(\omega\)-FWHM of about 0.02° demonstrates the high quality of the layers. XRD and TEM measurements also show that relaxation of the layers happens via misfit dislocations at the interface to the substrate. The second part of the thesis is concerned with the crystal chirality. Here azimuthal \(\phi\)-scans of asymmetric XRD reflections reveal twin domains with a \(\pm\)30° rotation to the substrate. These twin domains seem to consist of left and right-handed MnSi, which are connected by a mirror operation at the \((\bar{1}10)\) plane. For some of the asymmetric XRD reflections this results in different intensities for the different twin domains, which reveals that one of the domains is rotated +30° and the other is rotated -30°. From XRD and TEM measurements an equal volume fraction of both domains is deduced. Different mechanisms to suppress these twin domains are investigated and successfully achieved with the growth on chiral Si surfaces, namely Si\((321)\) and Si\((531)\). Azimuthal \(\phi\)-scans of asymmetric XRD reflections demonstrate a suppression of up to 92\%. The successful twin suppression is an important step in the use of MnSi for the proposed spintronics applications with skyrmions as information carriers, as discussed in the introduction. Because of this achievement, the third part of the thesis on the magnetic properties of the MnSi thin films is not only concerned with the principal behavior, but also with the difference between twinned and twin suppressed layers. Magnetometry measurements are used to demonstrate, that the MnSi layers behave principally as expected from the literature. The analysis of saturation and residual magnetization hints to the twin suppression on Si\((321)\) and Si\((531)\) substrates and further investigations with more samples can complete this picture. For comparable layers on Si\((111)\), Si\((321)\) and Si\((531)\) the Curie-Weiss temperature is identical within 1 K and the critical field within 0.1 T. Temperature dependent magnetoresistivity measurements also demonstrate the expected \(T^2\) behavior not only on Si\((111)\) but also on Si\((321)\) substrates. This demonstrates the successful growth of MnSi on Si\((321)\) and Si\((531)\) substrates. The latter measurements also reveal a residual resistivity of less then half for MnSi on Si\((321)\) in comparison to Si\((111)\). This can be explained with the reduced number of domain boundaries demonstrating the successful suppression of one of the twin domains. The homogeneity of the residual resistivity as well as the charge carrier density over a wide area of the Si\((111)\) wafer is also demonstrated with these measurements as well as Hall effect measurements. The fourth part shows the AMR and PHE of MnSi depending on the angle between in plane current and magnetic field direction with respect to the crystal direction. This was proposed as a tool to identify skyrmions [YKT+15]. The influence of the higher C\(_{3\mathrm{v}}\) symmetry of the twinned system instead of the C\(_3\) symmetry of a B20 single crystal is demonstrated. The difference could serve as a useful additional tool to prove the twin suppression on the chiral substrates. But this is only possible for rotations with specific symmetry surfaces and not for the studied unsymmetrical Si\((321)\) surface. Measurements for MnSi layers on Si\((111)\) above the critical magnetic field demonstrate the attenuation of AMR and PHE parameters for increasing resistivity, as expected from literature [WC67]. Even if a direct comparison to the parameters on Si\((321)\) is not possible, the higher values of the parameters on Si\((321)\) can be explained considering the reduced charge carrier scattering from domain boundaries. Below the critical magnetic field, which would be the region where a skyrmion lattice could be expected, magnetic hysteresis complicates the analysis. Only one phase transition at the critical magnetic field can be clearly observed, which leaves the existence of a skyrmion lattice in thin epitaxial MnSi layers open. The best method to solve this question seems to be a more direct approach in the form of Lorentz-TEM, which was also successfully used to visualize the skyrmion lattice for thin plates of bulk MnSi [TYY+12]. For the detection of in plane skyrmions, lamellas would have to be prepared for a side view, which seems in principle possible. The demonstrated successful twin suppression for MnSi on Si\((321)\) and Si\((531)\) substrates may also be applied to other material systems. Suppressing the twinning in FeGe on Si\((111)\) would lead to a single chirality skyrmion lattice near room temperature [HC12]. This could bring the application of skyrmions as information carriers in spintronics within reach. Glossary: MBE Molecular Beam Epitaxy XRD X-Ray Diffraction HMS Higher Manganese Silicide FWHM Full Width Half Maximum TEM Tunneling Electron Microscopy AMR Anisotropic MagnetoResistance PHE Planar Hall Effect Bibliography: [IEM+85] M. Ishida, Y. Endoh, S. Mitsuda, Y. Ishikawa, and M. Tanaka. Crystal Chirality and Helicity of the Helical Spin Density Wave in MnSi. II. Polarized Neutron Diffraction. Journal of the Physical Society of Japan, 54(8):2975, 1985. [DBS+18] B. Das, B. Balasubramanian, R. Skomski, P. Mukherjee, S. R. Valloppilly, G. C. Hadjipanayis, and D. J. Sellmyer. Effect of size confinement on skyrmionic properties of MnSi nanomagnets. Nanoscale, 10(20):9504, 2018. [YKT+15] T. Yokouchi, N. Kanazawa, A. Tsukazaki, Y. Kozuka, A. Kikkawa, Y. Taguchi, M. Kawasaki, M. Ichikawa, F. Kagawa, and Y. Tokura. Formation of In-plane Skyrmions in Epitaxial MnSi Thin Films as Revealed by Planar Hall Effect. Journal of the Physical Society of Japan, 84(10):104708, 2015. [WC67] R. H. Walden and R. F. Cotellessa. Magnetoresistance of Nickel-Copper Single-Crystal Thin Films. Journal of Applied Physics, 38(3):1335, 1967. [TYY+12] A. Tonomura, X. Yu, K. Yanagisawa, T. Matsuda, Y. Onose, N. Kanazawa, H. S. Park, and Y. Tokura. Real-Space Observation of Skyrmion Lattice in Helimagnet MnSi Thin Samples. Nano Letters, 12(3):1673, 2012. [HC12] S. X. Huang and C. L. Chien. Extended Skyrmion Phase in Epitaxial FeGe(111) Thin Films. Physical Review Letters, 108(26):267201, 2012.}, subject = {Molekularstrahlepitaxie}, language = {en} }