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Multislice HAADF - STEM image simulations of SrTiO 3 are performed at 300 K.The procedure of these simulations and the used techniques are briefly ex-plained and reasoned. The results are presented and discussed in a conciseway and in an attached paper a comparison to experimental images is made.The paper proofs that the electron optical setup developed in Dresden is indeed capable of producing atomic-sized EVBs, a precondition for measuring EMCD with atomic resolution.

Physics and potential applications of femtosecond laser pulses interacting with matter have captured interest in various fields, such as nonlinear optics, laser micromachining, integrated optics, and solar cell technologies. On the one hand, such ultrashort intense pulses make them practical elegant tools to be utilized for direct structuring of materials with high accuracy and numerous potential applications. On the other hand, studying the fundamental aspects and nonlinear nature of such interactions opens new remarkable venues for various unique investigations. In recent years, the emerging topic of structured light (also known as twisted or optical vortex light), i.e., a beam of light with a twisted wave-front that can carry orbital angular momentum (OAM), has attracted the attention of many researchers working in the field of light-matter interaction. Such beams offer various applications from classical and quantum communication to imaging, micro/nano-manipulation, and modification of fundamental processes involved in light-matter interactions, e.g., absorption and emission. Nevertheless, the fabrication of complex structures, controlled modification, and achieving a high spatial resolution in material processing still remain in the spotlight. Moreover, the fundamental role of orbital angular momentum in the nonlinear absorption of materials, particularly in solids, has yet remained a subject of debate. Addressing these points was the main motive behind this dissertation. To accomplish this objective and investigate new aspects of structured light-matter interaction, I conducted various experiments, the results of which are presented in this work. The general idea was to study the interaction of femtosecond laser radiation, having a structured phase and polarization, with the matter in two aspects: (i) surface morphology modification and (ii) nonlinear absorption of solids. In this regard, I studied surface processing of crystalline silicon and CVD diamond with femtosecond laser vortex pulses generated by a birefringent phase-plate, known as q-plate, in single and multiple pulse irradiation regimes, respectively. The characterization of the modified region was performed using optical microscopy, scanning electron microscopy (SEM), and atomic force microscopy (AFM). I demonstrated that upon irradiation of a single vortex pulse on silicon, a nano-cone structure is formed within the ablated crater, whose height was independent of the helicity of the twisted light. However, for a linearly polarized vortex pulse, the height of the nano-cone decreases at higher pulse energies. The dynamics of nano-cone formation and the role of polarization were also investigated by simulating the mass transport function in this process. Moreover, using superimposed vortex beams, we fabricated complex patterns containing several nano-cones, by single-shot irradiation on the silicon surface. My experimental results offer an ability to actively control and manipulate material, in terms of the nanocones position, in two dimensions with an ultra-high resolution. I further proceeded with our experiments in the multiple pulse regime on a diamond target. By irradiation of a high number of superimposed vortex pulses, I was able to imprint complex polarization states of structured light on the target surface in the form of periodic nano-ripples. This procedure enabled us to not only generate spatially varying nano-gratings but also directly visualize and study very complex states of polarization. Besides these surface structuring, I carried out experimental studies to investigate the response of bulk material to an incident circularly polarized vortex beam that carries orbital angular momentum. The experimental results reveal, for the first time, that such an interaction can produce a differential absorption that gives rise to helical dichroism. We demonstrate that this response is sensitive to the handedness and degree of the twist in the incident vortex beam. Such a dichroism effect may be attributed to the excitation of dipole-forbidden atomic transitions, e.g., electric quadrupole transitions. However, this explanation is not absolute and remains open to further research and investigations.

The vectorial nature (polarization) of light plays a significant role in light-matter interaction that leads to a variety of optical devices. The polarization property of light has been exploited in imaging, metrology, data storage, optical communication and also extended to biological studies. Most of the past studies fully explored and dealt with the conventional polarization state of light that has spatially symmetric electrical field geometry such as linear and circular polarization. Recently, researchers have been attracted to light whose electric field vector varies in space, the so-called optical vector vortex beam (VVB). Such light is expected to further enhance and improve the efficiency of optical systems. For instance, a radially polarized light under focusing condition is capable of a tighter focus more than the general optical beams with a uniform polarization structure, which improves the resolution of the imaging system [1]. Interaction of ultrafast laser pulses with matter leads to numerous applications in material processing and biology for imaging and generation of microfluidic systems. A femtosecond pulse, with very high intensities of (10^{12} - 10^{13} W/cm^2), has the potential to trigger a phenomenon of optical breakdown at the surface and therefore induce permanent material modification. With such high intensities and taking into account the fact that most materials possess large bandgap, the interaction is completely nonlinear in nature, and the target material can be modified locally upon the surface and even further in bulk. The phenomenon of optical breakdown can be further investigated by studying the nonlinear absorption. Properties like very short pulse duration and the high irradiance of ultrashort laser pulse lead to more precise results during the laser ablation process over the long pulsed laser. The duration of femtosecond laser pulse provides a high resolution for material processing because of the significant low heat-affected zone (HAZ) beyond the desired interaction spot generated upon irradiating the material. Under certain condition, the interaction of intense ultrashort light pulses with the material gives rise to the generation of periodic surface structures with a sub-micron periodicity, i.e., much smaller than the laser wavelength. The self-oriented periodic surface structures generated by irradiating the material with multiple femtosecond laser pulses results in improving the functionality of the material's surface such as controlling wettability, improving thin film adhesion, and minimizing friction losses in automobile engines, consequently, influences positively on many implementations. In this work, we introduced a new method to study complex polarization states of light by imprinting them on a solid surface in the form of periodic nano-structures. Micro/Nanostructuring of diamond by ultrafast pulses is of extreme importance because of its potential applications in photonics and other related fields. We investigated periodic surface structures usually known as laser-induced periodic surface structures (LIPSS) formed by Gaussian beam as well as with structured light carrying orbital angular momentum (OAM), generated by a birefringent optical device called a q-plate (QP). We generated conventional nano-structures on diamond surface using linearly and circularly polarized Gaussian lights at different number of pulses and variable pulse energies. In addition, imprinting the complex polarization state of different orders of optical vector vortex beams on a solid surface was fulfilled in the form of periodic structures oriented parallel to the local electric field of optical light. We also produced a variety of unconventional surface structures by superimposing a Gaussian beam with a vector vortex beam or by superposition of different order vector vortex beams. This thesis is divided into five chapters, giving a brief description about laser-matter interaction, underlying the unique characterization of femtosecond laser over the longer pulse laser and mechanisms of material ablation under the irradiation of fs laser pulse. This chapter also presents some earlier studies reported in formation of (LIPSS) fabricated on diamond with Gaussian. The second chapter explains the properties of twisted light possessing orbital angular momentum in its wavefront, a few techniques used for OAM generation including a full explanation of the q-plate from the fabrication to the function of the q-plate, and the tool utilized to represent the polarization state of light (SoP), a Poincar'e sphere. Finally, the experimental details and results are discussed in the third and fourth chapters, respectively, following with a conclusion chapter that briefly summarizes the thesis and some potential application of our findings.

In this thesis, two selected topics in magnetism are studied using theoretical modelling and computational methods. The first of these is the magnetocrystalline anisotropy energy (MAE) of transition metal based magnets. In particular, ways of finding 3d transition metal based materials with large MAE are considered. This is motivated by the need for new permanent magnet materials, not containing rare-earth elements, but is also of interest for other technological applications, where the MAE is a key quantity. The mechanisms of the MAE in the relevant materials are reviewed and approaches to increasing this quantity are discussed. Computational methods, largely based on density functional theory (DFT), are applied to guide the search for relevant materials. The computational work suggests that the MAE of Fe1-xCox alloys can be significantly enhanced by introducing a tetragonality with interstitial B or C impurities. This is also experimentally corroborated. Alloying is considered as a method of tuning the electronic structure around the Fermi energy and thus also the MAE, for example in the tetragonal compound (Fe1-xCox)2B. Additionally, it is shown that small amounts (2.5-5 at.%) of various 5d dopants on the Fe/Co-site can enhance the MAE of this material with as much as 70%. The magnetic properties of several technologically interesting, chemically ordered, L10 structured binary compounds, tetragonal Fe5Si1-xPxB2 and Hexagonal Laves phase Fe2Ta1-xWx are also investigated. The second topic studied is that of magnetic effects on the elastic scattering of fast electrons, in the context of transmission electron microscopy (TEM). A multislice solution is implemented for a paraxial version of the Pauli equation. Simulations require the magnetic fields in the sample as input. A realistic description of magnetism in a solid, for this purpose, is derived in a scheme starting from a DFT calculation of the spin density or density matrix. Calculations are performed for electron vortex beams passing through magnetic solids and a magnetic signal, defined as a difference in intensity for opposite orbital angular momentum beams, integrated over a disk in the diffraction plane, is observed. For nanometer sized electron vortex beams carrying orbital angular momentum of a few tens of ħ, a relative magnetic signal of order 10-3 is found. This is considered realistic to be observed in experiments. In addition to electron vortex beams, spin polarised and phase aberrated electron beams are considered and also for these a magnetic signal, albeit weaker than that of the vortex beams, can be obtained. / <p>Felaktigt ISBN i den tryckta versionen: 9789155497149</p><p></p>