Using Nd instead of La increased structural distortions and, at the same time, hindered exsolution. Increasing the amount of Ca doping also increased distortions and additionally changed the Fe oxidation states, resulting in exsolution being shifted to higher temperatures as well. Using the easily reducible element Co as the B-site dopant significantly facilitated the exsolution process and led to much smaller and homogeneously distributed exsolved particles. Therefore, the Co-doped perovskite is a promising material for applications in catalysis, even more so as Co is catalytically a highly active element. The results show that fine-tuning of the perovskite composition will allow tailored exsolution of nanoparticles, which can be used for highly sophisticated catalyst design.This study uses theoretically methods to investigate, for metal diiodides MI2 (M = Mg, Ca, Mn, Fe, Cd, Pb) with CdI2 (2H polytype) structure, the mutual correlation between the structure-characterizing parameters (the flatness parameter of monolayers f, the Madelung constant A, and bonding angle I-M-I) and correlation of these parameters with contributions of the Coulomb and covalent energies to cohesive energy. The energy contributions to cohesive energy are determined with the use of empirical atomic potentials. It is demonstrated that the parameters f and A, and the bonding angle I-M-I are strictly correlated and increase in the same order FeI2 less then PbI2 less then MnI2 less then CdI2 less then MgI2 less then CaI2. It is found that with an increase of parameter A and bonding angle I-M-I the relative contribution of the Coulomb energy to cohesive energy increases, whereas the relative contribution of the covalent energy decreases. For a hypothetical MX2 layered compound with the CdI2 (2H polytype) structure, composed of regular MX6 octahedra (angle X-M-X = 90°), the flatness parameter and the Madelung constant are found to be freg = 2.449 and Areg = 2.183, respectively. Correlation of the covalent energy with the type of distortion of MI6 octahedra (elongation or compression) with respect to regular configuration (angle I-M-I = 90°) is also analyzed.A previously unknown cocrystal of olanzapine and phenol was identified from a volatile deep eutectic solvent as the intermediate species in the crystallization of olanzapine. This new nanocrystalline phase was investigated by electron diffraction, powder X-ray diffraction and differential scanning calorimetry. LC-2 The structure was determined by simulated annealing using 3D electron diffraction data and confirmed using DFT-D optimizations. Olanzapine and phenol cocrystallize in the triclinic space group P1, supporting the hypothesis of a dimeric growth unit, where a centrosymmetric dimer is stabilized by multiple weak C-H...π interactions and forms double N-H...N hydrogen bonding with adjacent dimers.Multiple-Edge Anomalous Diffraction (MEAD) has been applied to various quaternary sulfosalts belonging to the adamantine compound family in order to validate the distribution of copper, zinc and iron cations in the structure. Semiconductors from this group of materials are promising candidates for photovoltaic applications. Their properties strongly depend on point defects, in particular related to cation order-disorder. However, Cu+, Zn2+ and Fe2+ have very similar scattering factors and are all but indistinguishable in usual X-ray diffraction experiments. Anomalous diffraction utilizes the dependency of the atomic scattering factors f' and f'' of the energy of the radiation, especially close to the element-specific absorption edges. In the MEAD technique, individual Bragg peaks are tracked over an absorption edge. The intensity changes depending on the structure factor can be highly characteristic for Miller indices selected for a specific structural problem, but require very exact measurements. Beamline KMC-2 at synchrotron BESSY II, Berlin, has been recently upgraded for this technique. Anomalous X-ray powder diffraction and XAFS compliment the data. Application of this technique confirmed established cation distribution in Cu2ZnSnSe4 (CZTSe) and Cu2FeSnS4 (CFTS). In contrast to the literature, cation distribution in Cu2ZnSiSe4 (CZSiSe) is shown to adopt a highly ordered wurtz-kesterite structure type.A high-resolution single-crystal X-ray diffraction study of abiraterone acetate (1) has been carried out. The charge density distribution in the crystal of this anticancer drug is reconstructed from experimental data. The nature and the contributions of various intermolecular interactions to the total crystal energy are studied by means of the quantum theory `Atoms-in-Molecules', a non-covalent interactions method and energy framework plots. In general, dispersion C-H...H-C and C-H...π interactions play the main role in crystal packing of 1. The Voronoi tessellation analysis of 1 confirmed that contribution of hydrophobic and hydrophilic interactions to the molecular surface is close to their contribution to the total crystal energy. Similar analysis of abiraterone complexes with the cytochrome P450 family demonstrated that contribution of the C-H...H-C and C-H...π interactions to the molecular surface of the drug remains unchanged to fit the binding pocket, despite the presence of water and heme molecules, and hydrophilic groups within the pocket.Seven new metal-organic frameworks (MOFs), namely, [Zn2(L1)(H2O)3]n (1), [Zn2(L1)(dib)(H2O)2]n (2), [Zn2(L1)(4,4'-bipy)(H2O)2]·H2On (3), [Cd2(L1)(1,10-phen)]n (4), [Ni2(HL1)(4,4'-bipy)(μ3-OH)(μ2-H2O)]n (5), [Co4(L1)(4,4'-bibp)3]·(4,4'-bibp)3n (6), and [Co2(L2)(4,4'-bibp)2(H2O)]n (7), where H4L1 and H4L2 are semi-rigid 3-(3,5-dicarboxylphenoxy)phthalic acid and 4-(3,5-dicarboxylphenoxy)phthalic acid, respectively, and 4,4'-bipy is 4,4'-bipyridine, dib is 1,4-bis(1H-imidazol-1-yl)benzene, 1,10-phen is 1,10-phenanthroline and 4,4'-bipb is 1,4-bis(pyridin-4-yl)benzene, have been prepared under solvothermal conditions with ZnII, CdII, CoII and NiII ions in the presence of auxiliary N-donor ligands. The crystal structures and photoluminescence and magnetic properties of these compounds have been investigated. Compound 1 displays a 3,4,6-connected two-dimensional (2D) topology with a Schläfli symbol of (42.5)2(43.52.7)(45.56.63)2, and the 2D structure was further assembled to form a three-dimensional (3D) framework by intermolecular O-H.