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The magnetic properties of inorganic complexes are closely related to their molecular structures. This holds true for small dimeric systems and for large single-molecule magnets. My project aims to improve our understanding of these correlations by combining structural (X-ray) and magnetic characterization techniques with High-Frequency Electron Paramagnetic Resonance (HFEPR), all under pressure. In particular focussing on magnetically interesting Cu,Mn, Ni, Fe monomers, dimers and single-molecule magnets.