The main goal of this thesis is to pave the way towards a rational design of transition metal oxide nanocrystals with a tailored magnetic response. For that, the work herein presented delves into the intrinsic correlation between magnetic and crystal structure and shows how exerting control on lattice defects and different surface and interface-related phenomena allows a tunability of the magnetic anisotropy. Likewise, this work attempts to benchmark the utilization of Raman spectroscopy as a powerful technique to bridge the gap between a conventional structural characterization and magnetism at the nanoscale, where complex interfaces may emerge due to chemical segregation and cation redistribution effects. Lastly, it is further demonstrated that by customizing the synthetic methodology it is possible to engineer adequate heterostructures that meet the requirements for their application in the fields of magneto-optics and spintronics.
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