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The field of molecular spintronics has gained much attention since molecules withmagnetic centers form natural magnetic units, which do not suffer from the size limitations of conventional electronics, opening a new path towards miniaturization. To fabricate devices, the molecules have to be deposited on a substrate. The key questions are the interaction of the molecules with the substrate and the control of the magnetic properties. Considering molecule‐substrate hybrid interfaces as building blocks for spintronic devices, a deep understanding of the electronic structure and the coupling mechanisms is central to future applications. The orientation and reconstruction of the substrates can strongly affect the electronic and magnetic characteristics of the adsorbed molecule and drastically change the properties of the free molecules. In this chapter, we will discuss the interaction of transition metal‐centered porphyrins and phthalocyanines with different types of substrates, for example, ferromagnetic transition metals or graphene sheets, in the framework of state‐of‐the‐art density functional theory methods plus insights gained from X‐ray absorption/X‐ray magnetic circular dichroism experiments. The goal is to give an insight into the relevant processes on the atomic scale and to present possible routes to tailor magnetic properties in molecule‐ substrate hybrid structures.

Deposited Transition Metal‐Centered Porphyrin and Phthalocyanine Molecules: Influence of the Substrates on the Magnetic Properties