Theoretical study of hybrid architectures combining graphene substrate with single-molecule magnets

We explore the fascinating features of unique hybrid structures composed of single-molecule magnets (SMMs) integrated with two-dimensional nanomaterials, such as graphene. These hybrid systems exhibit novel magnetic, electronic, and quantum properties arising from the synergistic interaction between the molecular magnets and the two-dimensional substrate. The combination enhances functionalities like magnetic anisotropy, spin coherence, and charge transport, opening new avenues for applications in quantum computing, spintronics, and advanced nanoelectronics. The fascinating features of the unique hybrid structures made of single molecule magnets (SMMs) and two-dimensional nano-materials (like graphene) have drawn the attention of experimental researchers. Such systems might eventually form a reconfigurable array of magnetic nano-objects and give rise to cutting-edge spin-based technology like spin quantum memory. The stability of these hybrid structures and the kinds of interactions between the localized spin in SMM and the 2D material to which the molecule is grafted are examined in detail theoretically, and results are presented here. Our theoretical investigation is supported by density functional theory based on ab initio computations. We pay close attention to how to properly describe magnetism and van der Waals dispersive forces. In addition, we looked at a few types of SMMs (molecules with tetrahedrally coordinated Fe and Cr bound to two double bis(methanesulfonamido) benzene ligands), and we examined their adsorption to a graphene monolayer. In addition, we address the crucial topic of how structural defects in graphene (such as vacancies, N-dopants, etc.) affect the adhesion and magnetic characteristics of SMMs.

This work provides valuable insights into the design of graphene–SMM hybrid materials, emphasizing the role of molecular coordination and ligand architecture in achieving stable and functional interfaces. The findings pave the way for future exploration of SMM–graphene composites in nanoscale magnetic sensors, data storage, and quantum computing technologies, where the integration of magnetic molecules with two-dimensional materials could offer unprecedented control over spin-dependent phenomena.