Multiple magnetic states of CoPc molecule on a two-dimensional layer of NbSe2

Abstract

Abstract Molecular spintronics hinges on the detailed understanding of electronic and magnetic properties of molecules interfaced with various materials. Here we demonstrate with ab initio simulations that the prototypical Co-phthalocyanine (CoPc) molecule can surprisingly develop multi-spin states once deposited on the two-dimensional 2H–NbSe2 layer. Conventional calculations based on density functional theory (DFT) show the existence of low, regular and high spin states, which reduce to regular and high spins states once correlations are incorporated with a DFT + U approach. Depending on U, the ground state is either the low spin or high spin state with energy differences affected by the molecular orientation on top of the substrate. Our results are compared to recent scanning probe measurements and motivate further theoretical and experimental studies on the unveiled rich multi-magnetic behavior of CoPc molecule.