Spin molecular-orbit coupling and magnetic properties of the decorated honeycomb layers of Mo3S7(dmit)3 crystals

We explore the magnetic properties of isolated a − b planes of trinuclear organometallic crystals, Mo3S7(dmit)3, in which an interplay of strong electronic correlations and spin molecular-orbital coupling (SMOC) occurs. The magnetic properties can be described by a XXZ+1200, S = 1 Heisenberg model on a honeycomb lattice with single-spin anisotropy, D, which depends strongly on SMOC. Based on ab initio estimates of SMOC in Mo3S7(dmit)3 crystals, we predict that the honeycomb layers of Mo3S7(dmit)3 are Néel ordered. However, in materials with a greater degree of magnetic frustration, Néel order can give way to a large-D phase