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 N´eel ordered. However, in materials with a greater degree of magnetic frustration, N´eel order can give way to a large-D phaseJ. M. acknowledges financial support from (MAT2015-66128-R) MINECO/FEDER, UE, and A.R. from the French National Research Agency (Contract ORGANISO, ANR-15-CE09- 0017). Work at the University of Queensland was supported by the Australian Research Council (DP160100060