Heisenberg and Dzyaloshinskii-Moriya interactions controlled by molecular packing in trinuclear organometallic clusters

This is the authors' abstract. We don't add key points for this paper.

Motivated by recent synthetic and theoretical progress we consider magnetism in crystals of multinuclear organometallic complexes. We calculate the Heisenberg symmetric exchange and the Dzyaloshinskii-Moriya antisymmetric exchange. We show how, in the absence of spin-orbit coupling, the interplay of electronic correlations and quantum interference leads to a quasi-one-dimensional effective spin model in a typical trinuclear complex, Mo₃S₇(dmit)₃, despite its underlying three-dimensional band structure. We show that both intra- and intermolecular spin-orbit coupling can cause an effective Dzyaloshinskii-Moriya interaction. Furthermore, we show that even for an isolated pair of molecules the relative orientation of the molecules controls the nature of the Dzyaloshinskii-Moriya coupling. We show that interference effects also play a crucial role in determining the Dzyaloshinskii-Moriya interaction. Thus, we argue that multinuclear organometallic complexes represent an ideal platform to investigate the effects of Dzyaloshinskii-Moriya interactions on quantum magnets.