Dzyaloshinskii-Moriya interactions, Néel skyrmions and V$_4$ magnetic clusters in multiferroic lacunar spinel GaV$_4$S$_8$

Abstract: Using ab initio density functional theory with static mean-field correlations, we calculate the Heisenberg and Dzyaloshinskii-Moriya interactions (DMI) for an atomistic spin Hamiltonian for the lacunar spinel, GaV$4$S$_8$. The parameters describing these interactions are used in atomistic spin dynamics and micromagnetic simulations. The magnetic properties of the lacunar spinel GaV$_4$S$_8$, a material well-known from experiment to host magnetic skyrmions of N\'eel character, are simulated with these ab initio calculated parameters. The Dzyaloshinskii-Moriya contribution to the micromagnetic energy is a sum of two Lifshitz invariants, supporting the formation of N\'eel skyrmions and its symmetry agrees with what is usually expected for $C{3\nu}$-symmetric systems. The are several conclusions one may draw from this work. One concerns the quantum nature of the magnetism, where we show that the precise magnetic state of the V$_4$ cluster is crucial for understanding quantitatively the magnetic phase diagram. In particular we demonstrate that a distributed-moment state of each V$_4$ cluster explains well a variety of properties of GaV$_4$S$_8$, such as the band gap, observed Curie temperature and especially the stability of N\'eel skyrmions in the experimentally relevant temperature and magnetic-field range. In addition, we find that electronic correlations change visibly the calculated value of the DMI.