Spin model for the Honeycomb $\rm NiPS_3$

Abstract

In the Van der Waal material $\rm NiPS_3$, Ni atoms have spin S=1 and realize a honeycomb lattice. Six sulfur atoms surround each Ni and split their d manifold into three filled and two unfilled bands. Aimed to determine the spin Hamiltonian of $\rm NiPS_3$, we study its exchange mechanisms using a two-band half-filled Hubbard model. Hopping between d orbitals is mediated by p orbitals of sulfur and gives rise to bilinear and biquadratic spin couplings in the limit of strong electronic correlations. The microscopic model exposed a ferromagnetic biquadratic spin interaction $\rm K_1$ allowing the completion of a minimal $\rm J_1-J_3-K_1$ spin Hamiltonian for $\rm NiPS_3$. In bulk, a ferromagnetic first nearest neighbor $\rm J_1$ and a more significant antiferromagnetic third nearest neighbor spin coupling $\rm J_3$ agreed with the literature, while in monolayer $\rm J_1$ is positive and very small in comparison. Using a variational scheme we found that a zig-zag antiferromagnetic order is the ground state of bulk samples. The zig-zag pattern is adjacent to commensurate and incommensurate spin spirals, which could hint at the puzzling results reported in $\rm NiPS_3$ monolayers.