A Quantum Monte Carlo study of the structural, energetic, and magnetic properties of two-dimensional (2D) H and T phase VSe₂

Abstract

Previous works have controversially claimed near-room temperature ferromagnetism in two-dimensional (2D) VSe₂, with conflicting results throughout the literature. These discrepancies in magnetic properties between both phases (T and H phase) of 2D VSe₂ are most likely due to the structural parameters being coupled to the magnetic properties. Specifically, both phases have a close lattice match and similar total energies, which makes it difficult to determine which phase is being observed experimentally. In this study, we used a combination of density functional theory (DFT), highly accurate diffusion Monte Carlo (DMC) and a surrogate Hessian line-search optimization technique to resolve the previously reported discrepancy in structural parameters and relative phase stability. With DMC accuracy, we determined the freestanding geometry of both phases and constructed a phase diagram. Our findings demonstrate the successes of the DMC method coupled with the surrogate Hessian structural optimization technique when applied to a 2D magnetic system.