Parameter free treatment of a layered correlated van der Waals magnet: CrPS$_{4}$

TL;DR

This study uses a parameter-free density functional approach to accurately analyze the electronic, magnetic, and optical properties of layered CrPS$_{4}$, revealing layer-dependent magnetic states and band gaps consistent with experimental data.

Contribution

It provides a comprehensive, parameter-free theoretical analysis of CrPS$_{4}$'s magnetic and electronic properties across different layer thicknesses, including optical characteristics.

Findings

Bulk CrPS$_{4}$ is A-AFM with a 1.34 eV band gap.

Monolayer CrPS$_{4}$ is a ferromagnetic insulator with a 1.37 eV gap.

Layer-dependent magnetic states and optical properties are characterized.

Abstract

The electronic and magnetic structure of CrPS$_{4}$, a 2D magnetic semiconductor is examined by employing the SCAN meta-GGA density functional. We find the resulting magnetic moment and band gap are in excellent agreement with experiment. From the bulk magnetic configurations, we confirm the experimentally observed A-type antiferromagnetic (A-AFM) ordered ground state with a magnetic moment of 2.78 $\mu_B$ per chromium atom and band gap of 1.34 eV. To gain insight into the evolution of the ground state with layers, the total energy of each magnetic configuration is calculated for a variety of thicknesses. Monolayer CrPS$_{4}$ is predicted to be a ferromagnetic insulator with a band gap of 1.37 eV, and A-AFM for bilayer and trilayer, with band gaps of 1.35 eV and 1.30 eV, respectively. The electronic structure is reported for the single, two, three layer and bulk CrPS$_{4}$. Finally, we explore the optical properties of the 2D structure and report the dielectric tensor components and Kerr parameters for the monolayer.