Systematic DFT+U and Quantum Monte Carlo benchmark of magnetic two-dimensional (2D) CrX$_3$ (X = I, Br, Cl, F)

TL;DR

This paper develops a combined DFT+U and Quantum Monte Carlo workflow to accurately predict magnetic properties and critical temperatures of 2D CrX3 materials, improving understanding of their electron correlations.

Contribution

It introduces a novel workflow integrating DFT+U and DMC methods to study 2D magnetic systems, providing more reliable estimates of critical temperatures.

Findings

Estimated T_c of 43.56 K for CrI3

Estimated T_c of 20.78 K for CrBr3

Analyzed spin densities and magnetic properties with DMC and DFT+U

Abstract

The search for two-dimensional (2D) magnetic materials has attracted a great deal of attention because of the experimental synthesis of 2D CrI$_3$, which has a measured Curie temperature of 45 K. Often times, these monolayers have a higher degree of electron correlation and require more sophisticated methods beyond density functional theory (DFT). Diffusion Monte Carlo (DMC) is a correlated electronic structure method that has been demonstrated successful for calculating the electronic and magnetic properties of a wide variety of 2D and bulk systems, since it has a weaker dependence on the Hubbard parameter (U) and density functional. In this study we designed a workflow that combines DFT+U and DMC in order to treat 2D correlated magnetic systems. We chose monolayer CrX$_3$ (X = I, Br, Cl, F), with a stronger focus on CrI$_3$ and CrBr$_3$, as a case study due to the fact that they have been experimentally realized and have a finite critical temperature. With this DFT+U and DMC workflow and the analytical method of Torelli and Olsen, we estimated an upper bound of 43.56 K for the T$_c$ of CrI$_3$ and 20.78 K for the T$_c$ of CrBr$_3$, in addition to analyzing the spin densities and magnetic properties with DMC and DFT+U. We expect that running this workflow for a well-known material class will aid in the future discovery and characterization of lesser known and more complex correlated 2D magnetic materials.