A pathway towards high throughput Quantum Monte Carlo simulations for alloys: A case study of two-dimensional (2D) $GaS_xSe_{1-x}$

TL;DR

This paper introduces a high-throughput workflow using variational and diffusion Monte Carlo methods for alloy simulations, demonstrated on 2D GaS_xSe_{1-x}, with a novel Jastrow sharing technique that reduces computational costs.

Contribution

It proposes a new high-throughput approach combining VMC and DMC with Jastrow sharing to efficiently simulate alloy energy hulls, improving accuracy over traditional DFT methods.

Findings

Jastrow sharing reduces computational cost by 75%.

Workflow successfully applied to 2D GaS_xSe_{1-x} alloys.

Demonstrates feasibility of chemically accurate high-throughput alloy simulations.

Abstract

The study of alloys using computational methods has been a difficult task due to the usually unknown stoichiometry and local atomic ordering of the different structures experimentally. In order to combat this, first-principles methods have been coupled with statistical methods such as the Cluster Expansion formalism in order to construct the energy hull diagram, which helps to determine if an alloyed structure can exist in nature. Traditionally, density functional theory (DFT) has been used in such workflows. In this work we propose to use chemically accurate many-body variational Monte Carlo (VMC) and diffusion Monte Carlo (DMC) methods to construct the energy hull diagram of an alloy system, due to the fact that such methods have a weaker dependence on the starting wavefunction and density functional, scale similarly to DFT with the number of electrons, and have had demonstrated success for a variety of materials. To carry out these simulations in a high-throughput manner, we propose a method called Jastrow sharing, which involves recycling the optimized Jastrow parameters between alloys with different stoichiometries. We show that this eliminates the need for extra VMC Jastrow optimization calculations and results in a significant computational cost savings (on average 1/4 savings of total computational time). Since it is a novel post-transition metal chalcogenide alloy series that has been synthesized in its few-layer form, we used monolayer $GaS_xSe_{1-x}$ as a case study for our workflow. By extensively testing our Jastrow sharing procedure for monolayer $GaS_xSe_{1-x}$ and quantifying the cost savings, we demonstrate how a pathway towards chemically accurate high-throughput simulations of alloys can be achieved using many-body VMC and DMC methods.