Diffusion Quantum Monte Carlo Benchmarking of Magnetic Moments in MnBi2Te4

Abstract

The intrinsically antiferromagnetic topological insulator, MnBi₂Te₄ (MBT), has garnered significant attention recently due to its potential to host numerous exotic topological quantum states. Unfortunately, their consistent realization has been hindered by intrinsic antisite defects among the Mn and Bi sublattices. In this work, we establish Mn magnetization of pristine MBT through high level diffusion Monte Carlo calculations, which can serve as a precise starting point for various models to estimate antisite defect concentrations in actual MBT samples. The benchmark quality of DMC calculations is further identified from out model estimating antisite defect concentrations, which combines the benchmarked Mn magnetization with data from magnetic susceptibility and intermediate field magnetization measurements. This reproduces well Bi_Mn and Mn_Bi concentrations measured in the experiments. We anticipate these theoretically based magnetic purity measures may be used as minimization targets in cycles of refinement to synthesize MBT with low antisite defect concentrations and more reproducible topological properties.