Magnetic measures of purity for MnBi$_2$Te$_4$ (2204.04268v1)

Abstract: The intrinsically anti-ferromagnetic topological insulator, MnBi$2$Te$_4$ (MBT), has garnered significant attention recently. The excitement for this layered van der Waals bonded compound stems from its potential to host numerous exotic topological quantum states. For instance, quantum anomalous Hall states are predicted for odd-layer compounds and axion insulator states for the even-layer compounds. Unfortunately, the realization of these phenomena has been hindered by experimental challenges such as the existence of negative charge carriers, i.e., electron doping, which have been linked to anti-site defects among the Mn and Bi sub-lattices. Based on high level diffusion Monte Carlo (DMC) and DMC-tuned DFT+U calculations, we provide benchmark quality results for the bulk Mn magnetization as well as for Mn${Bi}$ and Bi$_{Mn}$ defects. We use this information to refine and extend models that estimate the anti-site defect concentration in actual MBT samples when combined with data from magnetic susceptibility and intermediate field magnetization measurements. Our models are validated through favorable comparison with prior experimental studies that obtained both magnetic and site occupancy data. We then extend our estimates to a larger set of prior samples to identify a probable zone of low defect density that has yet to be reached in synthesis. We anticipate our theoretically based magnetic purity measures may be used as minimization targets in the cycle of refinement needed to synthesize MBT samples with low anti-site defect concentrations and more reproducible topological properties.