CrI3 revisited with a many-body ab initio theoretical approach

Tom Ichibha, Oak Ridge National Laboratory
Allison L. Dzubak, Oak Ridge National Laboratory
Jaron T. Krogel, Oak Ridge National Laboratory
Valentino R. Cooper, Oak Ridge National Laboratory
Fernando A. Reboredo, Oak Ridge National Laboratory


CrI3 has recently been shown to exhibit low-dimensional, long-range magnetic ordering from few layers to single layers of CrI3. The properties of CrI3 bulk and few-layered systems are uniquely defined by a combination of short-range intralayer and long-range interlayer interactions, including strong correlations, exchange, and spin-orbit coupling. Unfortunately, both the long-range van der Waals interactions, which are driven by dynamic, many-body electronic correlations, and the competing strong intralayer correlations, present a formidable challenge for the local or semilocal mean-field approximations employed in workhorse electronic structure approaches like density-functional theory. In this paper we employ a sophisticated many-body approach that can simultaneously describe long- and short-range correlations. We establish that the fixed-node diffusion Monte Carlo (FNDMC) method reproduces the experimental interlayer separation distance of bulk CrI3 for the high-temperature monoclinic phase with a reliable prediction of the interlayer binding energy. We subsequently employed the FNDMC results to benchmark the accuracy of several density-functional theory exchange-correlation approximations.