Magnetic, Structural, and Electronic Properties of CrOCl with the PBE Functional

TL;DR

This study shows that the PBE functional accurately describes the magnetic, structural, and electronic properties of CrOCl, a layered antiferromagnetic insulator, without needing Hubbard corrections, thus providing a reliable ab initio approach.

Contribution

It demonstrates that PBE alone suffices to correctly predict CrOCl's properties, simplifying computational modeling of this material.

Findings

PBE reproduces the antiferromagnetic ground state accurately.

PBE improves structural property predictions.

PBE reliably describes electronic structure.

Abstract

CrOCl is a van der Waals-layered insulator with an antiferromagnetic ground state, making it a promising platform for exfoliation and the exploration of low-dimensional magnetism. An accurate ab initio description is therefore essential. Previous density-functional studies have shown that DFT+$U$ calculations may erroneously favor ferromagnetic order depending on the choice of parametrization, an issue that cannot be remedied by simply adjusting the value of $U$. Here, we demonstrate that an explicit Hubbard correction is unnecessary: the PBE functional correctly reproduces the AFM ground state while simultaneously improving the description of structural properties. Moreover, PBE provides a reliable account of the electronic structure. These findings clarify the role of correlation effects in CrOCl and identify PBE as a robust starting point for future ab initio studies of CrOCl-based materials.