First-Principles Investigation into the Antiferromagnetic Characteristics and Electronic Structures of the Novel Two-Dimensional CrAl\(_2\)S\(_3\)Cl\(_3\)

Abstract

Two-dimensional materials with intrinsic magnetic properties are expected to be crucial for future spintronic devices and magnetic memory devices, which are easy to exfoliate and maintain magnetic properties for extended periods, spanning from several layers down to single-molecule layers. In this work, the electronic structures and magnetic properties of two-dimensional CrAl\(_2\)S\(_3\)Cl\(_3\) were studied by first-principles calculations using the density functional theory within the generalized gradient approximation with non-collinear magnetic structure calculations. Calculated results indicate that CrAl\(_2\)S\(_3\)Cl\(_3\) exhibits Néel antiferromagnetic behavior, with an indirect bandgap of 1.21 eV, demonstrating an excellent structural stability. The Néel antiferromagnetic behavior originates from direct exchange interactions generated by the d electrons of Cr. The phase transition temperature of CrAl\(_2\)S\(_3\)Cl\(_3\) is around 58.5 K estimated by Monte Carlo simulations within Heisenberg model. Our investigation demonstrates that two-dimensional CrAl\(_2\)S\(_3\)Cl\(_3\) may be a promising candidate in the field of optoelectronics and provides theoretical guidance for exploring two-dimensional semiconductors.