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In this study, we examine the electronic and magnetic structure of CrPS₄, a 2D magnetic semiconductor, by employing the SCAN meta-GGA density functional yielding magnetic moments and band gaps in excellent agreement with experiment across 2D and correlated material classes. We find that the magnetic configurations considered, thus far, predict the experimentally observed A-type antiferromagnetic (A-AFM) ordered ground state, with a magnetic moment of 2.77??B per chromium atom. To gain insight into the evolution of the ground state with thickness, the total energy of each magnetic configuration is calculated for a variety of thicknesses, where a monolayer of CrPS₄ is predicted to be a ferromagnetic (FM) insulator with a band gap of 1.379 eV, A-AFM bilayer with 1.367 eV band gap, and A-AFM trilayer with a 1.341 eV band gap. Using the theoretically determined classical energy for each magnetic configuration, we compare the total energies from DFT and estimate the exchange interactions as a function of thickness.

 

LA-UR-21-29890

 

This work was supported by the U.S. DOE NNSA under Cont. No. 89233218CNA000001 through the LANL LDRD Prog. and the CINT, a DOE BES user facility