Tunable Electronic Bandgaps and Optical and Magnetic Properties in Antiferromagnetic MPS3/GaN (M = Mn, Fe, and Ni) Heterobilayers.

Research on two dimensional (2D) antiferromagnetic materials and heterobilayers is gaining prominence in spintronics. This study focuses on MPS3 monolayers and their van der Waals heterobilayers with GaN monolayers. We systematically investigated the structural stability, electronic properties, and magnetic characteristics of MPS3 (M = Mn, Fe, and Ni) monolayers via first-principles calculations, and explored their potential applications in optoelectronics and spintronics. Through phonon spectrum analysis, the dynamic stability of MPS3 monolayers was confirmed, and their bond lengths, charge distributions, and wide-bandgap semiconductor properties were analyzed in detail. In addition, the potential applications of MPS3 monolayers in UV detection were explored. Upon constructing the MPS3/GaN heterobilayer structure, a significant reduction in the bandgap was observed, thereby expanding its potential applications in the visible light spectrum. The intrinsic antiferromagnetic nature of MPS3 monolayers was confirmed through calculations, with the magnetic moments of the magnetic atoms M being 4.560, 3.672, and 1.517, respectively. Moreover, the heterobilayer structures further enhanced the magnetic moments of these elements. The magnetic properties of MPS3 monolayers were further analyzed using spin-orbit coupling (SOC), confirming their magnetic anisotropy. These results provide a theoretical basis for the design of novel two-dimensional spintronic and optoelectronic devices based on MPS3.