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.