Zigzag Antiferromagnetic Property of Two-Dimensional Nipx3 (X=S/Se) in Pristine Structure and Janus Phase

Abstract

Transition metal phosphorous trichalcogenides TMPX3 (TM = Transition Metal, X = S and Se), with a variety of spin configuration, serve as an excellent platform for studying magnetic properties in two-dimensional system. As an antiferromagnetic semiconductor,  the coexistence of ferromagnetic and antiferromagnetic couplings between the nearest neighboring metal ions of NiPX3 remains a debatable topic. In this work, the electronic structures and magnetic properties of NiPX3 system in pristine structure and Janus phase were systemically investigated by means of first-principles calculations. It is found that NiPX3 system is an indirect band gap semiconductor in its zigzag antiferromagnetic ground state, with a sizable N´eel temperature estimated by Monte Carlo simulations. Electronic structures and crystal orbital Hamilton populations analyses reveal that the zigzag antiferromagnetic ordering is primarily driven by superexchange interactions through p − d hybridization, the coexistence of ferromagnetic and antiferromagnetic couplings is facilitated by a combination of antibonding and bonding states below the Fermi level. This work provides a new approach to explore the diverse and intriguing magnetic properties in two-dimensional materials.

Keywords: Transition metal phosphorous trichalcogenides, zigzag antiferromagnetic property, electronic structures, First-principles study.