Beyond Janus Atomic Ordering: High-Throughput First-Principles Search for Hidden MoSO Monolayer Structures

Abstract

Despite the growing interest in two-dimensional (2D) MoSO systems, existing studies have exclusively focused on conventional Janus structures. In this work, we perform high-throughput first-principles calculations to explore novel stable 2D MoSO monolayers. Combined with random sampling strategy, graph theory and group theory, we successfully screen out three novel non-Janus 2D MoSO monolayers from 1325 candidate structures, namely Reversed 2H-MoSO, Hybrid 2H-MoSO, and Hybrid 1T'-MoSO. Compared with Janus MoSO monolayers, the non-Janus MoSO counterparts possess lower binding energies, varying from -4.38 to -4.51 eV/atom. A systematic combination of dynamic, thermodynamic, and mechanical stability analyses corroborates their excellent structural robustness. Ab initio molecular dynamics (AIMD) simulations confirm their superior thermal resistance, with the structures remaining stable at temperatures beyond 2000 K. Interestingly, unlike the semiconducting Janus MoSO, the Hybrid 1T'-MoSO monolayer exhibits distinct metallic characteristics. Furthermore, we found that strain and curvature can enable controlled phase transitions of MoSO among semiconducting, semimetallic, and metallic phases. More importantly, the Hybrid 1T'-MoSO exhibits favorable HER activity with a Gibbs free energy of -0.002 eV, rendering it a promising candidate for hydrogen evolution catalysis. This work not only expands the family of 2D MoSO materials but also provides a reliable strategy for discovering stable functional 2D materials via high-throughput computation.