Reversible Ferroelastic Strain Engineering Enables Stabilization of a Hidden Ga2O3 Polymorph

Abstract

Abstract Understanding the formation, transformation, and stabilization of metastable polymorphs in functional compounds is a central challenge in materials science and has a profound impact on phase engineering and property control. Ga2O3 is an ultrawide bandgap semiconductor whose rich polymorphism underpins diverse electronic and optoelectronic functionalities, motivating continued exploration of its metastable phases. Among the known Ga2O3 polymorphs, the P1̅-phase has been predicted to have the closest energy to the thermodynamically stable β-phase; however, its existence has not been definitively identified experimentally, and feasible preparation routes remain unclear up to now. Here, combining large-scale molecular dynamics simulations with a high-accuracy machine learning potential, we reveal a reversible strain-induced ferroelastic β–P1̅ phase transition in Ga2O3 and further investigate the origin of instability of P1̅-Ga2O3. Our work not only explains the absence of experimental observations of P1̅-Ga2O3 from the perspectives of mechanical stability and crystallization kinetics but also extends the application of strain engineering in phase transitions of wide-bandgap semiconductor single-crystal materials.