Two-dimensional ferroelectric MoS₂/Ga₂O₃ heterogeneous bilayers with highly tunable photocatalytic and electrical...

Two-dimensional van der Waals heterostructures with strong intrinsic ferroelectrics are highly promising for novel devices with designed electronic properties. The polarization reversal transition of the 2D ferroelectric Ga₂O₃ monolayer offers a new approach to tune the photocatalytic and electrical properties of MoS₂/Ga₂O₃ heterogeneous bilayers. In this work, we study MoS₂/Ga₂O₃ heterogeneous bilayers with different intrinsic polarization using hybrid-functional calculations. We closely investigate the structural, electronic and optical properties of two stable stacking configurations with opposite polarization. The results reveal a distinct switch from type-I to type-II heterostructures owing to polarization reversal transition of the 2D ferroelectric Ga₂O₃ monolayer. Biaxial strain engineering leads to type-I-to-II and type-II-to-III transitions in the two polarized models, respectively. Intriguingly, one of the MoS₂/Ga₂O₃ heterolayers has a larger spatial separation of the valence and conduction band edges and excellent optical absorption ranging from infrared to ultraviolet region under biaxial strain, thus ensuring promising novel applications such as flexible electrical and optical devices. Based on the highly tunable physical properties of the bilayer heterostructures, we further explore their potential applications, such as photocatalytic water splitting and field-controlled switch channel in MOSFET devices.