Quasi-Van der Waals Epitaxial Growth of γ′-GaSe Nanometer-Thick Films on GaAs(111)B Substrates
Mingyu Yu, Sahani Amaya Iddawela, Jiayang Wang, Maria Hilse, Jessica L. Thompson, Danielle Reifsnyder Hickey, Susan B. Sinnott, Stephanie Law
Abstract
GaSe is an important member of the post-transition-metal chalcogenide family and is an emerging two-dimensional (2D) semiconductor material. Because it is a van der Waals material, it can be fabricated into atomic-scale ultrathin films, making it suitable for the preparation of compact, heterostructure devices. In addition, GaSe possesses unusual optical and electronic properties, such as a shift from an indirect-bandgap single-layer film to a direct-bandgap bulk material, rare intrinsic p-type conduction, and nonlinear optical behaviors. These properties make GaSe an appealing candidate for the fabrication of field-effect transistors, photodetectors, and photovoltaics. However, the wafer-scale production of pure GaSe single-crystal thin films remains challenging. This study develops an approach for the direct growth of nanometer-thick GaSe films on GaAs substrates by using molecular beam epitaxy. It yields smooth thin GaSe films with a rare γ'-polymorph. We analyze the formation mechanism of γ'-GaSe using density-functional theory and speculate that it is stabilized by Ga vacancies since the formation enthalpy of γ'-GaSe tends to become lower than that of other polymorphs when the Ga vacancy concentration increases. Finally, we investigate the growth conditions of GaSe, providing valuable insights for exploring 2D/three-dimensional (3D) quasi-van der Waals epitaxial growth.