摘要:Two-dimensional (2D) layered GaSe films were grown on GaAs (001), GaN/Sapphire, and Mica substrates by molecular beam epitaxy (MBE). The in situ reflective high-energy electron diffraction monitoring reveals randomly in-plane orientations of nucleated GaSe layers grown on hexagonal GaN/Sapphire and Mica substrates, whereas single-orientation GaSe domain is predominant in the GaSe/GaAs (001) sample. Strong red-shifts in the frequency of in-plane $${E}_{2g}^,$$ vibration modes and bound exciton emissions observed from Raman scattering and photoluminescence spectra in all samples are attributed to the unintentionally biaxial in-plane tensile strains, induced by the dissimilarity of symmetrical surface structure between the 2D-GaSe layers and the substrates during the epitaxial growth. The results in this study provide an important understanding of the MBE-growth process of 2D-GaSe on 2D/3D hybrid-heterostructures and pave the way in strain engineering and optical manipulation of 2D layered GaSe materials for novel optoelectronic integrated technologies.