Modulating the mechanical properties and valence band of LiGaO2 by forming the highly mismatched Li(Ga1−xBix)O2 alloys

β-LiGaO2 with a wurtzite-like crystal structure is a direct ultra-wide bandgap semiconductor. Similar to many wide bandgap oxides, the valence band of LiGaO2 is predominantly composed of O-2p orbital, leading to a low valence band position, drastically limiting its applications. In this work, we employ first-principles calculations to demonstrate that adding a small amount of Bi into LiGaO2 to form the highly mismatched Li(Ga1−xBix)O2 alloys can dramatically modulate the valence band compositions. Compared to LiGaO2, the valence band maximum of the alloys is significantly elevated, and a fully occupied intermediate valence band appears, further raising the valence band positions. Despite the appearance of intermediate valence bands that significantly reduce the alloys’ bandgap, the bandgap remains over 3.10 eV, ensuring visible light transparency. With increasing Bi composition in the alloys, the bulk modulus increases while the shear modulus gradually decreases, which improves the ductility. Moreover, the compliant elastic constants of the alloys indicate mechanical stability. These findings suggest that Li(Ga1−xBix)O2 alloys are promising flexible transparent conductive oxides, offering valuable insights for future applications.