Electronic and optical properties of oxygen vacancies in amorphous TaO from first principles.

Oxygen vacancies are important defects considered to play a central role in the electronic and optical properties of tantalum pentoxide (TaO) films and devices. Despite extensive experimental studies on oxygen vacancies in TaO, the reported defect states are ambiguously identified due to the absence of accurate and conclusive theoretical evidence. Here we investigate the thermodynamic, electronic, and optical properties of oxygen vacancies in amorphous TaO by first-principles calculations based on hybrid-functional density functional theory (DFT). The calculated thermodynamic and optical transition levels are in good agreement with a broad range of diverse measured properties with various experimental methods, providing conclusive evidence for the identification of the defect states observed in experiments as originating from oxygen vacancies. Our calculations also predict the formation of spin-polarized polarons. Our results elucidate the fundamental atomistic properties of oxygen vacancies in various oxidation states as a function of growth conditions and provide guidance to control the properties of TaO films/devices.