GW calculations on La3Ta0.5Ga5.5O14 with oxygen vacancies at non-equivalent sites

Langatate (La3Ta0.5Ga5.5O14, LTG) has been widely used in piezoelectric sensors in high temperature applications because of its structural and piezoelectric reliability at high temperature. However, in the low oxygen partial pressure and elevated temperature ranging from 300 to 700 °C, an increase of electrical conductivity originated from intrinsic oxygen vacancies have been observed in a previous experimental result. In this study, to elucidate the oxygen vacancies effects on LTG, formation energy of each electronic state of oxygen vacancies (VO, VO and VO×) at non-equivalent Wyckoff positions (2d and 6g) and their electronic structures were calculated by combining GW quasi-particle scheme and conventional density functional theory (DFT). The formation energy of VO(6g) was lower than the formation energy of VO(2d) in each electronic state. Thus, relatively stable oxygen vacancies at 6g sites (VO(6g)) can be major oxygen vacancies in LTG system. Also, calculated band gaps of LTG with thermodynamically stable defects such as VO(6g) or VO(6g)× were higher than band gaps of LTG with VO(2d) or VO(2d)× at Γ-point. By the band interpolation based on Boltzmann transport theory, calculated electrical conductivities per unit relaxation time (σ/τ  ) of the LTG with VO(2d) and VO(6g) were similar at the same electron energy, however, σ/τ   of the LTG with VO(2d)× was higher than that of the LTG with VO(6g)×.

► Theoretical calculations of two oxygen vacancies at 2d and 6g sites in langatate.
► We performed quasi-particle GW and Boltzmann transport calculations.
► The formation energy of oxygen vacancy at 6g site was lower than 2d   site.
► The electrical conductivity of two different VO were similar.
► The conductivity of LTG with VO(2d)× was higher than that of LTG with VO(6g)×.