Origin of the Bipolar Doping Behavior of SnO from X-ray Spectroscopy and Density Functional Theory

Abstract

The origin of the almost unique combination of optical transparency and the ability to bipolar dope tin monoxide is explained using a combination of soft and hard X-ray photoemission spectroscopy, O K -edge X-ray emission and absorption spectroscopy, and density functional theory calculations incorporating van der Waals corrections. We reveal that the origin of the high hole mobility, bipolar ability, and transparency is a result of (i) significant Sn 5 s character at the valence band maximum (due to O 2 p –Sn 5 s antibonding character associated with the lone pair distortion), (ii) the combination of a small indirect band gap of ∼0.7 eV (Γ–M) and a much larger direct band gap of 2.6–2.7 eV, and (iii) the location of both band edges with respect to the vacuum level. This work supports Sn 2+ -based oxides as a paradigm for next-generation transparent semiconducting oxides.