A consistent picture of excitations in cubic BaSnO3 revealed by combining theory and experiment

• Published in: Communications materials Vol. 3; no. 1; pp. 1 - 10
• Main Authors: Aggoune, Wahib, Eljarrat, Alberto, Nabok, Dmitrii, Irmscher, Klaus, Zupancic, Martina, Galazka, Zbigniew, Albrecht, Martin, Koch, Christoph, Draxl, Claudia
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group 01.12.2022; Nature Portfolio
• Subjects: Absorption; Barium stannate; Carrier mobility; Crystal defects; Electron energy; Electron energy loss spectroscopy; Electronic structure; Energy gap; Excitation; Perovskites; Phonons; Room temperature; Single crystals; Spectrum analysis; Temperature dependence
• ISSN: 2662-4443; 2662-4443
• DOI: 10.1038/s43246-022-00234-6

Abstract Among the transparent conducting oxides, the perovskite barium stannate is most promising for various electronic applications due to its outstanding carrier mobility achieved at room temperature. However, most of its important characteristics, such as band gaps, effective masses, and absorption edge, remain controversial. Here, we provide a fully consistent picture by combining state-of-the-art ab initio methodology with forefront electron energy-loss spectroscopy and optical absorption measurements. Valence electron energy-loss spectra, featuring signals originating from band gap transitions, are acquired on defect-free sample regions of a BaSnO 3 single crystal. These high-energy-resolution measurements are able to capture also very weak excitations below the optical gap, attributed to indirect transitions. By temperature-dependent optical absorption measurements, we assess band-gap renormalization effects induced by electron-phonon coupling. Overall, we find for the effective electronic mass, the direct and the indirect gap, the optical gap, as well as the absorption onsets and spectra, excellent agreement between both experimental techniques and the theoretical many-body results, supporting also the picture of a phonon-mediated mechanism where indirect transitions are activated by phonon-induced symmetry lowering. This work demonstrates a fruitful connection between different high-level theoretical and experimental methods for exploring the characteristics of advanced materials.