Diffusion dominant thermal transport in mixed valent Ba4Sn4Se9

Abstract

New material developments are of paramount importance from the perspective of developing a fundamental understanding of material properties as well as transitioning from materials to devices. Among the different classes of materials of interest, mixed valence Sn compositions have been known to display technologically important properties and are of interest for the design and synthesis of novel compositions for targeted applications. Herein, we report on electronic, optical and thermal properties of the previously unexplored mixed valence composition Ba4Sn4Se9, a material with a direct optical band gap of 2.36 eV. As revealed by single crystal synchrotron X-ray diffraction, Ba4Sn4Se9 crystallizes in the orthorhombic space group Pnma with a large unit cell comprised of 58 atoms. Heat capacity data reveals a low Debye temperature with many low frequency optic modes. Our low temperature thermal conductivity data and analyses show that thermal diffusion dominates thermal transport above 80 K. Furthermore, high lattice anharmonicity contributes to the very low thermal conductivity. Our results and analyses will motivate further investigations of this as well as other compositions in the Ba-Sn-Se system, as well as other mixed valence chalcogenides for technological applications.