Capturing anharmonic and anisotropic natures in the thermotics and mechanics of Bi2Te3 thermoelectric material through an accurate and efficient potential

Abstract

Force-field-(FF)-based molecular simulation is essential but challenging in the theoretical research of complex thermoelectric (TE) materials. As they are general and crucial in TE semiconductors, the structural natures of anharmonicity and anisotropy can help us understand the inherent relation between thermal and mechanical behavior, and therefore the reliability of FF studies can be assessed. In this paper, given prior knowledge of the structural, mechanical and thermal properties as well as the limitations and necessary approximations of the FF method, a feasible and detailed FF modeling scheme and simulation has been designed for Bi2Te3, which is a typical high-performance TE material. Using the complementary approach combining quasi-harmonic lattice and molecular dynamics, the obtained potential is systematically confirmed to be accurate and efficient for the prediction of anharmonic and anisotropic behavior in thermotics and mechanics over a wide temperature range compared with the present Bi2Te3 models. This reveals that the intrinsic anisotropy and anharmonicity can measure the asymmetry of crystal lattices and the interatomic force in the current state. In addition, the significant distinction of temperature-dependent anharmonic effects in different directions of Bi2Te3 stems from its layered hierarchical structure, in which weak van der Waals bonding will probably be the key structural factor in comprehensively improving performance for mass production and wearable application. This prior-knowledge-based FF study is also suggested as a bridge between the theoretical understanding of micro-mechanisms and the experimental measurement of TE material properties, leading to a general framework of molecular simulation for other complex energy materials.