Topological insulators (TIs) and thermoelectric (TE) materials seem to belong to distinct physical realms; however, in practice, they both share common characteristics. Introducing concepts from TIs into TE materials to enhance their performance and achieve better understanding of electronic transport requires extensive research. Particularly, grain size, misorientation, and grain boundary (GB) character are of utmost importance to attain effective charge carrier transport in TE polycrystals; these factors, however, have not been thoroughly explored. Herein, we investigate the correlation between grain size, misorientation, and lattice strain in Bi2Te3 and its TI signature, aiming to improve its TE performance. We reveal an unusual behavior showing that electron mobility increases upon the increase of grain size, reaching at a maximum value of 495 cm2/V·s for an optimum grain size of 600 nm and most-frequent GB misorientation angle of 60° and then decreases with increasing grain size. It is also indicated that the combined effects of grain size reduction and point defects induce lattice strain in the Bi2Te3-matrix that is essential to trigger the TI contribution to TE transport. This trend is corroborated by first-principles calculations showing that compressive strains form multiple valleys in the valence band and opens the TI band gap. Such a combination of physical phenomena in a well-known TE material is unique and can promote our understanding of the nature of TE transport with implications for TE energy conversion.
Keywords: bismuth-telluride; density functional theory (DFT); grain boundary misorientation; thermoelectric materials; thermoelectric transport coefficients; topological insulators.