Roles of Defects and Sb-Doping in the Thermoelectric Properties of Full-Heusler FeTiSn.

The potential of FeTiSn full-Heusler compounds for thermoelectric applications has been suggested theoretically, but not yet proven experimentally, due to the difficulty in obtaining reproducible, homogeneous, phase-pure and defect-free samples. In this work, we studied FeTiSnSb polycrystals ( from 0 to 0.6), fabricated by high-frequency melting and long-time high-temperature annealing. We obtained fairly good phase purity, a homogeneous microstructure, and good matrix stoichiometry. Although the intrinsic p-type transport behavior is dominant, n-type charge compensation by Sb-doping is demonstrated. Calculations of the formation energy of defects and electronic properties carried out using the density functional theory formalism reveal that charged iron vacancies V are the dominant defects responsible for the intrinsic p-type doping of FeTiSn under all types of (except Fe-rich) growing conditions. In addition, Sb substitutions at the Sn site give rise either to Sb, Sb, which are responsible for n-type doping and magnetism (Sb) or to magnetic Sb, which act as additional p-type dopants. Our experimental data highlight good thermoelectric properties close to room temperature, with Seebeck coefficients up to 56 μV/K in the = 0.2 sample and power factors up to 4.8 × 10 W m K in the = 0.1 sample. Our calculations indicate the appearance of a pseudogap under Ti-rich conditions and a large Sb-doping level, possibly improving further the thermoelectric properties.