Roles of Defects and Sb-doping in the Thermoelectric Properties of Full-Heusler Fe2TiSn (2502.12636v1)

Abstract: The potential of Fe2TiSn full-Heusler compounds for thermoelectric applications has been suggested theoretically, but not yet grounded experimentally, due to the difficulty of obtaining reproducible, homogeneous, phase pure and defect free samples. In this work, we study Fe2TiSn1-xSbx polycrystals (x from 0 to 0.6), fabricated by high-frequency melting and long-time high-temperature annealing. We obtain fairly good phase purity, homogeneous microstructure and good matrix stoichiometry. Although intrinsic p-type transport behavior is dominant, n-type charge compensation by Sb doping is demonstrated. Calculations of formation energy of defects and electronic properties carried out in the density functional theory formalism reveal that charged iron vacancies VFe2- are the dominant defects responsible for the intrinsic p-type doping of Fe2TiSn in all types of growing conditions except Fe-rich. Additionally, Sb substitutions at Sn site give rise either to SbSn, SbSn1+ which are responsible for n-type doping and magnetism (SbSn) or to magnetic SbSn1- which act as additional p-type dopants. Our experimental data highlight good thermoelectric properties close to room temperature, with Seebeck coefficients up to 56 microV/K in the x=0.2 sample and power factors up to 4.8x10^-4 W m^-1 K^-2 in the x=0.1 sample. Our calculations indicate the appearance of a pseudogap in Ti-rich conditions and large Sb doping, possibly improving further the thermoelectric properties.