Abstract
Deeper understanding of electrical and thermal transport is critical for further development of thermoelectric materials. Here we describe the thermoelectric performance of a group of rare-earth-bearing half-Heusler phases determined in a wide temperature range. Polycrystalline samples of $\mathrm{Sc}\mathrm{Ni}\mathrm{Sb}$, $\mathrm{Dy}\mathrm{Ni}\mathrm{Sb}$, $\mathrm{Er}\mathrm{Ni}\mathrm{Sb}$, $\mathrm{Tm}\mathrm{Ni}\mathrm{Sb}$, and $\mathrm{Lu}\mathrm{Ni}\mathrm{Sb}$ are synthesized by arc melting and densified by spark plasma sintering. They are characterized by powder x-ray diffraction and scanning electron microscopy. The physical properties are studied by means of heat-capacity and Hall-effect measurements performed in the temperature range from 2 to 300 K, as well as electrical-resistivity, Seebeck-coefficient, and thermal-conductivity measurements performed in the temperature range from 2 to 950 K. All the materials except $\mathrm{Tm}\mathrm{Ni}\mathrm{Sb}$ are found to be narrow-gap intrinsic $p$-type semiconductors with rather light charge carriers. In $\mathrm{Tm}\mathrm{Ni}\mathrm{Sb}$, the presence of heavy holes with large weighted mobility is evidenced by the highest power factor among the series ($17\phantom{\rule{0.2em}{0ex}}\ensuremath{\mu}\mathrm{W}\phantom{\rule{0.2em}{0ex}}{\mathrm{K}}^{\ensuremath{-}2}\phantom{\rule{0.2em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$ at 700 K). The experimental electronic relaxation time calculated with the parabolic band formalism is found to range from $0.8\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}$ to $2.8\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}$ s. In all the materials studied, the thermal conductivity is between 3 and $6\phantom{\rule{0.2em}{0ex}}{\mathrm{W m}}^{\ensuremath{-}1}\phantom{\rule{0.2em}{0ex}}{\mathrm{K}}^{\ensuremath{-}1}$ near room temperature (i.e., smaller than in other pristine $d$-electron half-Heusler phases reported in the literature). The experimental observation of the reduced thermal conductivity appears fully consistent with the estimated low sound velocity as well as strong point-defect scattering revealed by Debye-Callaway modeling. Furthermore, analysis of the bipolar contribution to the measured thermal conductivity yields abnormally large differences between the mobilities of $n$-type and $p$-type carriers. The latter feature makes the compounds examined excellent candidates for further optimization of their thermoelectric performance via electron doping.
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