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We report a study of the temperature-dependent electrical resistivity, Seebeck coefficient, thermal conductivity, specific heat, and $^{27}\mathrm{Al}$ nuclear magnetic resonance (NMR) in Heusler-type ${\mathrm{Ru}}_{2}\mathrm{TaAl}$, to shed light on its semimetallic behavior. While the temperature dependence of the electrical resistivity exhibits semiconductorlike behavior, the analysis of low-temperature specific heat reveals a residual Fermi-level density of states (DOS). Both observations can be realized by means of a semimetallic scenario with the Fermi energy located in the pseudogap of the electronic DOS. The NMR Knight shift and spin-lattice relaxation rate show activated behavior at higher temperatures, attributing to the thermally excited carriers across a pseudogap in ${\mathrm{Ru}}_{2}\mathrm{TaAl}$. From the first-principles band structure calculations, we further provide a clear picture that an indirect overlap between electron and hole pockets is responsible for the formation of a pseudogap in the vicinity of the Fermi level of ${\mathrm{Ru}}_{2}\mathrm{TaAl}$. In addition, an effort for improving the thermoelectric performance of ${\mathrm{Ru}}_{2}\mathrm{TaAl}$ has been made by investigating the thermoelectric properties of ${\mathrm{Ru}}_{1.95}{\mathrm{Ta}}_{1.05}\mathrm{Al}$. We found significant enhancements in the electrical conductivity and Seebeck coefficient and marked reduction in the thermal conductivity via the off-stoichiometric approach. This leads to an increase in the figure-of-merit $ZT$ value from $6.1\ifmmode\times\else\texttimes\fi{}\phantom{\rule{0.16em}{0ex}}{10}^{\ensuremath{-}4}$ in ${\mathrm{Ru}}_{2}\mathrm{TaAl}$ to $3.4\ifmmode\times\else\texttimes\fi{}\phantom{\rule{0.16em}{0ex}}{10}^{\ensuremath{-}3}$ in ${\mathrm{Ru}}_{1.95}{\mathrm{Ta}}_{1.05}\mathrm{Al}$ at room temperature. In this respect, a further improvement of thermoelectric performance based on ${\mathrm{Ru}}_{2}\mathrm{TaAl}$ through other off-stoichiometric attempts is highly probable.

physical review. b./physical review. b

Semimetallic behavior in Heusler-type <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:msub><mml:mi>Ru</mml:mi><mml:mn>2</mml:mn></mml:msub><mml:mi>TaAl</mml:mi></mml:mrow></mml:math> and thermoelectric performance improved by off-stoichiometry

Semimetallic behavior in Heusler-type Ru2TaAl and thermoelectric performance improved by off-stoichiometry