Thermoelectric properties of sintered Ba2AgSi3 crystals and search for impurities to control conductivity type by first-principles calculation

Abstract

In this study, the basic properties of Ba2AgSi3 were investigated in detail from both experimental and computational viewpoints. Polycrystalline Ba2AgSi3 formed by an arc-melting apparatus under an argon atmosphere was ground into powders, and then powder samples were sintered using the spark plasma sintering method. Both n-type and p-type samples were obtained. This may be due to a slight deviation from the stoichiometric composition. The energy bandgap of Ba2AgSi3 was measured to be around 0.17 eV from the temperature dependence of electrical conductivity and was in agreement with that by first-principles calculations. Sintered samples exhibited a high Seebeck coefficient of −273 μV K−1 and a high power factor of 0.38 mW m−1 K−2 at 307 K for n-type samples. They were 217 μV K−1 and 0.23 mW m−1 K−2, respectively, at 320 K for p-type samples. The electronic structures of impurity-doped Ba2AgSi3 were also discussed using first-principles calculations to investigate the insertion site of impurity atoms. The calculations suggest that the substitution of B (P) at any Si site shifts the Fermi level and transforms it into p-type (n-type) semiconductors. On the other hand, substitution of Ba or Ag sites with B or P is unlikely to occur in terms of formation energy.