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GeTe, a self-doping $p$-type semiconductor where the high free hole concentration is determined by Ge vacancies is a well-known base for high-efficiency $\mathrm{A}{\mathrm{g}}_{x}\mathrm{S}{\mathrm{b}}_{x}\mathrm{G}{\mathrm{e}}_{50\ensuremath{-}2x}\mathrm{T}{\mathrm{e}}_{50}$ (a tellurium-antimony-germanium-silver series) thermoelectric materials. Here it is shown that the replacement of Ge by Ag in GeTe (a $\mathrm{A}{\mathrm{g}}_{x}\mathrm{G}{\mathrm{e}}_{50\ensuremath{-}x}\mathrm{T}{\mathrm{e}}_{50}$ system) significantly decreases the Seebeck coefficient, whereas the replacement by Sb $(\mathrm{S}{\mathrm{b}}_{x}\mathrm{G}{\mathrm{e}}_{50\ensuremath{-}x}\mathrm{T}{\mathrm{e}}_{50})$ increases it. These effects can be attributed to a change in carrier concentration and consistent with $^{125}\mathrm{Te}$ NMR spin-lattice relaxation measurements and NMR signal position, which is mostly dependent on the Knight shift. Opposite changes in carrier concentration in $\mathrm{A}{\mathrm{g}}_{x}\mathrm{G}{\mathrm{e}}_{50\ensuremath{-}x}\mathrm{T}{\mathrm{e}}_{50}$ and $\mathrm{S}{\mathrm{b}}_{x}\mathrm{G}{\mathrm{e}}_{50\ensuremath{-}x}\mathrm{T}{\mathrm{e}}_{50}$ can be explained by different valence electron configurations of Ag and Sb compared to that of Ge, which results in a different local electron imbalance and/or in a change in Ge vacancy formation energy and affects the total carrier concentration. Comparison of our data for GeTe, $\mathrm{A}{\mathrm{g}}_{2}\mathrm{G}{\mathrm{e}}_{48}\mathrm{T}{\mathrm{e}}_{50}$, and $\mathrm{S}{\mathrm{b}}_{2}\mathrm{G}{\mathrm{e}}_{48}\mathrm{T}{\mathrm{e}}_{50}$ with those for $\mathrm{A}{\mathrm{g}}_{2}\mathrm{S}{\mathrm{b}}_{2}\mathrm{G}{\mathrm{e}}_{46}\mathrm{T}{\mathrm{e}}_{50}$ shows that the effects from Ag and Sb compensate for each other and supports the formation of $[\mathrm{Ag}+\mathrm{Sb}]$ atomic pairs suggested earlier based on theoretical calculations.

physical review. b./physical review. b

Effects of Ge substitution in GeTe by Ag or Sb on the Seebeck coefficient and carrier concentration derived from<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mmultiscripts><mml:mi>Te</mml:mi><mml:mprescripts /><mml:none /><mml:mn>125</mml:mn></mml:mmultiscripts></mml:math>NMR

Effects of Ge substitution in GeTe by Ag or Sb on the Seebeck coefficient and carrier concentration derived fromTe125NMR