Valence-band structure of highly efficient p-type thermoelectric PbTe-PbS alloys

Christopher M. Jaworski; Michele D. Nielsen; Hsin Wang; Steven N. Girard; Wei Cai; Wally D. Porter; Mercouri G. Kanatzidis; Joseph P. Heremans

doi:10.1103/PhysRevB.87.045203

Valence-band structure of highly efficient p-type thermoelectric PbTe-PbS alloys

Christopher M. Jaworski^*, Michele D. Nielsen, Hsin Wang, Steven N. Girard, Wei Cai, Wally D. Porter, Mercouri G. Kanatzidis, Joseph P. Heremans

^*Corresponding author for this work

Chemistry

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57 Scopus citations

Abstract

Experimental evidence is given relevant to the temperature dependence of the valence band structure of PbTe and PbTe_1-xS_xaloys (0.04≤x≤0.12), and its effect on the thermoelectric figure of merit ZT. The x=0.08 sample has ZT∼1.55 at 773 K. The magnetic field dependence of the high-temperature Hall resistivity of heavily p-type (>1019 cm^-3) Na-doped PbTe_1-xS_x reveals the presence of high-mobility electrons. This casts doubts on prior analyses of the Hall coefficient suggesting that temperature induces a rapid rise in energy of the "heavy" hole relative to the "light" hole bands. The electron-like behavior is likely induced by the topology of the Fermi surface when the L- and Σ-bands merge. Negative values for the low-temperature thermopower are also observed. The data show that PbTe continues to be a direct-gap semiconductor at temperatures where the ZT and S2σ of p-type PbTe are optimal, e.g., 700-800 K.

Original language	English (US)
Article number	045203
Journal	Physical Review B - Condensed Matter and Materials Physics
Volume	87
Issue number	4
DOIs	https://doi.org/10.1103/PhysRevB.87.045203
State	Published - Jan 4 2013

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Condensed Matter Physics

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abstract = "Experimental evidence is given relevant to the temperature dependence of the valence band structure of PbTe and PbTe1-xSxaloys (0.04≤x≤0.12), and its effect on the thermoelectric figure of merit ZT. The x=0.08 sample has ZT∼1.55 at 773 K. The magnetic field dependence of the high-temperature Hall resistivity of heavily p-type (>1019 cm-3) Na-doped PbTe1-xSx reveals the presence of high-mobility electrons. This casts doubts on prior analyses of the Hall coefficient suggesting that temperature induces a rapid rise in energy of the {"}heavy{"} hole relative to the {"}light{"} hole bands. The electron-like behavior is likely induced by the topology of the Fermi surface when the L- and Σ-bands merge. Negative values for the low-temperature thermopower are also observed. The data show that PbTe continues to be a direct-gap semiconductor at temperatures where the ZT and S2σ of p-type PbTe are optimal, e.g., 700-800 K.",

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Valence-band structure of highly efficient p-type thermoelectric PbTe-PbS alloys. / Jaworski, Christopher M.; Nielsen, Michele D.; Wang, Hsin; Girard, Steven N.; Cai, Wei; Porter, Wally D.; Kanatzidis, Mercouri G.; Heremans, Joseph P.

In: Physical Review B - Condensed Matter and Materials Physics, Vol. 87, No. 4, 045203, 04.01.2013.

Research output: Contribution to journal › Article › peer-review

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AU - Jaworski, Christopher M.

AU - Nielsen, Michele D.

AU - Wang, Hsin

AU - Girard, Steven N.

AU - Cai, Wei

AU - Porter, Wally D.

AU - Kanatzidis, Mercouri G.

AU - Heremans, Joseph P.

PY - 2013/1/4

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N2 - Experimental evidence is given relevant to the temperature dependence of the valence band structure of PbTe and PbTe1-xSxaloys (0.04≤x≤0.12), and its effect on the thermoelectric figure of merit ZT. The x=0.08 sample has ZT∼1.55 at 773 K. The magnetic field dependence of the high-temperature Hall resistivity of heavily p-type (>1019 cm-3) Na-doped PbTe1-xSx reveals the presence of high-mobility electrons. This casts doubts on prior analyses of the Hall coefficient suggesting that temperature induces a rapid rise in energy of the "heavy" hole relative to the "light" hole bands. The electron-like behavior is likely induced by the topology of the Fermi surface when the L- and Σ-bands merge. Negative values for the low-temperature thermopower are also observed. The data show that PbTe continues to be a direct-gap semiconductor at temperatures where the ZT and S2σ of p-type PbTe are optimal, e.g., 700-800 K.

AB - Experimental evidence is given relevant to the temperature dependence of the valence band structure of PbTe and PbTe1-xSxaloys (0.04≤x≤0.12), and its effect on the thermoelectric figure of merit ZT. The x=0.08 sample has ZT∼1.55 at 773 K. The magnetic field dependence of the high-temperature Hall resistivity of heavily p-type (>1019 cm-3) Na-doped PbTe1-xSx reveals the presence of high-mobility electrons. This casts doubts on prior analyses of the Hall coefficient suggesting that temperature induces a rapid rise in energy of the "heavy" hole relative to the "light" hole bands. The electron-like behavior is likely induced by the topology of the Fermi surface when the L- and Σ-bands merge. Negative values for the low-temperature thermopower are also observed. The data show that PbTe continues to be a direct-gap semiconductor at temperatures where the ZT and S2σ of p-type PbTe are optimal, e.g., 700-800 K.

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Valence-band structure of highly efficient p-type thermoelectric PbTe-PbS alloys

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