Amphoteric Indium Enables Carrier Engineering to Enhance the Power Factor and Thermoelectric Performance in n-Type Ag n Pb 100 In n Te 100+2 n (LIST)

Yu Xiao, Haijun Wu, Dongyang Wang, Changlei Niu, Yanling Pei, Yang Zhang, Ioannis Spanopoulos, Ian Thomas Witting, Xin Li, Stephen J. Pennycook, Gerald Jeffrey Snyder, Mercouri G Kanatzidis, Li Dong Zhao

Research output: Contribution to journalArticle

2 Citations (Scopus)

Abstract

The Ag and In co-doped PbTe, Ag n Pb 100 In n Te 100+2 n (LIST), exhibits n-type behavior and features unique inherent electronic levels that induce self-tuning carrier density. Results show that In is amphoteric in the LIST, forming both In 3+ and In 1+ centers. Through unique interplay of valence fluctuations in the In centers and conduction band filling, the electron carrier density can be increased from ≈3.1 × 10 18 cm −3 at 323 K to ≈2.4 × 10 19 cm −3 at 820 K, leading to large power factors peaking at ≈16.0 µWcm −1 K −2 at 873 K. The lone pair of electrons from In + can be thermally continuously promoted into the conduction band forming In 3+ , consistent with the amphoteric character of In. Moreover, with rising temperature, the Fermi level shifts into the conduction band, which enlarges the optical band gap based on the Moss–Burstein effect, and reduces bipolar diffusion and thermal conductivity. Adding extra Ag in LIST improves the electrical transport properties and meanwhile lowers the lattice thermal conductivity to ≈0.40 Wm −1 K −1 . The addition of Ag creates spindle-shaped Ag 2 Te nanoprecipitates and atomic-scale interstitials that scatter a broader set of phonons. As a result, a maximum ZT value ≈1.5 at 873 K is achieved in Ag 6 Pb 100 InTe 102 (LIST).

Original languageEnglish
Article number1900414
JournalAdvanced Energy Materials
DOIs
Publication statusPublished - Jan 1 2019

Fingerprint

Indium
Conduction bands
Carrier concentration
Thermal conductivity
Electrons
Optical band gaps
Phonons
Fermi level
Transport properties
Tuning
Temperature

Keywords

  • bipolar diffusion
  • LIST
  • power factor
  • thermoelectrics
  • ZT

ASJC Scopus subject areas

  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)

Cite this

Amphoteric Indium Enables Carrier Engineering to Enhance the Power Factor and Thermoelectric Performance in n-Type Ag n Pb 100 In n Te 100+2 n (LIST) . / Xiao, Yu; Wu, Haijun; Wang, Dongyang; Niu, Changlei; Pei, Yanling; Zhang, Yang; Spanopoulos, Ioannis; Witting, Ian Thomas; Li, Xin; Pennycook, Stephen J.; Snyder, Gerald Jeffrey; Kanatzidis, Mercouri G; Zhao, Li Dong.

In: Advanced Energy Materials, 01.01.2019.

Research output: Contribution to journalArticle

Xiao, Yu ; Wu, Haijun ; Wang, Dongyang ; Niu, Changlei ; Pei, Yanling ; Zhang, Yang ; Spanopoulos, Ioannis ; Witting, Ian Thomas ; Li, Xin ; Pennycook, Stephen J. ; Snyder, Gerald Jeffrey ; Kanatzidis, Mercouri G ; Zhao, Li Dong. / Amphoteric Indium Enables Carrier Engineering to Enhance the Power Factor and Thermoelectric Performance in n-Type Ag n Pb 100 In n Te 100+2 n (LIST) In: Advanced Energy Materials. 2019.
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abstract = "The Ag and In co-doped PbTe, Ag n Pb 100 In n Te 100+2 n (LIST), exhibits n-type behavior and features unique inherent electronic levels that induce self-tuning carrier density. Results show that In is amphoteric in the LIST, forming both In 3+ and In 1+ centers. Through unique interplay of valence fluctuations in the In centers and conduction band filling, the electron carrier density can be increased from ≈3.1 × 10 18 cm −3 at 323 K to ≈2.4 × 10 19 cm −3 at 820 K, leading to large power factors peaking at ≈16.0 µWcm −1 K −2 at 873 K. The lone pair of electrons from In + can be thermally continuously promoted into the conduction band forming In 3+ , consistent with the amphoteric character of In. Moreover, with rising temperature, the Fermi level shifts into the conduction band, which enlarges the optical band gap based on the Moss–Burstein effect, and reduces bipolar diffusion and thermal conductivity. Adding extra Ag in LIST improves the electrical transport properties and meanwhile lowers the lattice thermal conductivity to ≈0.40 Wm −1 K −1 . The addition of Ag creates spindle-shaped Ag 2 Te nanoprecipitates and atomic-scale interstitials that scatter a broader set of phonons. As a result, a maximum ZT value ≈1.5 at 873 K is achieved in Ag 6 Pb 100 InTe 102 (LIST).",
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author = "Yu Xiao and Haijun Wu and Dongyang Wang and Changlei Niu and Yanling Pei and Yang Zhang and Ioannis Spanopoulos and Witting, {Ian Thomas} and Xin Li and Pennycook, {Stephen J.} and Snyder, {Gerald Jeffrey} and Kanatzidis, {Mercouri G} and Zhao, {Li Dong}",
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AU - Wu, Haijun

AU - Wang, Dongyang

AU - Niu, Changlei

AU - Pei, Yanling

AU - Zhang, Yang

AU - Spanopoulos, Ioannis

AU - Witting, Ian Thomas

AU - Li, Xin

AU - Pennycook, Stephen J.

AU - Snyder, Gerald Jeffrey

AU - Kanatzidis, Mercouri G

AU - Zhao, Li Dong

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N2 - The Ag and In co-doped PbTe, Ag n Pb 100 In n Te 100+2 n (LIST), exhibits n-type behavior and features unique inherent electronic levels that induce self-tuning carrier density. Results show that In is amphoteric in the LIST, forming both In 3+ and In 1+ centers. Through unique interplay of valence fluctuations in the In centers and conduction band filling, the electron carrier density can be increased from ≈3.1 × 10 18 cm −3 at 323 K to ≈2.4 × 10 19 cm −3 at 820 K, leading to large power factors peaking at ≈16.0 µWcm −1 K −2 at 873 K. The lone pair of electrons from In + can be thermally continuously promoted into the conduction band forming In 3+ , consistent with the amphoteric character of In. Moreover, with rising temperature, the Fermi level shifts into the conduction band, which enlarges the optical band gap based on the Moss–Burstein effect, and reduces bipolar diffusion and thermal conductivity. Adding extra Ag in LIST improves the electrical transport properties and meanwhile lowers the lattice thermal conductivity to ≈0.40 Wm −1 K −1 . The addition of Ag creates spindle-shaped Ag 2 Te nanoprecipitates and atomic-scale interstitials that scatter a broader set of phonons. As a result, a maximum ZT value ≈1.5 at 873 K is achieved in Ag 6 Pb 100 InTe 102 (LIST).

AB - The Ag and In co-doped PbTe, Ag n Pb 100 In n Te 100+2 n (LIST), exhibits n-type behavior and features unique inherent electronic levels that induce self-tuning carrier density. Results show that In is amphoteric in the LIST, forming both In 3+ and In 1+ centers. Through unique interplay of valence fluctuations in the In centers and conduction band filling, the electron carrier density can be increased from ≈3.1 × 10 18 cm −3 at 323 K to ≈2.4 × 10 19 cm −3 at 820 K, leading to large power factors peaking at ≈16.0 µWcm −1 K −2 at 873 K. The lone pair of electrons from In + can be thermally continuously promoted into the conduction band forming In 3+ , consistent with the amphoteric character of In. Moreover, with rising temperature, the Fermi level shifts into the conduction band, which enlarges the optical band gap based on the Moss–Burstein effect, and reduces bipolar diffusion and thermal conductivity. Adding extra Ag in LIST improves the electrical transport properties and meanwhile lowers the lattice thermal conductivity to ≈0.40 Wm −1 K −1 . The addition of Ag creates spindle-shaped Ag 2 Te nanoprecipitates and atomic-scale interstitials that scatter a broader set of phonons. As a result, a maximum ZT value ≈1.5 at 873 K is achieved in Ag 6 Pb 100 InTe 102 (LIST).

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