First-principles thermodynamic theory of Seebeck coefficients

Yi Wang, Yong Jie Hu, Brandon Bocklund, Shun Li Shang, Bi Cheng Zhou, Zi Kui Liu, Long Qing Chen

Research output: Contribution to journalArticle

5 Citations (Scopus)

Abstract

Thermoelectric effects, measured by the Seebeck coefficients, refer to the phenomena in which a temperature difference or gradient imposed across a thermoelectric material induces an electrical potential difference or gradient, and vice versa, enabling the direct conversion of thermal and electric energies. All existing first-principles calculations of Seebeck coefficients have been based on the Boltzmann kinetic transport theory. In this work, we present a fundamentally different method for the first-principles calculations of Seebeck coefficients without using any assumptions of the electron-scattering mechanism, being in contrast to the traditional theory by Cutler and Mott that shows the dependence of the Seebeck coefficient on the scattering mechanisms. It is shown that the Seebeck coefficient is a well-defined thermodynamic quantity that can be determined from the change in the chemical potential of electrons induced by the temperature change and thus can be computed solely based on the electronic density of states through first-principles calculations at different temperatures. The proposed approach is demonstrated using the prototype PbTe and SnSe thermoelectric materials.

Original languageEnglish (US)
Article number224101
JournalPhysical Review B
Volume98
Issue number22
DOIs
StatePublished - Dec 3 2018

Fingerprint

Seebeck coefficient
Seebeck effect
Thermodynamics
thermodynamics
thermoelectric materials
temperature gradients
Thermoelectricity
Electronic density of states
Electron scattering
transport theory
Chemical potential
thermal energy
Temperature
electron scattering
prototypes
Scattering
gradients
Kinetics
temperature
Electrons

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Condensed Matter Physics

Cite this

Wang, Yi ; Hu, Yong Jie ; Bocklund, Brandon ; Shang, Shun Li ; Zhou, Bi Cheng ; Liu, Zi Kui ; Chen, Long Qing. / First-principles thermodynamic theory of Seebeck coefficients. In: Physical Review B. 2018 ; Vol. 98, No. 22.
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First-principles thermodynamic theory of Seebeck coefficients. / Wang, Yi; Hu, Yong Jie; Bocklund, Brandon; Shang, Shun Li; Zhou, Bi Cheng; Liu, Zi Kui; Chen, Long Qing.

In: Physical Review B, Vol. 98, No. 22, 224101, 03.12.2018.

Research output: Contribution to journalArticle

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AU - Wang, Yi

AU - Hu, Yong Jie

AU - Bocklund, Brandon

AU - Shang, Shun Li

AU - Zhou, Bi Cheng

AU - Liu, Zi Kui

AU - Chen, Long Qing

PY - 2018/12/3

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AB - Thermoelectric effects, measured by the Seebeck coefficients, refer to the phenomena in which a temperature difference or gradient imposed across a thermoelectric material induces an electrical potential difference or gradient, and vice versa, enabling the direct conversion of thermal and electric energies. All existing first-principles calculations of Seebeck coefficients have been based on the Boltzmann kinetic transport theory. In this work, we present a fundamentally different method for the first-principles calculations of Seebeck coefficients without using any assumptions of the electron-scattering mechanism, being in contrast to the traditional theory by Cutler and Mott that shows the dependence of the Seebeck coefficient on the scattering mechanisms. It is shown that the Seebeck coefficient is a well-defined thermodynamic quantity that can be determined from the change in the chemical potential of electrons induced by the temperature change and thus can be computed solely based on the electronic density of states through first-principles calculations at different temperatures. The proposed approach is demonstrated using the prototype PbTe and SnSe thermoelectric materials.

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