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 language | English (US) |
|---|---|
| Article number | 224101 |
| Journal | Physical Review B |
| Volume | 98 |
| Issue number | 22 |
| DOIs | |
| State | Published - Dec 3 2018 |
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All Science Journal Classification (ASJC) codes
- Electronic, Optical and Magnetic Materials
- Condensed Matter Physics
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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 journal › Article
TY - JOUR
T1 - First-principles thermodynamic theory of Seebeck coefficients
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
Y1 - 2018/12/3
N2 - 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.
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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U2 - 10.1103/PhysRevB.98.224101
DO - 10.1103/PhysRevB.98.224101
M3 - Article
AN - SCOPUS:85057578695
VL - 98
JO - Physical Review B-Condensed Matter
JF - Physical Review B-Condensed Matter
SN - 2469-9950
IS - 22
M1 - 224101
ER -