First-principles thermodynamic theory of Seebeck coefficients

Journal Article · 03 December 2018 · Physical Review B

DOI: https://doi.org/10.1103/PhysRevB.98.224101 · OSTI ID:1544153

Wang, Yi ^[1]; Hu, Yong-Jie ^[1]; Bocklund, Brandon ^[1]; Shang, Shun-Li ^[1]; Zhou, Bi-Cheng ^[1]; Liu, Zi-Kui ^[1]; Chen, Long-Qing ^[1]

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1. The Pennsylvania State Univ., University Park, PA (United States)

To begin, 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.

• Research Organization: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
• Grant/Contract Number: FG02-07ER46417; AC02-05CH11231
• OSTI ID: 1544153
• Alternate ID(s): OSTI ID: 1484325
• Journal Information: Physical Review B, Vol. 98, Issue 22; ISSN 2469-9950
• Publisher: American Physical Society (APS)Copyright Statement
• Country of Publication: United States
• Language: English