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Title: First-principles assessment of thermoelectric properties of CuFeS 2

Abstract

Composed of inexpensive and naturally abundant elements, the chalcopyrite mineral CuFeS 2 has received attention as a potentially useful thermoelectric. We use first-principles electronic structure and Boltzmann transport theory calculations to investigate thermoelectric properties of n-doped CuFeS 2. We find that energy-dependent carrier lifetimes that are inversely proportional to the electronic density-of-states are crucial for reproducing experimental data on the transport properties, including the measured values of the Seebeck coefficient, α. The heavy-effective-mass conduction band promotes high values of α, but it also leads to low mobility due to strong electron-acoustic-phonon scattering. Low mobility forces one to rely on high carrier concentration to achieve high conductivity, which decreases α and limits the achievable power factor. Our calculations predict that ideally doped CuFeS 2 that has been nanostructured to an average grain size d≈20nm can attain thermoelectric figures of merit zT=0.25 to 0.8 for T=300 to 700 K, respectively, due to a reduction in the lattice thermal conductivity.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]
  1. Univ. of California, Los Angeles, CA (United States)
  2. Northwestern Univ., Evanston, IL (United States)
  3. Yale Univ., New Haven, CT (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1529974
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 125; Journal Issue: 12; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Park, Junsoo, Xia, Yi, and Ozoliņš, Vidvuds. First-principles assessment of thermoelectric properties of CuFeS2. United States: N. p., 2019. Web. doi:10.1063/1.5088165.
Park, Junsoo, Xia, Yi, & Ozoliņš, Vidvuds. First-principles assessment of thermoelectric properties of CuFeS2. United States. doi:10.1063/1.5088165.
Park, Junsoo, Xia, Yi, and Ozoliņš, Vidvuds. Fri . "First-principles assessment of thermoelectric properties of CuFeS2". United States. doi:10.1063/1.5088165.
@article{osti_1529974,
title = {First-principles assessment of thermoelectric properties of CuFeS2},
author = {Park, Junsoo and Xia, Yi and Ozoliņš, Vidvuds},
abstractNote = {Composed of inexpensive and naturally abundant elements, the chalcopyrite mineral CuFeS2 has received attention as a potentially useful thermoelectric. We use first-principles electronic structure and Boltzmann transport theory calculations to investigate thermoelectric properties of n-doped CuFeS2. We find that energy-dependent carrier lifetimes that are inversely proportional to the electronic density-of-states are crucial for reproducing experimental data on the transport properties, including the measured values of the Seebeck coefficient, α. The heavy-effective-mass conduction band promotes high values of α, but it also leads to low mobility due to strong electron-acoustic-phonon scattering. Low mobility forces one to rely on high carrier concentration to achieve high conductivity, which decreases α and limits the achievable power factor. Our calculations predict that ideally doped CuFeS2 that has been nanostructured to an average grain size d≈20nm can attain thermoelectric figures of merit zT=0.25 to 0.8 for T=300 to 700 K, respectively, due to a reduction in the lattice thermal conductivity.},
doi = {10.1063/1.5088165},
journal = {Journal of Applied Physics},
number = 12,
volume = 125,
place = {United States},
year = {2019},
month = {3}
}

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