skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: First-principles assessment of thermoelectric properties of CuFeS2

Abstract

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.

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. https://www.osti.gov/servlets/purl/1529974.
@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}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 6 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Low effective mass leading to high thermoelectric performance
journal, January 2012

  • Pei, Yanzhong; LaLonde, Aaron D.; Wang, Heng
  • Energy & Environmental Science, Vol. 5, Issue 7
  • DOI: 10.1039/c2ee21536e

High Band Degeneracy Contributes to High Thermoelectric Performance in p-Type Half-Heusler Compounds
journal, August 2014

  • Fu, Chenguang; Zhu, Tiejun; Pei, Yanzhong
  • Advanced Energy Materials, Vol. 4, Issue 18
  • DOI: 10.1002/aenm.201400600

Computationally guided discovery of thermoelectric materials
journal, August 2017


Quantum–continuum simulation of underpotential deposition at electrified metal–solution interfaces
journal, January 2017


Material descriptors for predicting thermoelectric performance
journal, January 2015

  • Yan, Jun; Gorai, Prashun; Ortiz, Brenden
  • Energy & Environmental Science, Vol. 8, Issue 3
  • DOI: 10.1039/C4EE03157A

High Thermoelectric Power Factor and Efficiency from a Highly Dispersive Band in Ba 2 Bi Au
journal, January 2019


Complex thermoelectric materials
journal, February 2008

  • Snyder, G. Jeffrey; Toberer, Eric S.
  • Nature Materials, Vol. 7, Issue 2, p. 105-114
  • DOI: 10.1038/nmat2090

Thinking Like a Chemist: Intuition in Thermoelectric Materials
journal, April 2016

  • Zeier, Wolfgang G.; Zevalkink, Alex; Gibbs, Zachary M.
  • Angewandte Chemie International Edition, Vol. 55, Issue 24
  • DOI: 10.1002/anie.201508381

Ultralow thermal conductivity and high thermoelectric figure of merit in SnSe crystals
journal, April 2014

  • Zhao, Li-Dong; Lo, Shih-Han; Zhang, Yongsheng
  • Nature, Vol. 508, Issue 7496, p. 373-377
  • DOI: 10.1038/nature13184

Ultrahigh power factor and thermoelectric performance in hole-doped single-crystal SnSe
journal, November 2015


3D charge and 2D phonon transports leading to high out-of-plane ZT in n-type SnSe crystals
journal, May 2018


Cubic AgPbmSbTe2+m: Bulk Thermoelectric Materials with High Figure of Merit
journal, February 2004


Broad temperature plateau for thermoelectric figure of merit ZT>2 in phase-separated PbTe0.7S0.3
journal, July 2014

  • Wu, H. J.; Zhao, L. -D.; Zheng, F. S.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5515

Realizing zT of 2.3 in Ge 1− x y Sb x In y Te via Reducing the Phase-Transition Temperature and Introducing Resonant Energy Doping
journal, January 2018


Thin-film thermoelectric devices with high room-temperature figures of merit
journal, October 2001

  • Venkatasubramanian, Rama; Siivola, Edward; Colpitts, Thomas
  • Nature, Vol. 413, Issue 6856, p. 597-602
  • DOI: 10.1038/35098012

High-Thermoelectric Performance of Nanostructured Bismuth Antimony Telluride Bulk Alloys
journal, May 2008


Dense dislocation arrays embedded in grain boundaries for high-performance bulk thermoelectrics
journal, April 2015


Tuning Multiscale Microstructures to Enhance Thermoelectric Performance of n-Type Bismuth-Telluride-Based Solid Solutions
journal, June 2015


Thermoelectric Property Studies on Cu-Doped n-type CuxBi2Te2.7Se0.3 Nanocomposites
journal, June 2011

  • Liu, Wei-Shu; Zhang, Qinyong; Lan, Yucheng
  • Advanced Energy Materials, Vol. 1, Issue 4, p. 577-587
  • DOI: 10.1002/aenm.201100149

High Thermoelectric Performance in Non-Toxic Earth-Abundant Copper Sulfide
journal, March 2014


Thermoelectrics with earth abundant elements: low thermal conductivity and high thermopower in doped SnS
journal, January 2014

  • Tan, Qing; Zhao, Li-Dong; Li, Jing-Feng
  • J. Mater. Chem. A, Vol. 2, Issue 41
  • DOI: 10.1039/C4TA04462B

Remarkable electron and phonon band structures lead to a high thermoelectric performance ZT > 1 in earth-abundant and eco-friendly SnS crystals
journal, January 2018

  • He, Wenke; Wang, Dongyang; Dong, Jin-Feng
  • Journal of Materials Chemistry A, Vol. 6, Issue 21
  • DOI: 10.1039/C8TA03150A

Thermoelectric transport properties of diamond-like Cu 1−x Fe 1+x S 2 tetrahedral compounds
journal, November 2014

  • Li, Yulong; Zhang, Tiansong; Qin, Yuting
  • Journal of Applied Physics, Vol. 116, Issue 20
  • DOI: 10.1063/1.4902849

Phase Stability and Thermoelectric Properties of CuFeS2-Based Magnetic Semiconductor
journal, March 2014

  • Tsujii, Naohito; Mori, Takao; Isoda, Yukihiro
  • Journal of Electronic Materials, Vol. 43, Issue 6
  • DOI: 10.1007/s11664-014-3072-y

High Thermoelectric Power Factor in a Carrier-Doped Magnetic Semiconductor CuFeS 2
journal, April 2013


Synthesis and property evaluation of CuFeS2−x as earth-abundant and environmentally-friendly thermoelectric materials
journal, February 2013


Effect of Nanostructuring and High-Pressure Torsion Process on Thermal Conductivity of Carrier-Doped Chalcopyrite
journal, November 2015

  • Tsujii, Naohito; Meng, Fanqiang; Tsuchiya, Koich
  • Journal of Electronic Materials, Vol. 45, Issue 3
  • DOI: 10.1007/s11664-015-4147-0

The Role of Zn in Chalcopyrite CuFeS 2 : Enhanced Thermoelectric Properties of Cu 1- x Zn x FeS 2 with In Situ Nanoprecipitates
journal, October 2016

  • Xie, Hongyao; Su, Xianli; Zheng, Gang
  • Advanced Energy Materials, Vol. 7, Issue 3
  • DOI: 10.1002/aenm.201601299

First-principles calculations of Seebeck coefficients in a magnetic semiconductor CuFeS 2
journal, February 2017

  • Takaki, Hirokazu; Kobayashi, Kazuaki; Shimono, Masato
  • Applied Physics Letters, Vol. 110, Issue 7
  • DOI: 10.1063/1.4976574

Thermoelectric properties of a magnetic semiconductor CuFeS2
journal, December 2017


Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965


Projector augmented-wave method
journal, December 1994


Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Ab initiomolecular dynamics for liquid metals
journal, January 1993


Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium
journal, May 1994


Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998

  • Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
  • Physical Review B, Vol. 57, Issue 3, p. 1505-1509
  • DOI: 10.1103/PhysRevB.57.1505

Structural, electronic, and elastic properties of CuFeS2: first-principles study
journal, December 2014


Oxidation and magnetic states of chalcopyrite CuFeS2: A first principles calculation
journal, June 2014


Ab initio characterization of magnetic CuFeS 2
journal, November 2004


Symmetry of Magnetic Structures: Magnetic Structure of Chalcopyrite
journal, December 1958


Electronic Structure and Magnetic Properties of CuFeS 2
journal, April 2015


A hybrid-exchange density functional study of the bonding and electronic structure in bulk CuFeS 2
journal, May 2016

  • Martínez-Casado, Ruth; Chen, Vincent H. -Y.; Mallia, Giuseppe
  • The Journal of Chemical Physics, Vol. 144, Issue 18
  • DOI: 10.1063/1.4947080

New Semiconductors with the Chalcopyrite Structure
journal, January 1956

  • Austin, I. G.; Goodman, C. H. L.; Pengelly, A. E.
  • Journal of The Electrochemical Society, Vol. 103, Issue 11
  • DOI: 10.1149/1.2430171

Semiconductors with Chalcopyrite Structure
journal, August 1956

  • Austin, I. G.; Goodman, C. H. L.; Pengelly, A. E.
  • Nature, Vol. 178, Issue 4530
  • DOI: 10.1038/178433a0

Optical Properties of a Magnetic Semiconductor: Chalcopyrite CuFeS 2 .: I. Absorption Spectra of CuFeS 2 and Fe-Doped CuAlS 2 and CuGaS 2
journal, June 1974

  • Teranishi, Teruo; Sato, Katsuaki; Kondo, Ken'ichi
  • Journal of the Physical Society of Japan, Vol. 36, Issue 6
  • DOI: 10.1143/JPSJ.36.1618

BoltzTraP. A code for calculating band-structure dependent quantities
journal, July 2006


Thermoelectric band engineering: The role of carrier scattering
journal, November 2017

  • Witkoske, Evan; Wang, Xufeng; Lundstrom, Mark
  • Journal of Applied Physics, Vol. 122, Issue 17
  • DOI: 10.1063/1.4994696

First Principles Explanation of the Positive Seebeck Coefficient of Lithium
journal, May 2014


High Thermoelectric Power Factor in Intermetallic Co Si Arising from Energy Filtering of Electrons by Phonon Scattering
journal, February 2019


Thermoelectric properties and figure of merit of a Te-doped InSb bulk single crystal
journal, November 2005

  • Yamaguchi, Shigeo; Matsumoto, Takayuki; Yamazaki, Jun
  • Applied Physics Letters, Vol. 87, Issue 20
  • DOI: 10.1063/1.2130390

Convergence of electronic bands for high performance bulk thermoelectrics
journal, May 2011

  • Pei, Yanzhong; Shi, Xiaoya; LaLonde, Aaron
  • Nature, Vol. 473, Issue 7345, p. 66-69
  • DOI: 10.1038/nature09996

Observation of Dirac-like energy band and ring-torus Fermi surface associated with the nodal line in topological insulator CaAgAs
journal, January 2018


Classification of Valleytronics in Thermoelectricity
journal, March 2016

  • Norouzzadeh, Payam; Vashaee, Daryoosh
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep22724

High-Performance Pseudocubic Thermoelectric Materials from Non-cubic Chalcopyrite Compounds
journal, April 2014


Band convergence in the non-cubic chalcopyrite compounds Cu 2 MGeSe 4
journal, January 2014

  • Zeier, Wolfgang G.; Zhu, Hong; Gibbs, Zachary M.
  • J. Mater. Chem. C, Vol. 2, Issue 47
  • DOI: 10.1039/C4TC02218A

Lattice Anharmonicity and Thermal Conductivity from Compressive Sensing of First-Principles Calculations
journal, October 2014


ShengBTE: A solver of the Boltzmann transport equation for phonons
journal, June 2014

  • Li, Wu; Carrete, Jesús; A. Katcho, Nebil
  • Computer Physics Communications, Vol. 185, Issue 6
  • DOI: 10.1016/j.cpc.2014.02.015

Phonons and related crystal properties from density-functional perturbation theory
journal, July 2001

  • Baroni, Stefano; de Gironcoli, Stefano; Dal Corso, Andrea
  • Reviews of Modern Physics, Vol. 73, Issue 2
  • DOI: 10.1103/RevModPhys.73.515

High-performance nanostructured thermoelectric materials
journal, October 2010


Bulk nanostructured thermoelectric materials: current research and future prospects
journal, January 2009

  • Minnich, A. J.; Dresselhaus, M. S.; Ren, Z. F.
  • Energy & Environmental Science, Vol. 2, Issue 5
  • DOI: 10.1039/b822664b

    Works referencing / citing this record:

    First Principles Investigation of Anomalous Pressure-Dependent Thermal Conductivity of Chalcopyrites
    journal, October 2019

    • Elalfy, Loay; Music, Denis; Hu, Ming
    • Materials, Vol. 12, Issue 21
    • DOI: 10.3390/ma12213491

    First Principles Investigation of Anomalous Pressure-Dependent Thermal Conductivity of Chalcopyrites
    journal, October 2019

    • Elalfy, Loay; Music, Denis; Hu, Ming
    • Materials, Vol. 12, Issue 21
    • DOI: 10.3390/ma12213491