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

Title: Large thermoelectric power factor from crystal symmetry-protected non-bonding orbital in half-Heuslers

Abstract

Modern society relies on high charge mobility for efficient energy production and fast information technologies. The power factor of a material—the combination of electrical conductivity and Seebeck coefficient—measures its ability to extract electrical power from temperature differences. Recent advancements in thermoelectric materials have achieved enhanced Seebeck coefficient by manipulating the electronic band structure. However, this approach generally applies at relatively low conductivities, preventing the realization of exceptionally high-power factors. In contrast, half-Heusler semiconductors have been shown to break through that barrier in a way that could not be explained. Here, we show that symmetry-protected orbital interactions can steer electron–acoustic phonon interactions towards high mobility. This high-mobility regime enables large power factors in half-Heuslers, well above the maximum measured values. We anticipate that our understanding will spark new routes to search for better thermoelectric materials, and to discover high electron mobility semiconductors for electronic and photonic applications.

Authors:
ORCiD logo [1];  [2];  [1]; ORCiD logo [1];  [3]; ORCiD logo [4];  [2];  [2];  [5];  [6];  [2]; ORCiD logo [1]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Mechanical Engineering
  2. Univ. of Houston, Houston, TX (United States). Dept. of Physics and Texas Center for Superconductivity
  3. Institut für Metallische Werkstoffe, Dresden (Germany). IFW Dresden
  4. Univ. of Houston, Houston, TX (United States). Dept. of Physics and Texas Center for Superconductivity and Dept. of Mechanical Engineering
  5. Univ. of California, Santa Barbara, CA (United States). Dept. of Mechanical Engineering
  6. Univ. of Missouri, Columbia, MO (United States). Dept. of Physics and Astronomy
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1526317
Grant/Contract Number:  
SC0001299; FG02-09ER46577
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING

Citation Formats

Zhou, Jiawei, Zhu, Hangtian, Liu, Te -Huan, Song, Qichen, He, Ran, Mao, Jun, Liu, Zihang, Ren, Wuyang, Liao, Bolin, Singh, David J., Ren, Zhifeng, and Chen, Gang. Large thermoelectric power factor from crystal symmetry-protected non-bonding orbital in half-Heuslers. United States: N. p., 2018. Web. https://doi.org/10.1038/s41467-018-03866-w.
Zhou, Jiawei, Zhu, Hangtian, Liu, Te -Huan, Song, Qichen, He, Ran, Mao, Jun, Liu, Zihang, Ren, Wuyang, Liao, Bolin, Singh, David J., Ren, Zhifeng, & Chen, Gang. Large thermoelectric power factor from crystal symmetry-protected non-bonding orbital in half-Heuslers. United States. https://doi.org/10.1038/s41467-018-03866-w
Zhou, Jiawei, Zhu, Hangtian, Liu, Te -Huan, Song, Qichen, He, Ran, Mao, Jun, Liu, Zihang, Ren, Wuyang, Liao, Bolin, Singh, David J., Ren, Zhifeng, and Chen, Gang. Mon . "Large thermoelectric power factor from crystal symmetry-protected non-bonding orbital in half-Heuslers". United States. https://doi.org/10.1038/s41467-018-03866-w. https://www.osti.gov/servlets/purl/1526317.
@article{osti_1526317,
title = {Large thermoelectric power factor from crystal symmetry-protected non-bonding orbital in half-Heuslers},
author = {Zhou, Jiawei and Zhu, Hangtian and Liu, Te -Huan and Song, Qichen and He, Ran and Mao, Jun and Liu, Zihang and Ren, Wuyang and Liao, Bolin and Singh, David J. and Ren, Zhifeng and Chen, Gang},
abstractNote = {Modern society relies on high charge mobility for efficient energy production and fast information technologies. The power factor of a material—the combination of electrical conductivity and Seebeck coefficient—measures its ability to extract electrical power from temperature differences. Recent advancements in thermoelectric materials have achieved enhanced Seebeck coefficient by manipulating the electronic band structure. However, this approach generally applies at relatively low conductivities, preventing the realization of exceptionally high-power factors. In contrast, half-Heusler semiconductors have been shown to break through that barrier in a way that could not be explained. Here, we show that symmetry-protected orbital interactions can steer electron–acoustic phonon interactions towards high mobility. This high-mobility regime enables large power factors in half-Heuslers, well above the maximum measured values. We anticipate that our understanding will spark new routes to search for better thermoelectric materials, and to discover high electron mobility semiconductors for electronic and photonic applications.},
doi = {10.1038/s41467-018-03866-w},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {4}
}

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

Citation Metrics:
Cited by: 30 works
Citation information provided by
Web of Science

Figures / Tables:

Fig. 1 Fig. 1: Electron–phonon interaction and deformation potential. a, b Electron–phonon coupling matrix along high-symmetry lines. The coupling matrices are calculated along two different directions in the Brillouin zone for a longitudinal acoustic phonons and b optical phonons, respectively, with the initial electron state located at the conduction band edge (kXmore » = (0, 0, 2$π$/$a$), where $α$ is the lattice constant) and the final electron in the same band (intra-band coupling). The insets in a and b illustrate the lattice distortions corresponding to acoustic and optical phonons. c, d Averaged deformation potential for acoustic and optical phonons. The deformation potentials are extracted as the slopes from a, b, for the two different directions (one is parallel with kX while the other is perpendicular), defined as $Ξ$ and $Ξ$. The deformation potential generally depends on the directional angle of the phonon state, but for simplicity we calculate averaged deformation potential defined as $\bar{Ξ}$ = $Ξ ^{1/3}_{∥}$$Ξ ^{2/3}_{⟂}$« less

Save / Share:

Works referenced in this record:

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

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

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009

  • Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
  • Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
  • DOI: 10.1088/0953-8984/21/39/395502

The intrinsic disorder related alloy scattering in ZrNiSn half-Heusler thermoelectric materials
journal, November 2014

  • Xie, Hanhui; Wang, Heng; Fu, Chenguang
  • Scientific Reports, Vol. 4, Issue 1
  • DOI: 10.1038/srep06888

Recent progress of half-Heusler for moderate temperature thermoelectric applications
journal, October 2013


EPW: A program for calculating the electron–phonon coupling using maximally localized Wannier functions
journal, December 2010

  • Noffsinger, Jesse; Giustino, Feliciano; Malone, Brad D.
  • Computer Physics Communications, Vol. 181, Issue 12, p. 2140-2148
  • DOI: 10.1016/j.cpc.2010.08.027

Convergence of multi-valley bands as the electronic origin of high thermoelectric performance in CoSb3 skutterudites
journal, October 2015

  • Tang, Yinglu; Gibbs, Zachary M.; Agapito, Luis A.
  • Nature Materials, Vol. 14, Issue 12
  • DOI: 10.1038/nmat4430

Connecting Thermoelectric Performance and Topological-Insulator Behavior: Bi 2 Te 3 and Bi 2 Te 2 Se from First Principles
journal, January 2015


Deformation Potentials and Mobilities in Non-Polar Crystals
journal, October 1950


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

Enhancement of Thermoelectric Efficiency in PbTe by Distortion of the Electronic Density of States
journal, July 2008

  • Heremans, J. P.; Jovovic, V.; Toberer, E. S.
  • Science, Vol. 321, Issue 5888, p. 554-557
  • DOI: 10.1126/science.1159725

Achieving high power factor and output power density in p-type half-Heuslers Nb 1-x Ti x FeSb
journal, November 2016

  • He, Ran; Kraemer, Daniel; Mao, Jun
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 48
  • DOI: 10.1073/pnas.1617663113

Prediction and accelerated laboratory discovery of previously unknown 18-electron ABX compounds
journal, March 2015

  • Gautier, Romain; Zhang, Xiuwen; Hu, Linhua
  • Nature Chemistry, Vol. 7, Issue 4
  • DOI: 10.1038/nchem.2207

Crystal orbital Hamilton populations (COHP): energy-resolved visualization of chemical bonding in solids based on density-functional calculations
journal, August 1993

  • Dronskowski, Richard; Bloechl, Peter E.
  • The Journal of Physical Chemistry, Vol. 97, Issue 33
  • DOI: 10.1021/j100135a014

High-performance bulk thermoelectrics with all-scale hierarchical architectures
journal, September 2012

  • Biswas, Kanishka; He, Jiaqing; Blum, Ivan D.
  • Nature, Vol. 489, Issue 7416, p. 414-418
  • DOI: 10.1038/nature11439

Evaluation of Half-Heusler Compounds as Thermoelectric Materials Based on the Calculated Electrical Transport Properties
journal, October 2008

  • Yang, Jiong; Li, Huanming; Wu, Ting
  • Advanced Functional Materials, Vol. 18, Issue 19, p. 2880-2888
  • DOI: 10.1002/adfm.200701369

Wannier interpolation of the electron-phonon matrix elements in polar semiconductors: Polar-optical coupling in GaAs
journal, August 2015


New trends, strategies and opportunities in thermoelectric materials: A perspective
journal, June 2017


Fröhlich Electron-Phonon Vertex from First Principles
journal, October 2015


Electron Transport in InSb, InAs, and InP
journal, May 1971


Engineering half-Heusler thermoelectric materials using Zintl chemistry
journal, May 2016

  • Zeier, Wolfgang G.; Schmitt, Jennifer; Hautier, Geoffroy
  • Nature Reviews Materials, Vol. 1, Issue 6
  • DOI: 10.1038/natrevmats.2016.32

Electron-phonon interactions from first principles
journal, February 2017


Large Seebeck effect by charge-mobility engineering
journal, June 2015

  • Sun, Peijie; Wei, Beipei; Zhang, Jiahao
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8475

Charge Transport in Organic Semiconductors
journal, April 2007

  • Coropceanu, Veaceslav; Cornil, Jérôme; da Silva Filho, Demetrio A.
  • Chemical Reviews, Vol. 107, Issue 4
  • DOI: 10.1021/cr050140x

Enhanced thermoelectric performance of rough silicon nanowires
journal, January 2008

  • Hochbaum, Allon I.; Chen, Renkun; Delgado, Raul Diaz
  • Nature, Vol. 451, Issue 7175, p. 163-167
  • DOI: 10.1038/nature06381

Theory of Superconductivity
journal, December 1957


Thermoelectric Properties of Half-Heusler Bismuthides ZrCo1−x Ni x Bi (x = 0.0 to 0.1)
journal, June 2007

  • Ponnambalam, V.; Zhang, Bo; Tritt, Terry M.
  • Journal of Electronic Materials, Vol. 36, Issue 7
  • DOI: 10.1007/s11664-007-0153-1

Cooling, Heating, Generating Power, and Recovering Waste Heat with Thermoelectric Systems
journal, September 2008


The rise of graphene
journal, March 2007

  • Geim, A. K.; Novoselov, K. S.
  • Nature Materials, Vol. 6, Issue 3, p. 183-191
  • DOI: 10.1038/nmat1849

Experimental Realization of a Three-Dimensional Dirac Semimetal
journal, July 2014


Acoustic deformation potentials and heterostructure band offsets in semiconductors
journal, April 1987


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


Doping and temperature dependence of thermoelectric properties in Mg 2 (Si,Sn)
journal, October 2012


A stable three-dimensional topological Dirac semimetal Cd3As2
journal, May 2014

  • Liu, Z. K.; Jiang, J.; Zhou, B.
  • Nature Materials, Vol. 13, Issue 7
  • DOI: 10.1038/nmat3990

The rise of graphene
book, August 2009

  • Rodgers, Peter; Geim, A. K.; Novoselov, K. S.
  • Nanoscience and Technology: A Collection of Reviews from Nature Journals, p. 11-19
  • DOI: 10.1142/9789814287005_0002

    Works referencing / citing this record:

    The rise of graphene
    journal, March 2007

    • Geim, A. K.; Novoselov, K. S.
    • Nature Materials, Vol. 6, Issue 3, p. 183-191
    • DOI: 10.1038/nmat1849

    Cooling, Heating, Generating Power, and Recovering Waste Heat with Thermoelectric Systems
    journal, September 2008


    Electron-phonon interactions from first principles
    journal, February 2017


    Wannier interpolation of the electron-phonon matrix elements in polar semiconductors: Polar-optical coupling in GaAs
    journal, August 2015


    Convergence of multi-valley bands as the electronic origin of high thermoelectric performance in CoSb3 skutterudites
    journal, October 2015

    • Tang, Yinglu; Gibbs, Zachary M.; Agapito, Luis A.
    • Nature Materials, Vol. 14, Issue 12
    • DOI: 10.1038/nmat4430

    The intrinsic disorder related alloy scattering in ZrNiSn half-Heusler thermoelectric materials
    journal, November 2014

    • Xie, Hanhui; Wang, Heng; Fu, Chenguang
    • Scientific Reports, Vol. 4, Issue 1
    • DOI: 10.1038/srep06888

    High-performance bulk thermoelectrics with all-scale hierarchical architectures
    journal, September 2012

    • Biswas, Kanishka; He, Jiaqing; Blum, Ivan D.
    • Nature, Vol. 489, Issue 7416, p. 414-418
    • DOI: 10.1038/nature11439

    Electron Transport in InSb, InAs, and InP
    journal, May 1971


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


    Charge Transport in Organic Semiconductors
    journal, April 2007

    • Coropceanu, Veaceslav; Cornil, Jérôme; da Silva Filho, Demetrio A.
    • Chemical Reviews, Vol. 107, Issue 4
    • DOI: 10.1021/cr050140x

    A stable three-dimensional topological Dirac semimetal Cd3As2
    journal, May 2014

    • Liu, Z. K.; Jiang, J.; Zhou, B.
    • Nature Materials, Vol. 13, Issue 7
    • DOI: 10.1038/nmat3990

    Fröhlich Electron-Phonon Vertex from First Principles
    journal, October 2015


    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

    Theory of Superconductivity
    journal, December 1957


    EPW: A program for calculating the electron–phonon coupling using maximally localized Wannier functions
    journal, December 2010

    • Noffsinger, Jesse; Giustino, Feliciano; Malone, Brad D.
    • Computer Physics Communications, Vol. 181, Issue 12, p. 2140-2148
    • DOI: 10.1016/j.cpc.2010.08.027

    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

    Connecting Thermoelectric Performance and Topological-Insulator Behavior: Bi 2 Te 3 and Bi 2 Te 2 Se from First Principles
    journal, January 2015


    Evaluation of Half-Heusler Compounds as Thermoelectric Materials Based on the Calculated Electrical Transport Properties
    journal, October 2008

    • Yang, Jiong; Li, Huanming; Wu, Ting
    • Advanced Functional Materials, Vol. 18, Issue 19, p. 2880-2888
    • DOI: 10.1002/adfm.200701369

    Enhancement of Thermoelectric Efficiency in PbTe by Distortion of the Electronic Density of States
    journal, July 2008

    • Heremans, J. P.; Jovovic, V.; Toberer, E. S.
    • Science, Vol. 321, Issue 5888, p. 554-557
    • DOI: 10.1126/science.1159725

    Crystal orbital Hamilton populations (COHP): energy-resolved visualization of chemical bonding in solids based on density-functional calculations
    journal, August 1993

    • Dronskowski, Richard; Bloechl, Peter E.
    • The Journal of Physical Chemistry, Vol. 97, Issue 33
    • DOI: 10.1021/j100135a014

    Prediction and accelerated laboratory discovery of previously unknown 18-electron ABX compounds
    journal, March 2015

    • Gautier, Romain; Zhang, Xiuwen; Hu, Linhua
    • Nature Chemistry, Vol. 7, Issue 4
    • DOI: 10.1038/nchem.2207

    Recent progress of half-Heusler for moderate temperature thermoelectric applications
    journal, October 2013


    Doping and temperature dependence of thermoelectric properties in Mg 2 (Si,Sn)
    journal, October 2012


    Thermoelectric Properties of Half-Heusler Bismuthides ZrCo1−x Ni x Bi (x = 0.0 to 0.1)
    journal, June 2007

    • Ponnambalam, V.; Zhang, Bo; Tritt, Terry M.
    • Journal of Electronic Materials, Vol. 36, Issue 7
    • DOI: 10.1007/s11664-007-0153-1

    Engineering half-Heusler thermoelectric materials using Zintl chemistry
    journal, May 2016

    • Zeier, Wolfgang G.; Schmitt, Jennifer; Hautier, Geoffroy
    • Nature Reviews Materials, Vol. 1, Issue 6
    • DOI: 10.1038/natrevmats.2016.32

    Deformation Potentials and Mobilities in Non-Polar Crystals
    journal, October 1950


    Achieving high power factor and output power density in p-type half-Heuslers Nb 1-x Ti x FeSb
    journal, November 2016

    • He, Ran; Kraemer, Daniel; Mao, Jun
    • Proceedings of the National Academy of Sciences, Vol. 113, Issue 48
    • DOI: 10.1073/pnas.1617663113

    Large Seebeck effect by charge-mobility engineering
    journal, June 2015

    • Sun, Peijie; Wei, Beipei; Zhang, Jiahao
    • Nature Communications, Vol. 6, Issue 1
    • DOI: 10.1038/ncomms8475

    New trends, strategies and opportunities in thermoelectric materials: A perspective
    journal, June 2017


    Experimental Realization of a Three-Dimensional Dirac Semimetal
    journal, July 2014


    Enhanced thermoelectric performance of rough silicon nanowires
    journal, January 2008

    • Hochbaum, Allon I.; Chen, Renkun; Delgado, Raul Diaz
    • Nature, Vol. 451, Issue 7175, p. 163-167
    • DOI: 10.1038/nature06381

    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

    QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
    journal, September 2009

    • Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
    • Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
    • DOI: 10.1088/0953-8984/21/39/395502

    Acoustic deformation potentials and heterostructure band offsets in semiconductors
    journal, April 1987


    Simultaneously high electron and hole mobilities in cubic boron-V compounds: BP, BAs, and BSb
    journal, August 2018


    Fiber‐Based Energy Conversion Devices for Human‐Body Energy Harvesting
    journal, June 2019


    2D Single‐Layer π‐Conjugated Nickel Bis(dithiolene) Complex: A Good‐Electron‐Poor‐Phonon Thermoelectric Material
    journal, March 2019

    • Deng, Tianqi; Yong, Xue; Shi, Wen
    • Advanced Electronic Materials, Vol. 5, Issue 4
    • DOI: 10.1002/aelm.201800892

    Manipulation of Ni Interstitials for Realizing Large Power Factor in TiNiSn‐Based Materials
    journal, May 2019

    • Ren, Wuyang; Zhu, Hangtian; Mao, Jun
    • Advanced Electronic Materials, Vol. 5, Issue 7
    • DOI: 10.1002/aelm.201900166

    Discovery of TaFeSb-based half-Heuslers with high thermoelectric performance
    journal, January 2019


    Designing chemical analogs to PbTe with intrinsic high band degeneracy and low lattice thermal conductivity
    journal, February 2019


    Inertial effective mass as an effective descriptor for thermoelectrics via data-driven evaluation
    journal, January 2019

    • Suwardi, Ady; Bash, Daniil; Ng, Hong Kuan
    • Journal of Materials Chemistry A, Vol. 7, Issue 41
    • DOI: 10.1039/c9ta05967a

    Atomistic study of an ideal metal/thermoelectric contact: The full-Heusler/half-Heusler interface
    journal, January 2019

    • Spataru, Catalin D.; He, Yuping; Léonard, François
    • APL Materials, Vol. 7, Issue 1
    • DOI: 10.1063/1.5052271

    Impact of the scattering physics on the power factor of complex thermoelectric materials
    journal, October 2019

    • Graziosi, Patrizio; Kumarasinghe, Chathurangi; Neophytou, Neophytos
    • Journal of Applied Physics, Vol. 126, Issue 15
    • DOI: 10.1063/1.5116793

    Thermoelectric transport trends in group 4 half-Heusler alloys
    journal, October 2019

    • Berland, Kristian; Shulumba, Nina; Hellman, Olle
    • Journal of Applied Physics, Vol. 126, Issue 14
    • DOI: 10.1063/1.5117288

    Advances in thermoelectrics
    journal, April 2018


    Half Heusler compounds: promising materials for mid-to-high temperature thermoelectric conversion
    journal, September 2019


    Leveraging electron-phonon interaction to enhance the thermoelectric power factor in graphene-like semimetals
    journal, November 2019


    Characterization of rattling in relation to thermal conductivity: Ordered half-Heusler semiconductors
    journal, February 2020


    Phase Boundary Mapping in ZrNiSn Half-Heusler for Enhanced Thermoelectric Performance
    journal, January 2020


      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.