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

Title: Manipulation of ionized impurity scattering for achieving high thermoelectric performance in n-type Mg 3 Sb 2 -based materials

Abstract

Achieving higher carrier mobility plays a pivotal role for obtaining potentially high thermoelectric performance. In principle, the carrier mobility is governed by the band structure as well as by the carrier scattering mechanism. Here, we demonstrate that by manipulating the carrier scattering mechanism in n-type Mg 3Sb 2-based materials, a substantial improvement in carrier mobility, and hence the power factor, can be achieved. In this work, Fe, Co, Hf, and Ta are doped on the Mg site of Mg 3.2Sb 1.5Bi 0.49Te 0.01, where the ionized impurity scattering crosses over to mixed ionized impurity and acoustic phonon scattering. A significant improvement in Hall mobility from ~16 to ~81 cm 2∙V -1∙s -1 is obtained, thus leading to a notably enhanced power factor of ~13 μW∙cm -1∙K -2 from ~5 μW∙cm -1∙K -2. A simultaneous reduction in thermal conductivity is also achieved. Collectively, a figure of merit ( ZT) of ~1.7 is obtained at 773 K in Mg 3.1Co 0.1Sb 1.5Bi 0.49Te 0.01. The concept of manipulating the carrier scattering mechanism to improve the mobility should also be applicable to other material systems.

Authors:
; ; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC), Washington D.C. (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1392688
Alternate Identifier(s):
OSTI ID: 1470514
Grant/Contract Number:  
SC0001299; FG02-09ER46577
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 114 Journal Issue: 40; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 36 MATERIALS SCIENCE; 42 ENGINEERING; solar (photovoltaic); solar (thermal); solid state lighting; phonons; thermal conductivity, thermoelectric; defects; mechanical behavior; charge transport; spin dynamics; materials and chemistry by design; optics; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing); thermoelectric; carrier scattering mechanism; ionized impurity scattering; n-types Mg3Sb2

Citation Formats

Mao, Jun, Shuai, Jing, Song, Shaowei, Wu, Yixuan, Dally, Rebecca, Zhou, Jiawei, Liu, Zihang, Sun, Jifeng, Zhang, Qinyong, dela Cruz, Clarina, Wilson, Stephen, Pei, Yanzhong, Singh, David J., Chen, Gang, Chu, Ching-Wu, and Ren, Zhifeng. Manipulation of ionized impurity scattering for achieving high thermoelectric performance in n-type Mg 3 Sb 2 -based materials. United States: N. p., 2017. Web. doi:10.1073/pnas.1711725114.
Mao, Jun, Shuai, Jing, Song, Shaowei, Wu, Yixuan, Dally, Rebecca, Zhou, Jiawei, Liu, Zihang, Sun, Jifeng, Zhang, Qinyong, dela Cruz, Clarina, Wilson, Stephen, Pei, Yanzhong, Singh, David J., Chen, Gang, Chu, Ching-Wu, & Ren, Zhifeng. Manipulation of ionized impurity scattering for achieving high thermoelectric performance in n-type Mg 3 Sb 2 -based materials. United States. doi:10.1073/pnas.1711725114.
Mao, Jun, Shuai, Jing, Song, Shaowei, Wu, Yixuan, Dally, Rebecca, Zhou, Jiawei, Liu, Zihang, Sun, Jifeng, Zhang, Qinyong, dela Cruz, Clarina, Wilson, Stephen, Pei, Yanzhong, Singh, David J., Chen, Gang, Chu, Ching-Wu, and Ren, Zhifeng. Mon . "Manipulation of ionized impurity scattering for achieving high thermoelectric performance in n-type Mg 3 Sb 2 -based materials". United States. doi:10.1073/pnas.1711725114.
@article{osti_1392688,
title = {Manipulation of ionized impurity scattering for achieving high thermoelectric performance in n-type Mg 3 Sb 2 -based materials},
author = {Mao, Jun and Shuai, Jing and Song, Shaowei and Wu, Yixuan and Dally, Rebecca and Zhou, Jiawei and Liu, Zihang and Sun, Jifeng and Zhang, Qinyong and dela Cruz, Clarina and Wilson, Stephen and Pei, Yanzhong and Singh, David J. and Chen, Gang and Chu, Ching-Wu and Ren, Zhifeng},
abstractNote = {Achieving higher carrier mobility plays a pivotal role for obtaining potentially high thermoelectric performance. In principle, the carrier mobility is governed by the band structure as well as by the carrier scattering mechanism. Here, we demonstrate that by manipulating the carrier scattering mechanism in n-type Mg3Sb2-based materials, a substantial improvement in carrier mobility, and hence the power factor, can be achieved. In this work, Fe, Co, Hf, and Ta are doped on the Mg site of Mg3.2Sb1.5Bi0.49Te0.01, where the ionized impurity scattering crosses over to mixed ionized impurity and acoustic phonon scattering. A significant improvement in Hall mobility from ~16 to ~81 cm2∙V-1∙s-1 is obtained, thus leading to a notably enhanced power factor of ~13 μW∙cm-1∙K-2 from ~5 μW∙cm-1∙K-2. A simultaneous reduction in thermal conductivity is also achieved. Collectively, a figure of merit (ZT) of ~1.7 is obtained at 773 K in Mg3.1Co0.1Sb1.5Bi0.49Te0.01. The concept of manipulating the carrier scattering mechanism to improve the mobility should also be applicable to other material systems.},
doi = {10.1073/pnas.1711725114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 40,
volume = 114,
place = {United States},
year = {2017},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1073/pnas.1711725114

Citation Metrics:
Cited by: 39 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Electron-Electron Scattering in Ti S 2
journal, December 1975


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

Improvement of dielectric loss tangent of Al2O3 doped Ba0.5Sr0.5TiO3 thin films for tunable microwave devices
journal, February 2004

  • Chong, K. B.; Kong, L. B.; Chen, Linfeng
  • Journal of Applied Physics, Vol. 95, Issue 3
  • DOI: 10.1063/1.1638615

Power Factor Enhancement by Modulation Doping in Bulk Nanocomposites
journal, June 2011

  • Zebarjadi, Mona; Joshi, Giri; Zhu, Gaohua
  • Nano Letters, Vol. 11, Issue 6
  • DOI: 10.1021/nl201206d

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

Thermal and Electrical Properties of Heavily Doped Ge‐Si Alloys up to 1300°K
journal, October 1964

  • Dismukes, J. P.; Ekstrom, L.; Steigmeier, E. F.
  • Journal of Applied Physics, Vol. 35, Issue 10
  • DOI: 10.1063/1.1713126

On Intensifying Carrier Impurity Scattering to Enhance Thermoelectric Performance in Cr-Doped Ce y Co 4 Sb 12
journal, October 2015

  • Wang, Shanyu; Yang, Jiong; Wu, Lihua
  • Advanced Functional Materials, Vol. 25, Issue 42
  • DOI: 10.1002/adfm.201502782

Thermal equilibrium concentrations and effects of negatively charged Ga vacancies in n-type GaAs
journal, March 1993

  • Tan, T. Y.; You, H. -M.; G�sele, U. M.
  • Applied Physics A Solids and Surfaces, Vol. 56, Issue 3
  • DOI: 10.1007/BF00539483

Ionized-Impurity Scattering Mobility of Electrons in Silicon
journal, September 1959


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

Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993


Strain field fluctuation effects on lattice thermal conductivity of ZrNiSn-based thermoelectric compounds
journal, August 2004

  • Yang, J.; Meisner, G. P.; Chen, L.
  • Applied Physics Letters, Vol. 85, Issue 7
  • DOI: 10.1063/1.1783022

Optimized Thermoelectric Properties of Sb-Doped Mg 2(1+ z ) Si 0.5– y Sn 0.5 Sb y through Adjustment of the Mg Content
journal, December 2011

  • Liu, Wei; Tang, Xinfeng; Li, Han
  • Chemistry of Materials, Vol. 23, Issue 23
  • DOI: 10.1021/cm202445d

Dielectric constant enhancement due to Si incorporation into HfO2
journal, October 2006

  • Tomida, Kazuyuki; Kita, Koji; Toriumi, Akira
  • Applied Physics Letters, Vol. 89, Issue 14
  • DOI: 10.1063/1.2355471

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

Band Engineering of Thermoelectric Materials
journal, October 2012


Size effect in thermoelectric materials
journal, December 2016


Lattice Dislocations Enhancing Thermoelectric PbTe in Addition to Band Convergence
journal, April 2017


Convergence of Conduction Bands as a Means of Enhancing Thermoelectric Performance of n -Type Mg 2 Si 1 x Sn x Solid Solutions
journal, April 2012


Thermoelectric Cooling and Power Generation
journal, July 1999


Enhanced Thermoelectric Properties in the Counter-Doped SnTe System with Strained Endotaxial SrTe
journal, February 2016

  • Zhao, Li-Dong; Zhang, Xiao; Wu, Haijun
  • Journal of the American Chemical Society, Vol. 138, Issue 7
  • DOI: 10.1021/jacs.5b13276

Grain Boundary Engineering for Achieving High Thermoelectric Performance in n-Type Skutterudites
journal, February 2017


Relationship between thermoelectric figure of merit and energy conversion efficiency
journal, June 2015

  • Kim, Hee Seok; Liu, Weishu; Chen, Gang
  • Proceedings of the National Academy of Sciences, Vol. 112, Issue 27
  • DOI: 10.1073/pnas.1510231112

Preparation of sintered degenerate n -type PbTe with a small grain size and its thermoelectric properties
journal, September 2002

  • Kishimoto, Kengo; Koyanagi, Tsuyoshi
  • Journal of Applied Physics, Vol. 92, Issue 5
  • DOI: 10.1063/1.1499206

The effect of Cr2O3, Nb2O5 and ZrO2 doping on the dielectric properties of CaCu3Ti4O12
journal, February 2008


Tuning the carrier scattering mechanism to effectively improve the thermoelectric properties
journal, January 2017

  • Shuai, Jing; Mao, Jun; Song, Shaowei
  • Energy & Environmental Science, Vol. 10, Issue 3
  • DOI: 10.1039/C7EE00098G

Point defect thermal equilibria in GaAs
journal, November 1991


Charged point defects in semiconductors
journal, December 2006

  • Seebauer, Edmund G.; Kratzer, Meredith C.
  • Materials Science and Engineering: R: Reports, Vol. 55, Issue 3-6
  • DOI: 10.1016/j.mser.2006.01.002

Discovery of high-performance low-cost n-type Mg3Sb2-based thermoelectric materials with multi-valley conduction bands
journal, January 2017

  • Zhang, Jiawei; Song, Lirong; Pedersen, Steffen Hindborg
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms13901

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


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


Thermoelectric Properties of n-type ZrNiPb-Based Half-Heuslers
journal, January 2017


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


Giant Dielectric Permittivity Observed in Li and Ti Doped NiO
journal, October 2002


Vacancy-induced dislocations within grains for high-performance PbSe thermoelectrics
journal, January 2017

  • Chen, Zhiwei; Ge, Binghui; Li, Wen
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms13828

Electron scattering by ionized impurities in semiconductors
journal, October 1981


Isotropic Conduction Network and Defect Chemistry in Mg 3+ δ Sb 2 -Based Layered Zintl Compounds with High Thermoelectric Performance
journal, September 2016

  • Tamaki, Hiromasa; Sato, Hiroki K.; Kanno, Tsutomu
  • Advanced Materials, Vol. 28, Issue 46
  • DOI: 10.1002/adma.201603955

Electrical Properties of N -Type Germanium
journal, February 1954


Dislocation strain as the mechanism of phonon scattering at grain boundaries
journal, January 2016

  • Kim, Hyun-Sik; Kang, Stephen D.; Tang, Yinglu
  • Materials Horizons, Vol. 3, Issue 3
  • DOI: 10.1039/C5MH00299K

Improvement of the Efficiency of Thermoelectric Energy Conversion by Utilizing Potential Barriers
journal, January 1997

  • Nishio, Yoshimasa; Hirano, Tohru
  • Japanese Journal of Applied Physics, Vol. 36, Issue Part 1, No. 1A
  • DOI: 10.1143/JJAP.36.170

Band engineering of high performance p-type FeNbSb based half-Heusler thermoelectric materials for figure of merit zT > 1
journal, January 2015

  • Fu, Chenguang; Zhu, Tiejun; Liu, Yintu
  • Energy & Environmental Science, Vol. 8, Issue 1
  • DOI: 10.1039/C4EE03042G

Enhancement of Thermoelectric Properties by Modulation-Doping in Silicon Germanium Alloy Nanocomposites
journal, January 2012

  • Yu, Bo; Zebarjadi, Mona; Wang, Hui
  • Nano Letters, Vol. 12, Issue 4, p. 2077-2082
  • DOI: 10.1021/nl3003045

On the tuning of electrical and thermal transport in thermoelectrics: an integrated theory–experiment perspective
journal, February 2016


Phonon scattering by nanoscale twin boundaries
journal, February 2017


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


Temperature Dependence of the Low-Field Galvanomagnetic Coefficients of Bismuth
journal, May 1969


Amorphous lanthanide-doped TiOx dielectric films
journal, May 1999

  • van Dover, R. B.
  • Applied Physics Letters, Vol. 74, Issue 20
  • DOI: 10.1063/1.124058

Mg-doped Ba0.6Sr0.4TiO3 thin films for tunable microwave applications
journal, July 2000

  • Joshi, P. C.; Cole, M. W.
  • Applied Physics Letters, Vol. 77, Issue 2
  • DOI: 10.1063/1.126953

Synthesis and characterization of nano-sized pure and Al-doped lithium ferrite having high value of dielectric constant
journal, March 2010


    Works referencing / citing this record:

    Improvement of Low‐Temperature zT in a Mg 3 Sb 2 –Mg 3 Bi 2 Solid Solution via Mg‐Vapor Annealing
    journal, July 2019

    • Wood, Maxwell; Kuo, Jimmy Jiahong; Imasato, Kazuki
    • Advanced Materials, Vol. 31, Issue 35
    • DOI: 10.1002/adma.201902337

    Extraordinary n‐Type Mg 3 SbBi Thermoelectrics Enabled by Yttrium Doping
    journal, June 2019

    • Shi, Xuemin; Zhao, Tingting; Zhang, Xinyue
    • Advanced Materials, Vol. 31, Issue 36
    • DOI: 10.1002/adma.201903387

    Multiscale Defects as Strong Phonon Scatters to Enhance Thermoelectric Performance in Mg 2 Sn 1– x Sb x Solid Solutions
    journal, July 2019


    Insights into the design of thermoelectric Mg3Sb2 and its analogs by combining theory and experiment
    journal, July 2019

    • Zhang, Jiawei; Song, Lirong; Iversen, Bo Brummerstedt
    • npj Computational Materials, Vol. 5, Issue 1
    • DOI: 10.1038/s41524-019-0215-y

    Understanding the asymmetrical thermoelectric performance for discovering promising thermoelectric materials
    journal, June 2019


    Flexible Organic Thermoelectric Materials and Devices for Wearable Green Energy Harvesting
    journal, May 2019