Soft anharmonic phonons and ultralow thermal conductivity in Mg 3 (Sb, Bi) 2 thermoelectrics
Abstract
The candidate thermoelectric compounds Mg3Sb2 and Mg3Bi2 show excellent performance near ambient temperature, enabled by an anomalously low lattice thermal conductivity (κl) comparable to those of much heavier PbTe or Bi2Te3. Contrary to common mass-trend expectations, replacing Mg with heavier Ca or Yb yields a threefold increase in κl in CaMg2Sb2 and YbMg2Bi2. Here, we report a comprehensive analysis of phonons in the series AMg2X2 (A= Mg, Ca, and Yb; X= Bi and Sb) based on inelastic neutron/x-ray scattering and first-principles simulations and show that the anomalously low κl of Mg3X2 has inherent phononic origins. We uncover a large phonon softening and flattening of low-energy transverse acoustic phonons in Mg3X2 compared to the ternary analogs and traced to a specific Mg-X bond, which markedly enlarges the scattering phase-space, enabling the threefold tuning in κl. These results provide key insights for manipulating phonon scattering without the traditional reliance on heavy elements.
- Authors:
-
[1];
[1];
[2];
[3];
[4];
- Department of Mechanical Engineering and Materials Science, Duke University, Durham, NC 27708, USA.
- Department of Chemical Engineering and Materials Science, Michigan State University, East Lansing, MI 48910, USA.
- Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA., Department of Physics and Astronomy, Purdue University, West Lafayette, IN 47906, USA.
- Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
- Advanced Photon Source, Argonne National Laboratory, Lemont, IL 60439, USA.
- Department of Mechanical Engineering and Materials Science, Duke University, Durham, NC 27708, USA., Department of Chemistry, Duke University, Durham, NC 27708, USA., Department of Physics, Duke University, Durham, NC 27708, USA.
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Michigan State Univ., East Lansing, MI (United States); Duke Univ., Durham, NC (United States)
- Sponsoring Org.:
- USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
- OSTI Identifier:
- 1784376
- Alternate Identifier(s):
- OSTI ID: 1815419
- Grant/Contract Number:
- SC0019299; SC0019252; AC02-05CH11231; AC02-06CH11357
- Resource Type:
- Published Article
- Journal Name:
- Science Advances
- Additional Journal Information:
- Journal Name: Science Advances Journal Volume: 7 Journal Issue: 21; Journal ID: ISSN 2375-2548
- Publisher:
- American Association for the Advancement of Science (AAAS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Ding, Jingxuan, Lanigan-Atkins, Tyson, Calderón-Cueva, Mario, Banerjee, Arnab, Abernathy, Douglas L., Said, Ayman, Zevalkink, Alexandra, and Delaire, Olivier. Soft anharmonic phonons and ultralow thermal conductivity in Mg 3 (Sb, Bi) 2 thermoelectrics. United States: N. p., 2021.
Web. doi:10.1126/sciadv.abg1449.
Ding, Jingxuan, Lanigan-Atkins, Tyson, Calderón-Cueva, Mario, Banerjee, Arnab, Abernathy, Douglas L., Said, Ayman, Zevalkink, Alexandra, & Delaire, Olivier. Soft anharmonic phonons and ultralow thermal conductivity in Mg 3 (Sb, Bi) 2 thermoelectrics. United States. https://doi.org/10.1126/sciadv.abg1449
Ding, Jingxuan, Lanigan-Atkins, Tyson, Calderón-Cueva, Mario, Banerjee, Arnab, Abernathy, Douglas L., Said, Ayman, Zevalkink, Alexandra, and Delaire, Olivier. Fri .
"Soft anharmonic phonons and ultralow thermal conductivity in Mg 3 (Sb, Bi) 2 thermoelectrics". United States. https://doi.org/10.1126/sciadv.abg1449.
@article{osti_1784376,
title = {Soft anharmonic phonons and ultralow thermal conductivity in Mg 3 (Sb, Bi) 2 thermoelectrics},
author = {Ding, Jingxuan and Lanigan-Atkins, Tyson and Calderón-Cueva, Mario and Banerjee, Arnab and Abernathy, Douglas L. and Said, Ayman and Zevalkink, Alexandra and Delaire, Olivier},
abstractNote = {The candidate thermoelectric compounds Mg3Sb2 and Mg3Bi2 show excellent performance near ambient temperature, enabled by an anomalously low lattice thermal conductivity (κl) comparable to those of much heavier PbTe or Bi2Te3. Contrary to common mass-trend expectations, replacing Mg with heavier Ca or Yb yields a threefold increase in κl in CaMg2Sb2 and YbMg2Bi2. Here, we report a comprehensive analysis of phonons in the series AMg2X2 (A= Mg, Ca, and Yb; X= Bi and Sb) based on inelastic neutron/x-ray scattering and first-principles simulations and show that the anomalously low κl of Mg3X2 has inherent phononic origins. We uncover a large phonon softening and flattening of low-energy transverse acoustic phonons in Mg3X2 compared to the ternary analogs and traced to a specific Mg-X bond, which markedly enlarges the scattering phase-space, enabling the threefold tuning in κl. These results provide key insights for manipulating phonon scattering without the traditional reliance on heavy elements.},
doi = {10.1126/sciadv.abg1449},
journal = {Science Advances},
number = 21,
volume = 7,
place = {United States},
year = {Fri May 21 00:00:00 EDT 2021},
month = {Fri May 21 00:00:00 EDT 2021}
}
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