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Title: Ab initio optimization of phonon drag effect for lower-temperature thermoelectric energy conversion

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
 [1];  [1];  [1];  [1];  [2];  [1];  [1]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  2. Rutgers Univ., Piscataway, NJ (United States)

Although the thermoelectric figure of merit zT above 300 K has seen significant improvement recently, the progress at lower temperatures has been slow, mainly limited by the relatively low Seebeck coefficient and high thermal conductivity. We report, for the first time to our knowledge, success in first-principles computation of the phonon drag effect—a coupling phenomenon between electrons and nonequilibrium phonons—in heavily doped region and its optimization to enhance the Seebeck coefficient while reducing the phonon thermal conductivity by nanostructuring. Our simulation quantitatively identifies the major phonons contributing to the phonon drag, which are spectrally distinct from those carrying heat, and further reveals that although the phonon drag is reduced in heavily doped samples, a significant contribution to Seebeck coefficient still exists. An ideal phonon filter is proposed to enhance zT of silicon at room temperature by a factor of 20 to ~0.25, and the enhancement can reach 70 times at 100 K. This work opens up a new venue toward better thermoelectrics by harnessing nonequilibrium phonons.

Research Organization:
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Energy Frontier Research Centers (EFRC) (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0001299; FG02-09ER46577; SC0001299/DE-FG02-09ER46577
OSTI ID:
1235174
Alternate ID(s):
OSTI ID: 1370969
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Vol. 112, Issue 48; ISSN 0027-8424
Publisher:
National Academy of SciencesCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 65 works
Citation information provided by
Web of Science

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First-principles dynamics of electrons and phonons* journal November 2016
TiO2–SrTiO3 Biphase Nanoceramics as Advanced Thermoelectric Materials journal September 2019
Towards predictive many-body calculations of phonon-limited carrier mobilities in semiconductors text January 2018
Leveraging Electron-Phonon Interaction to Enhance Thermoelectric Power Factor in Graphene-Like Semimetals text January 2019
A comparative study of low energy radiation response of AlAs, GaAs and GaAs/AlAs superlattice and the damage effects on their electronic structures journal January 2018