Intrinsic ultralow lattice thermal conductivity of the unfilled skutterudite
Abstract
It is generally accepted that unfilled skutterudites process high lattice thermal conductivity $$κ_l$$ that can be efficiently reduced upon filling. Here by using first-principles Boltzmann-Peierls transport calculations, we find pure skutterudite of with no filler in fact has an intrinsic ultralow $$κ_l$$ smaller than that of by one order of magnitude. The value is even smaller than those of most of the fully filled skutterudites. This finding means that with as a reference, filling does not necessarily lower $$κ_l$$. The ultralow $$κ_l$$ of is a consequence of the overall softening of phonon spectrum, especially the lowering in frequency of optical phonon branches associated with the weakly bonded rings. They overlap more with heat-carrying acoustic phonons and significantly increase the phase space for three-phonon anharmonic scattering processes. This provides an alternative non-filling-related mechanism for lowering the $$κ_l$$ of skutterudites.
- Authors:
-
- Jilin Univ., Changchun (China)
- Univ. of Missouri, Columbia, MO (United States)
- Shenzhen Univ., Shenzhen (China)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1388448
- Alternate Identifier(s):
- OSTI ID: 1290316
- Grant/Contract Number:
- SC0001299; FG02-09ER46577; SC0001299/DE-FG02-09ER46577
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 94; Journal Issue: 7; Related Information: S3TEC partners with Massachusetts Institute of Technology (lead); Boston College; Oak Ridge National Laboratory; Rensselaer Polytechnic Institute; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 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)
Citation Formats
Fu, Yuhao, Singh, David J., Li, Wu, and Zhang, Lijun. Intrinsic ultralow lattice thermal conductivity of the unfilled skutterudite FeSb3. United States: N. p., 2016.
Web. doi:10.1103/PhysRevB.94.075122.
Fu, Yuhao, Singh, David J., Li, Wu, & Zhang, Lijun. Intrinsic ultralow lattice thermal conductivity of the unfilled skutterudite FeSb3. United States. https://doi.org/10.1103/PhysRevB.94.075122
Fu, Yuhao, Singh, David J., Li, Wu, and Zhang, Lijun. Thu .
"Intrinsic ultralow lattice thermal conductivity of the unfilled skutterudite FeSb3". United States. https://doi.org/10.1103/PhysRevB.94.075122. https://www.osti.gov/servlets/purl/1388448.
@article{osti_1388448,
title = {Intrinsic ultralow lattice thermal conductivity of the unfilled skutterudite FeSb3},
author = {Fu, Yuhao and Singh, David J. and Li, Wu and Zhang, Lijun},
abstractNote = {It is generally accepted that unfilled skutterudites process high lattice thermal conductivity $κ_l$ that can be efficiently reduced upon filling. Here by using first-principles Boltzmann-Peierls transport calculations, we find pure skutterudite of FeSb3 with no filler in fact has an intrinsic ultralow $κ_l$ smaller than that of CoSb3 by one order of magnitude. The value is even smaller than those of most of the fully filled skutterudites. This finding means that with FeSb3 as a reference, filling does not necessarily lower $κ_l$. The ultralow $κ_l$ of FeSb3 is a consequence of the overall softening of phonon spectrum, especially the lowering in frequency of optical phonon branches associated with the weakly bonded Sb4 rings. They overlap more with heat-carrying acoustic phonons and significantly increase the phase space for three-phonon anharmonic scattering processes. This provides an alternative non-filling-related mechanism for lowering the $κ_l$ of skutterudites.},
doi = {10.1103/PhysRevB.94.075122},
journal = {Physical Review B},
number = 7,
volume = 94,
place = {United States},
year = {Thu Aug 11 00:00:00 EDT 2016},
month = {Thu Aug 11 00:00:00 EDT 2016}
}
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