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

Title: Two-channel model for ultralow thermal conductivity of crystalline Tl 3VSe 4

Abstract

Solids with ultralow thermal conductivity are of great interest as thermal barrier coatings for insulation or thermoelectrics for energy conversion. However, the theoretical limits of lattice thermal conductivity (κ) are unclear. In typical crystals a phonon picture is valid, whereas lowest κ values occur in highly disordered materials where this picture fails and heat is supposedly carried by random walk among uncorrelated oscillators. Here in this paper we identify a simple crystal, Tl 3VSe 4, with a calculated phonon κ [0.16 Watts per meter-Kelvin (W/m-K)] one-half that of our measured κ (0.30 W/m-K) at 300 K, approaching disorder κ values, although Raman spectra, specific heat, and temperature dependence of κ reveal typical phonon characteristics. Adding a transport component based on uncorrelated oscillators explains the measured κ and suggests that a two-channel model is necessary for crystals with ultralow κ.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [2]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division; Naval Research Lab. (NRL), Washington, DC (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1459275
Grant/Contract Number:  
AC05-00OR22725; AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Science
Additional Journal Information:
Journal Volume: 360; Journal Issue: 6396; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Mukhopadhyay, Saikat, Parker, David S., Sales, Brian C., Puretzky, Alexander A., McGuire, Michael A., and Lindsay, Lucas R.. Two-channel model for ultralow thermal conductivity of crystalline Tl3VSe4. United States: N. p., 2018. Web. doi:10.1126/science.aar8072.
Mukhopadhyay, Saikat, Parker, David S., Sales, Brian C., Puretzky, Alexander A., McGuire, Michael A., & Lindsay, Lucas R.. Two-channel model for ultralow thermal conductivity of crystalline Tl3VSe4. United States. doi:10.1126/science.aar8072.
Mukhopadhyay, Saikat, Parker, David S., Sales, Brian C., Puretzky, Alexander A., McGuire, Michael A., and Lindsay, Lucas R.. Fri . "Two-channel model for ultralow thermal conductivity of crystalline Tl3VSe4". United States. doi:10.1126/science.aar8072.
@article{osti_1459275,
title = {Two-channel model for ultralow thermal conductivity of crystalline Tl3VSe4},
author = {Mukhopadhyay, Saikat and Parker, David S. and Sales, Brian C. and Puretzky, Alexander A. and McGuire, Michael A. and Lindsay, Lucas R.},
abstractNote = {Solids with ultralow thermal conductivity are of great interest as thermal barrier coatings for insulation or thermoelectrics for energy conversion. However, the theoretical limits of lattice thermal conductivity (κ) are unclear. In typical crystals a phonon picture is valid, whereas lowest κ values occur in highly disordered materials where this picture fails and heat is supposedly carried by random walk among uncorrelated oscillators. Here in this paper we identify a simple crystal, Tl3VSe4, with a calculated phonon κ [0.16 Watts per meter-Kelvin (W/m-K)] one-half that of our measured κ (0.30 W/m-K) at 300 K, approaching disorder κ values, although Raman spectra, specific heat, and temperature dependence of κ reveal typical phonon characteristics. Adding a transport component based on uncorrelated oscillators explains the measured κ and suggests that a two-channel model is necessary for crystals with ultralow κ.},
doi = {10.1126/science.aar8072},
journal = {Science},
number = 6396,
volume = 360,
place = {United States},
year = {Fri Jun 29 00:00:00 EDT 2018},
month = {Fri Jun 29 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on June 29, 2019
Publisher's Version of Record

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

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


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

Lower limit to the thermal conductivity of disordered crystals
journal, September 1992

  • Cahill, David G.; Watson, S. K.; Pohl, R. O.
  • Physical Review B, Vol. 46, Issue 10, p. 6131-6140
  • DOI: 10.1103/PhysRevB.46.6131

Ultralow thermal conductivity and high thermoelectric figure of merit in SnSe crystals
journal, April 2014

  • Zhao, Li-Dong; Lo, Shih-Han; Zhang, Yongsheng
  • Nature, Vol. 508, Issue 7496, p. 373-377
  • DOI: 10.1038/nature13184

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


New and Old Concepts in Thermoelectric Materials
journal, November 2009

  • Sootsman, Joseph R.; Chung, Duck Young; Kanatzidis, Mercouri G.
  • Angewandte Chemie International Edition, Vol. 48, Issue 46, p. 8616-8639
  • DOI: 10.1002/anie.200900598

Intrinsically Minimal Thermal Conductivity in Cubic IVVI2 Semiconductors
journal, July 2008