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Title: Low-temperature heat capacity and localized vibrational modes in natural and synthetic tetrahedrites

Abstract

The heat capacity of natural (Cu12-x (Fe, Zn, Ag)x(Sb, As)4S13) and synthetic (Cu12-xZnxSb4S13 with x = 0, 1, 2) tetrahedrite compounds was measured between 2 K and 380 K. It was found that the temperature dependence of the heat capacity can be described using a Debye term and three Einstein oscillators with characteristic temperatures that correspond to energies of ~1.0 meV, ~2.8 meV, and ~8.4 meV. The existence of localized vibrational modes, which are assigned to the displacements of the trigonally coordinated Cu atoms in the structure, is discussed in the context of anharmonicity and its effect on the low lattice thermal conductivity exhibited by these compounds.

Authors:
 [1];  [1];  [1];  [1];  [2];  [2];  [2];  [2]
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  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  2. Michigan State Univ., East Lansing, MI (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Revolutionary Materials for Solid State Energy Conversion (RMSSEC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1386792
Grant/Contract Number:  
SC0001054
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 115; Journal Issue: 19; Related Information: RMSSEC partners with Michigan State University (lead); University of California, Los Angeles; University of Michigan; Northwestern University; Oak Ridge National Laboratory; Ohio State University; Wayne State University; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; solar (thermal); phonons; thermal conductivity; thermoelectric; mechanical behavior; charge transport; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing)

Citation Formats

Lara-Curzio, E., May, A. F., Delaire, O., McGuire, M. A., Lu, X., Liu, Cheng-Yun, Case, E. D., and Morelli, D. T. Low-temperature heat capacity and localized vibrational modes in natural and synthetic tetrahedrites. United States: N. p., 2014. Web. doi:10.1063/1.4878676.
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Lara-Curzio, E., May, A. F., Delaire, O., McGuire, M. A., Lu, X., Liu, Cheng-Yun, Case, E. D., & Morelli, D. T. Low-temperature heat capacity and localized vibrational modes in natural and synthetic tetrahedrites. United States. https://doi.org/10.1063/1.4878676
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Lara-Curzio, E., May, A. F., Delaire, O., McGuire, M. A., Lu, X., Liu, Cheng-Yun, Case, E. D., and Morelli, D. T. Wed . "Low-temperature heat capacity and localized vibrational modes in natural and synthetic tetrahedrites". United States. https://doi.org/10.1063/1.4878676. https://www.osti.gov/servlets/purl/1386792.
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@article{osti_1386792,
title = {Low-temperature heat capacity and localized vibrational modes in natural and synthetic tetrahedrites},
author = {Lara-Curzio, E. and May, A. F. and Delaire, O. and McGuire, M. A. and Lu, X. and Liu, Cheng-Yun and Case, E. D. and Morelli, D. T.},
abstractNote = {The heat capacity of natural (Cu12-x (Fe, Zn, Ag)x(Sb, As)4S13) and synthetic (Cu12-xZnxSb4S13 with x = 0, 1, 2) tetrahedrite compounds was measured between 2 K and 380 K. It was found that the temperature dependence of the heat capacity can be described using a Debye term and three Einstein oscillators with characteristic temperatures that correspond to energies of ~1.0 meV, ~2.8 meV, and ~8.4 meV. The existence of localized vibrational modes, which are assigned to the displacements of the trigonally coordinated Cu atoms in the structure, is discussed in the context of anharmonicity and its effect on the low lattice thermal conductivity exhibited by these compounds.},
doi = {10.1063/1.4878676},
journal = {Journal of Applied Physics},
number = 19,
volume = 115,
place = {United States},
year = {Wed May 21 00:00:00 EDT 2014},
month = {Wed May 21 00:00:00 EDT 2014}
}
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https://doi.org/10.1063/1.4878676
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Works referenced in this record:

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    Works referencing / citing this record:

    From Bonding Asymmetry to Anharmonic Rattling in Cu 12 Sb 4 S 13 Tetrahedrites: When Lone-Pair Electrons Are Not So Lonely
    journal, May 2015

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    • DOI: 10.1002/adfm.201500766

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    High-Temperature Transport Properties of Colusite Cu24 T 2V2Ge6S32 (T = Ni, Co)
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    Thermoelectric Properties of Magnesium-Doped Tetrahedrite Cu12−xMgxSb4S13
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    journal, January 2015

    • Bouyrie, Y.; Candolfi, C.; Pailhès, S.
    • Physical Chemistry Chemical Physics, Vol. 17, Issue 30
    • DOI: 10.1039/c5cp02900g

    On the microscopic dynamics of the ‘Einstein solids’ AlV 2 Al 20 and GaV 2 Al 20 , and of YV 2 Al 20 : a benchmark system for ‘rattling’ excitations
    journal, January 2015

    • Koza, Michael Marek; Mutka, Hannu; Okamoto, Yoshihiko
    • Physical Chemistry Chemical Physics, Vol. 17, Issue 38
    • DOI: 10.1039/c5cp04005a

    Tetrahedrites as thermoelectric materials: an overview
    journal, January 2015

    • Chetty, R.; Bali, A.; Mallik, R. C.
    • Journal of Materials Chemistry C, Vol. 3, Issue 48
    • DOI: 10.1039/c5tc02537k

    Structural analysis and thermoelectric properties of mechanically alloyed colusites
    journal, January 2016

    • Bourgès, Cédric; Gilmas, Margaux; Lemoine, Pierric
    • Journal of Materials Chemistry C, Vol. 4, Issue 31
    • DOI: 10.1039/c6tc02301k

    Powder metallurgically synthesized Cu 12 Sb 4 S 13 tetrahedrites: phase transition and high thermoelectricity
    journal, January 2017

    • Sun, Fu-Hua; Wu, Chao-Feng; Li, Zhiliang
    • RSC Advances, Vol. 7, Issue 31
    • DOI: 10.1039/c7ra02564e

    Promoted high temperature carrier mobility and thermoelectric performance of InTe enabled by altering scattering mechanism
    journal, January 2019

    • Zhu, Huaxing; Zhang, Bin; Wang, Guiwen
    • Journal of Materials Chemistry A, Vol. 7, Issue 19
    • DOI: 10.1039/c9ta00475k

    High-performance thermoelectric minerals: Colusites Cu 26 V 2 M 6 S 32 (M = Ge, Sn)
    journal, September 2014

    • Suekuni, Koichiro; Kim, Fiseong S.; Nishiate, Hirotaka
    • Applied Physics Letters, Vol. 105, Issue 13
    • DOI: 10.1063/1.4896998

    Research Update: Cu–S based synthetic minerals as efficient thermoelectric materials at medium temperatures
    journal, October 2016

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    • APL Materials, Vol. 4, Issue 10
    • DOI: 10.1063/1.4955398

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    journal, September 2019

    • Powell, Anthony V.
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    • DOI: 10.1111/jace.13838

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