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Title: Selective breakdown of phonon quasiparticles across superionic transition in CuCrSe 2

Abstract

Superionic crystals exhibit ionic mobilities comparable to liquids while maintaining a periodic crystalline lattice. The atomic dynamics leading to large ionic mobility have long been debated. A central question is whether phonon quasiparticles—which conduct heat in regular solids—survive in the superionic state, where a large fraction of the system exhibits liquid-like behaviour. Here we present the results of energy- and momentum-resolved scattering studies combined with first-principles calculations and show that in the superionic phase of CuCrSe 2, long-wavelength acoustic phonons capable of heat conduction remain largely intact, whereas specific phonon quasiparticles dominated by the Cu ions break down as a result of anharmonicity and disorder. The weak bonding and large anharmonicity of the Cu sublattice are present already in the normal ordered state, resulting in low thermal conductivity even below the superionic transition. Furthermore, these results demonstrate that anharmonic phonon dynamics are at the origin of low thermal conductivity and superionicity in this class of materials.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3];  [2];  [2]; ORCiD logo [3]; ORCiD logo [3];  [4]; ORCiD logo [2]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Duke Univ., Durham, NC (United States)
  2. Duke Univ., Durham, NC (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory, Oak Ridge Leadership Computing Facility (OLCF); Energy Frontier Research Centers (EFRC) (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1491346
Alternate Identifier(s):
OSTI ID: 1493733
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Physics
Additional Journal Information:
Journal Volume: 15; Journal Issue: 1; Journal ID: ISSN 1745-2473
Publisher:
Nature Publishing Group (NPG)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Niedziela, Jennifer L., Bansal, Dipanshu, May, Andrew F., Ding, Jingxuan, Lanigan-Atkins, Tyson, Ehlers, Georg, Abernathy, Douglas L., Said, Ayman, and Delaire, Olivier. Selective breakdown of phonon quasiparticles across superionic transition in CuCrSe2. United States: N. p., 2018. Web. doi:10.1038/s41567-018-0298-2.
Niedziela, Jennifer L., Bansal, Dipanshu, May, Andrew F., Ding, Jingxuan, Lanigan-Atkins, Tyson, Ehlers, Georg, Abernathy, Douglas L., Said, Ayman, & Delaire, Olivier. Selective breakdown of phonon quasiparticles across superionic transition in CuCrSe2. United States. doi:10.1038/s41567-018-0298-2.
Niedziela, Jennifer L., Bansal, Dipanshu, May, Andrew F., Ding, Jingxuan, Lanigan-Atkins, Tyson, Ehlers, Georg, Abernathy, Douglas L., Said, Ayman, and Delaire, Olivier. Mon . "Selective breakdown of phonon quasiparticles across superionic transition in CuCrSe2". United States. doi:10.1038/s41567-018-0298-2. https://www.osti.gov/servlets/purl/1491346.
@article{osti_1491346,
title = {Selective breakdown of phonon quasiparticles across superionic transition in CuCrSe2},
author = {Niedziela, Jennifer L. and Bansal, Dipanshu and May, Andrew F. and Ding, Jingxuan and Lanigan-Atkins, Tyson and Ehlers, Georg and Abernathy, Douglas L. and Said, Ayman and Delaire, Olivier},
abstractNote = {Superionic crystals exhibit ionic mobilities comparable to liquids while maintaining a periodic crystalline lattice. The atomic dynamics leading to large ionic mobility have long been debated. A central question is whether phonon quasiparticles—which conduct heat in regular solids—survive in the superionic state, where a large fraction of the system exhibits liquid-like behaviour. Here we present the results of energy- and momentum-resolved scattering studies combined with first-principles calculations and show that in the superionic phase of CuCrSe2, long-wavelength acoustic phonons capable of heat conduction remain largely intact, whereas specific phonon quasiparticles dominated by the Cu ions break down as a result of anharmonicity and disorder. The weak bonding and large anharmonicity of the Cu sublattice are present already in the normal ordered state, resulting in low thermal conductivity even below the superionic transition. Furthermore, these results demonstrate that anharmonic phonon dynamics are at the origin of low thermal conductivity and superionicity in this class of materials.},
doi = {10.1038/s41567-018-0298-2},
journal = {Nature Physics},
number = 1,
volume = 15,
place = {United States},
year = {2018},
month = {10}
}

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