Selective breakdown of phonon quasiparticles across superionic transition in CuCrSe2
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 behavior. 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, while 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. These results demonstrate that anharmonic phonon dynamics are at the origin of low thermal conductivity and superionicity in this class of materials. 2
- Authors:
-
[1];
[3];
[3];
[3];
[2]
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Duke Univ., Durham, NC (United States)
- Duke Univ., Durham, NC (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Energy Frontier Research Centers (EFRC) (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC); Argonne National Laboratory (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. https://doi.org/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. https://doi.org/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 behavior. 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, while 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. These results demonstrate that anharmonic phonon dynamics are at the origin of low thermal conductivity and superionicity in this class of materials. 2},
doi = {10.1038/s41567-018-0298-2},
journal = {Nature Physics},
number = 1,
volume = 15,
place = {United States},
year = {Mon Oct 08 00:00:00 EDT 2018},
month = {Mon Oct 08 00:00:00 EDT 2018}
}
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Figures / Tables:
Figure 1: Anomalous atomic dynamics across the superionic transition in CuCrSe2. (a) Room temperature crystal structure of CuCrSe2. (e) High temperature structure shown with Cu occupancy on $α$ and $β$ sites (indicated with half white-half red spheres). Tetrahedral hopping directions shown with thick red bands. (b-d) $S$(|$Q$|, $E$) maps measuredmore »
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