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Title: Anharmonic lattice dynamics and superionic transition in AgCrSe 2

Abstract

Intrinsically low lattice thermal conductivity ( κ l a t ) in superionic conductors is of great interest for energy conversion applications in thermoelectrics. Yet, the complex atomic dynamics leading to superionicity and ultralow thermal conductivity remain poorly understood. Here, we report a comprehensive study of the lattice dynamics and superionic diffusion in A g C r S e 2 from energy- and momentum-resolved neutron and X-ray scattering techniques, combined with first-principles calculations. Our results settle unresolved questions about the lattice dynamics and thermal conduction mechanism in A g C r S e 2 . We find that the heat-carrying long-wavelength transverse acoustic (TA) phonons coexist with the ultrafast diffusion of Ag ions in the superionic phase, while the short-wavelength nondispersive TA phonons break down. Strong scattering of phonon quasiparticles by anharmonicity and Ag disorder are the origin of intrinsically low κ l a t . The breakdown of short-wavelength TA phonons is directly related to the Ag diffusion, with the vibrational spectral weight associated to Ag oscillations evolving into stochastic decaying fluctuations. Furthermore, the origin of fast ionic diffusion is shown to arise from extended flat basins in the energy landscape and collective hopping behavior facilitated by strong repulsion between Ag ions. These results provide fundamental insights into the complex atomic dynamics of superionic conductors.

Authors:
; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1598367
Grant/Contract Number:  
SC0019299; SC0016166
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English

Citation Formats

Ding, Jingxuan, Niedziela, Jennifer L., Bansal, Dipanshu, Wang, Jiuling, He, Xing, May, Andrew F., Ehlers, Georg, Abernathy, Douglas L., Said, Ayman, Alatas, Ahmet, Ren, Yang, Arya, Gaurav, and Delaire, Olivier. Anharmonic lattice dynamics and superionic transition in AgCrSe 2. United States: N. p., 2020. Web. doi:10.1073/pnas.1913916117.
Ding, Jingxuan, Niedziela, Jennifer L., Bansal, Dipanshu, Wang, Jiuling, He, Xing, May, Andrew F., Ehlers, Georg, Abernathy, Douglas L., Said, Ayman, Alatas, Ahmet, Ren, Yang, Arya, Gaurav, & Delaire, Olivier. Anharmonic lattice dynamics and superionic transition in AgCrSe 2. United States. doi:10.1073/pnas.1913916117.
Ding, Jingxuan, Niedziela, Jennifer L., Bansal, Dipanshu, Wang, Jiuling, He, Xing, May, Andrew F., Ehlers, Georg, Abernathy, Douglas L., Said, Ayman, Alatas, Ahmet, Ren, Yang, Arya, Gaurav, and Delaire, Olivier. Thu . "Anharmonic lattice dynamics and superionic transition in AgCrSe 2". United States. doi:10.1073/pnas.1913916117.
@article{osti_1598367,
title = {Anharmonic lattice dynamics and superionic transition in AgCrSe 2},
author = {Ding, Jingxuan and Niedziela, Jennifer L. and Bansal, Dipanshu and Wang, Jiuling and He, Xing and May, Andrew F. and Ehlers, Georg and Abernathy, Douglas L. and Said, Ayman and Alatas, Ahmet and Ren, Yang and Arya, Gaurav and Delaire, Olivier},
abstractNote = {Intrinsically low lattice thermal conductivity ( κ l a t ) in superionic conductors is of great interest for energy conversion applications in thermoelectrics. Yet, the complex atomic dynamics leading to superionicity and ultralow thermal conductivity remain poorly understood. Here, we report a comprehensive study of the lattice dynamics and superionic diffusion in A g C r S e 2 from energy- and momentum-resolved neutron and X-ray scattering techniques, combined with first-principles calculations. Our results settle unresolved questions about the lattice dynamics and thermal conduction mechanism in A g C r S e 2 . We find that the heat-carrying long-wavelength transverse acoustic (TA) phonons coexist with the ultrafast diffusion of Ag ions in the superionic phase, while the short-wavelength nondispersive TA phonons break down. Strong scattering of phonon quasiparticles by anharmonicity and Ag disorder are the origin of intrinsically low κ l a t . The breakdown of short-wavelength TA phonons is directly related to the Ag diffusion, with the vibrational spectral weight associated to Ag oscillations evolving into stochastic decaying fluctuations. Furthermore, the origin of fast ionic diffusion is shown to arise from extended flat basins in the energy landscape and collective hopping behavior facilitated by strong repulsion between Ag ions. These results provide fundamental insights into the complex atomic dynamics of superionic conductors.},
doi = {10.1073/pnas.1913916117},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = ,
volume = ,
place = {United States},
year = {2020},
month = {2}
}

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