Anharmonic lattice dynamics and superionic transition in AgCrSe 2
Abstract
Intrinsically low lattice thermal conductivity ( ) 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 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 . 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 . 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 findings offer fundamental insights into the complex atomic dynamics of superionic conductors.
- Authors:
- Publication Date:
- Research Org.:
- Duke Univ., Durham, NC (United States); Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of California, Berkeley, CA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Contributing Org.:
- Oak Ridge National Laboratory Spallation Neutron Source; National Energy Research Scientific Computing Center
- OSTI Identifier:
- 1598367
- Alternate Identifier(s):
- OSTI ID: 1598277; OSTI ID: 1607011; OSTI ID: 1632173
- Grant/Contract Number:
- SC0019299; SC0016166; AC02-06CH11357; AC02-05CH11231; AC05-00OR22725
- 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 Volume: 117 Journal Issue: 8; Journal ID: ISSN 0027-8424
- Publisher:
- National Academy of Sciences
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Superionic conductor; Thermoelectrics; Thermal transport; Phonons; Diffusion; Anharmonic lattice dynamics; anharmonic lattice dynamics; superionic conductor; thermal transport; thermoelectrics
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. https://doi.org/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. https://doi.org/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 (κlat) 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 inAgCrSe2from 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 inAgCrSe2. 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 lowκlat. 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 findings offer 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 = 8,
volume = 117,
place = {United States},
year = {2020},
month = {2}
}
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Works referenced in this record:
Localised Ag+ vibrations at the origin of ultralow thermal conductivity in layered thermoelectric AgCrSe2
journal, March 2016
- Damay, F.; Petit, S.; Rols, S.
- Scientific Reports, Vol. 6, Issue 1
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
Temperature-dependent effective third-order interatomic force constants from first principles
journal, October 2013
- Hellman, Olle; Abrikosov, I. A.
- Physical Review B, Vol. 88, Issue 14
Power Factor Enhancement by Modulation Doping in Bulk Nanocomposites
journal, June 2011
- Zebarjadi, Mona; Joshi, Giri; Zhu, Gaohua
- Nano Letters, Vol. 11, Issue 6
Order–Disorder Transition in AgCrSe 2 : a New Route to Efficient Thermoelectrics
journal, May 2011
- Gascoin, Franck; Maignan, Antoine
- Chemistry of Materials, Vol. 23, Issue 10
Phonon spectra in superionic and normal states of the layered crystal AgCrSe2
journal, August 1990
- Wakamura, K.
- Solid State Ionics, Vol. 40-41
Localized vibrational modes in metallic solids
journal, October 1998
- Keppens, V.; Mandrus, D.; Sales, B. C.
- Nature, Vol. 395, Issue 6705
Suppression of atom motion and metal deposition in mixed ionic electronic conductors
journal, July 2018
- Qiu, Pengfei; Agne, Matthias T.; Liu, Yongying
- Nature Communications, Vol. 9, Issue 1
Suppression of thermal conductivity by rattling modes in thermoelectric sodium cobaltate
journal, August 2013
- Voneshen, D. J.; Refson, K.; Borissenko, E.
- Nature Materials, Vol. 12, Issue 11
Resonant bonding leads to low lattice thermal conductivity
journal, April 2014
- Lee, Sangyeop; Esfarjani, Keivan; Luo, Tengfei
- Nature Communications, Vol. 5, Issue 1
High-Energy Synchrotron X-Ray Diffraction and Its Application to In Situ Structural Phase-Transition Studies in Complex Sample Environments
journal, January 2012
- Ren, Yang
- JOM, Vol. 64, Issue 1
Neutron scattering study of short-range correlations and ionic diffusion in copper selenide
journal, November 2010
- Danilkin, S. A.; Avdeev, M.; Sakuma, T.
- Ionics, Vol. 17, Issue 1
A lithium superionic conductor
journal, July 2011
- Kamaya, Noriaki; Homma, Kenji; Yamakawa, Yuichiro
- Nature Materials, Vol. 10, Issue 9, p. 682-686
Order–disorder phenomena in layered CuCrSe2 crystals
journal, August 2014
- Gagor, A.; Gnida, D.; Pietraszko, A.
- Materials Chemistry and Physics, Vol. 146, Issue 3
Hopping Time Scales and the Phonon-Liquid Electron-Crystal Picture in Thermoelectric Copper Selenide
journal, April 2017
- Voneshen, D. J.; Walker, H. C.; Refson, K.
- Physical Review Letters, Vol. 118, Issue 14
New developments in fabrication of high-energy-resolution analyzers for inelastic X-ray spectroscopy
journal, March 2011
- Said, Ayman H.; Sinn, Harald; Divan, Ralu
- Journal of Synchrotron Radiation, Vol. 18, Issue 3
High-power all-solid-state batteries using sulfide superionic conductors
journal, March 2016
- Kato, Yuki; Hori, Satoshi; Saito, Toshiya
- Nature Energy, Vol. 1, Issue 4
High-performance bulk thermoelectrics with all-scale hierarchical architectures
journal, September 2012
- Biswas, Kanishka; He, Jiaqing; Blum, Ivan D.
- Nature, Vol. 489, Issue 7416, p. 414-418
Superionic Conduction in AgCrS[sub 2] and AgCrSe[sub 2]
journal, January 1977
- Murphy, D. W.
- Journal of The Electrochemical Society, Vol. 124, Issue 8
Computational and Experimental Investigations of Na-Ion Conduction in Cubic Na 3 PSe 4
journal, December 2015
- Bo, Shou-Hang; Wang, Yan; Kim, Jae Chul
- Chemistry of Materials, Vol. 28, Issue 1
Origin of fast ion diffusion in super-ionic conductors
journal, June 2017
- He, Xingfeng; Zhu, Yizhou; Mo, Yifei
- Nature Communications, Vol. 8, Issue 1
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
Crystal structures and magnetic structures of some metal(I) chromium(III) sulfides and selenides
journal, April 1973
- Engelsman, F. M. R.; Wiegers, G. A.; Jellinek, F.
- Journal of Solid State Chemistry, Vol. 6, Issue 4
Tuning mobility and stability of lithium ion conductors based on lattice dynamics
journal, January 2018
- Muy, Sokseiha; Bachman, John C.; Giordano, Livia
- Energy & Environmental Science, Vol. 11, Issue 4
Superionic Diffusion through Frustrated Energy Landscape
journal, September 2019
- Di Stefano, Davide; Miglio, Anna; Robeyns, Koen
- Chem, Vol. 5, Issue 9
CuCrSe2: a high performance phonon glass and electron crystal thermoelectric material
journal, January 2013
- Bhattacharya, Shovit; Basu, Ranita; Bhatt, Ranu
- Journal of Materials Chemistry A, Vol. 1, Issue 37
DynaPhoPy: A code for extracting phonon quasiparticles from molecular dynamics simulations
journal, December 2017
- Carreras, Abel; Togo, Atsushi; Tanaka, Isao
- Computer Physics Communications, Vol. 221
Structural features and ionic transport in two-dimensional MxYSe2 (M = Cu, Ag; Y = Cr, Nb) mixed conductors
journal, October 1988
- Yakshibayev, R.
- Solid State Ionics, Vol. 31, Issue 1
The new cold neutron chopper spectrometer at the Spallation Neutron Source: Design and performance
journal, August 2011
- Ehlers, G.; Podlesnyak, A. A.; Niedziela, J. L.
- Review of Scientific Instruments, Vol. 82, Issue 8
Direct atomic-scale observation of the Ag + diffusion structure in the quasi-2D “liquid-like” state of superionic thermoelectric AgCrSe 2
journal, January 2019
- Xie, Lin; Wu, Di; Yang, Hongliang
- Journal of Materials Chemistry C, Vol. 7, Issue 30
Selective breakdown of phonon quasiparticles across superionic transition in CuCrSe2
journal, October 2018
- Niedziela, Jennifer L.; Bansal, Dipanshu; May, Andrew F.
- Nature Physics, Vol. 15, Issue 1
High thermoelectric performance of (AgCrSe 2 ) 0.5 (CuCrSe 2 ) 0.5 nano-composites having all-scale natural hierarchical architectures
journal, January 2014
- Bhattacharya, Shovit; Bohra, Anil; Basu, Ranita
- J. Mater. Chem. A, Vol. 2, Issue 40
Magnetic and transport properties, and electronic structure of the layered chalcogenide AgCrSe2
journal, June 2002
- Gautam, Ujjal K.; Seshadri, Ram; Vasudevan, S.
- Solid State Communications, Vol. 122, Issue 11
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Influence of lattice dynamics on lithium-ion conductivity: A first-principles study
journal, March 2019
- Sagotra, Arun K.; Chu, Dewei; Cazorla, Claudio
- Physical Review Materials, Vol. 3, Issue 3
Potential for superionic conductors in thermoelectric applications
journal, April 2017
- Bailey, Trevor P.; Uher, Ctirad
- Current Opinion in Green and Sustainable Chemistry, Vol. 4
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Thermoelectric Transport in Cu 7 PSe 6 with High Copper Ionic Mobility
journal, August 2014
- Weldert, Kai S.; Zeier, Wolfgang G.; Day, Tristan W.
- Journal of the American Chemical Society, Vol. 136, Issue 34
Avoided crossing of rattler modes in thermoelectric materials
journal, August 2008
- Christensen, Mogens; Abrahamsen, Asger B.; Christensen, Niels B.
- Nature Materials, Vol. 7, Issue 10
Revisiting AgCrSe 2 as a promising thermoelectric material
journal, January 2016
- Wu, Di; Huang, Sizhao; Feng, Dan
- Physical Chemistry Chemical Physics, Vol. 18, Issue 34
Part-crystalline part-liquid state and rattling-like thermal damping in materials with chemical-bond hierarchy
journal, October 2014
- Qiu, Wujie; Xi, Lili; Wei, Ping
- Proceedings of the National Academy of Sciences, Vol. 111, Issue 42
Glass-like phonon scattering from a spontaneous nanostructure in AgSbTe2
journal, June 2013
- Ma, J.; Delaire, O.; May, A. F.
- Nature Nanotechnology, Vol. 8, Issue 6
Six-reflection meV-monochromator for synchrotron radiation
journal, May 2011
- Toellner, T. S.; Alatas, A.; Said, A. H.
- Journal of Synchrotron Radiation, Vol. 18, Issue 4
Design and operation of the wide angular-range chopper spectrometer ARCS at the Spallation Neutron Source
journal, January 2012
- Abernathy, D. L.; Stone, M. B.; Loguillo, M. J.
- Review of Scientific Instruments, Vol. 83, Issue 1
Lattice dynamics of anharmonic solids from first principles
journal, November 2011
- Hellman, O.; Abrikosov, I. A.; Simak, S. I.
- Physical Review B, Vol. 84, Issue 18
Self-interaction correction to density-functional approximations for many-electron systems
journal, May 1981
- Perdew, J. P.; Zunger, Alex
- Physical Review B, Vol. 23, Issue 10, p. 5048-5079
Superionic Phase Transition in Silver Chalcogenide Nanocrystals Realizing Optimized Thermoelectric Performance
journal, February 2012
- Xiao, Chong; Xu, Jie; Li, Kun
- Journal of the American Chemical Society, Vol. 134, Issue 9
Liquid-like thermal conduction in intercalated layered crystalline solids
journal, January 2018
- Li, B.; Wang, H.; Kawakita, Y.
- Nature Materials, Vol. 17, Issue 3
Dynamics of ions of the two-dimensional superionic conductor AgCr
journal, April 1983
- Brüesch, P.; Hibma, T.; Bührer, W.
- Physical Review B, Vol. 27, Issue 8
First-principles calculations of the ferroelastic transition between rutile-type and -type at high pressures
journal, October 2008
- Togo, Atsushi; Oba, Fumiyasu; Tanaka, Isao
- Physical Review B, Vol. 78, Issue 13
Copper ion liquid-like thermoelectrics
journal, March 2012
- Liu, Huili; Shi, Xun; Xu, Fangfang
- Nature Materials, Vol. 11, Issue 5, p. 422-425
Observation of anomalously increasing phonon damping constant in the β phase of the fast-ionic conductor SI
journal, February 1990
- Wakamura, Kunio; Miura, Fumitsuka; Kojima, Akira
- Physical Review B, Vol. 41, Issue 5
Breakdown of phonon glass paradigm in La- and Ce-filled Fe4Sb12 skutterudites
journal, August 2008
- Koza, Michael Marek; Johnson, Mark Robert; Viennois, Romain
- Nature Materials, Vol. 7, Issue 10