Higherorder phonon scattering: advancing the quantum theory of phonon linewidth, thermal conductivity and thermal radiative properties
Abstract
Phonon scattering plays a central role in the quantum theory of phonon linewidth, which in turn governs important properties including infrared spectra, Raman spectra, lattice thermal conductivity, thermal radiative properties, and also signifi cantly affects other important processes such as hot electron relaxation. Since Maradudin and Fein’s classic work in 1962, threephonon scattering had been considered as the dominant intrinsic phonon scattering mechanism and has seen tremendous advances. However, the role of the higherorder fourphonon scattering had been persistently unclear and so was ignored. The tremendous complexity of the formalism and computational challenges stood in the way, prohibiting the direct and quantitative treatment of fourphonon scattering. In 2016, a rigorous fourphonon scattering formalism was developed, and the prediction was realized using empirical potentials. In 2017, the method was extended using firstprinciples calculated force constants, and the thermal conductivities of boron arsenides (BAs), Si and diamond were predicted. The predictions for BAs were later confirmed by several independent experiments. Fourphonon scattering has since been investigated in a range of materials and established as an important intrinsic scattering mechanism for thermal transport and radiative properties. Specifically, fourphonon scattering is important when the fourthorder scattering potential or phase space becomes relatively large. Themore »
 Authors:

 ORNL
 Purdue University
 Publication Date:
 Research Org.:
 Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
 Sponsoring Org.:
 USDOE Office of Energy Efficiency and Renewable Energy (EERE)
 OSTI Identifier:
 1619009
 DOE Contract Number:
 AC0500OR22725
 Resource Type:
 Book
 Country of Publication:
 United States
 Language:
 English
Citation Formats
Feng, Tianli, and Ruan, Xiulin. Higherorder phonon scattering: advancing the quantum theory of phonon linewidth, thermal conductivity and thermal radiative properties. United States: N. p., 2020.
Web.
Feng, Tianli, & Ruan, Xiulin. Higherorder phonon scattering: advancing the quantum theory of phonon linewidth, thermal conductivity and thermal radiative properties. United States.
Feng, Tianli, and Ruan, Xiulin. Sun .
"Higherorder phonon scattering: advancing the quantum theory of phonon linewidth, thermal conductivity and thermal radiative properties". United States.
@article{osti_1619009,
title = {Higherorder phonon scattering: advancing the quantum theory of phonon linewidth, thermal conductivity and thermal radiative properties},
author = {Feng, Tianli and Ruan, Xiulin},
abstractNote = {Phonon scattering plays a central role in the quantum theory of phonon linewidth, which in turn governs important properties including infrared spectra, Raman spectra, lattice thermal conductivity, thermal radiative properties, and also signifi cantly affects other important processes such as hot electron relaxation. Since Maradudin and Fein’s classic work in 1962, threephonon scattering had been considered as the dominant intrinsic phonon scattering mechanism and has seen tremendous advances. However, the role of the higherorder fourphonon scattering had been persistently unclear and so was ignored. The tremendous complexity of the formalism and computational challenges stood in the way, prohibiting the direct and quantitative treatment of fourphonon scattering. In 2016, a rigorous fourphonon scattering formalism was developed, and the prediction was realized using empirical potentials. In 2017, the method was extended using firstprinciples calculated force constants, and the thermal conductivities of boron arsenides (BAs), Si and diamond were predicted. The predictions for BAs were later confirmed by several independent experiments. Fourphonon scattering has since been investigated in a range of materials and established as an important intrinsic scattering mechanism for thermal transport and radiative properties. Specifically, fourphonon scattering is important when the fourthorder scattering potential or phase space becomes relatively large. The former scenario includes: (i) nearly all materials when the temperature is high; (ii) strongly anharmonic (low thermal conductivity) materials, including most rocksalt compounds, halides, hydrides, chalcogenides and oxides. The latter scenario includes: (iii) materials with large acoustic–optical phonon band gaps, such as XY compounds with a large atomic mass ratio between X and Y; (iv) two dimensional materials with reflection symmetry, such as singlelayer graphene, singlelayer boron nitride and carbon nanotubes; and (v) phonons with a large density of states, such as optical phonons, which are important for Raman, infrared and thermal radiative properties. Fourphonon scattering is expected to gain broad interest in various technologically important materials for thermoelectrics, thermal barrier coatings, thermal energy storage, phase change, nuclear power, ultrahigh temperature ceramics, infrared spectra, Raman spectra, radiative transport, hot electron relaxation and radiative cooling. Fourphonon scattering has been, and will continue to be, established as an important intrinsic phonon scattering mechanism beyond threephonon scattering. The prediction of fourphonon scattering will transition from a breakthrough to a new routine in the next decade.},
doi = {},
url = {https://www.osti.gov/biblio/1619009},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2020},
month = {3}
}