Revisiting lattice thermal transport in PbTe: The crucial role of quartic anharmonicity

By Yi Xia. Applied Physics Letters, 2018

132 citations recorded by the source corpus.

We perform a first-principles study of lattice thermal transport in PbTe by explicitly considering anharmonicity up to 4th order. To determine the temperature-dependent lattice constant of PbTe beyond quasiharmonic approximation, we introduce a simple yet effective scheme to account for anharmonic phonon renormalization at finite temperature. Moreover, we explicitly compute mode-resolved phonon lifetimes by including both three- and four-phonon scatterings. We find that (1) anharmonic phonon renormalization leads to strong vibrational frequency shifts which improve the agreement between simulated and experimental lattice constants; (2) these frequency shifts lead to a significant increase in lattice thermal conductivity (κl) because of reduced phonon scattering phase space; and (3) four-phonon scatterings are responsible for severe reduction in κl on top of three-phonon scatterings, making κl consistent with experiments. Our results suggest that the predicted κl and its temperature dependence without considering thermal expansion, anharmonic phonon renormalization and four-phonon scatterings could accidentally agree with experiments due to error cancellation. Our study not only deepens the understanding of lattice thermal transport in PbTe but also exemplifies a widely applicable approach to investigate lattice dynamics and thermal transport properties from first-principles calculations including high-order anharmonicity.We perform a first-principles study of lattice thermal transport in PbTe by explicitly considering anharmonicity up to 4th order. To determine the temperature-dependent lattice constant of PbTe beyond quasiharmonic approximation, we introduce a simple yet effective scheme to account for anharmonic phonon renormalization at finite temperature. Moreover, we explicitly compute mode-resolved phonon lifetimes by including both three- and four-phonon scatterings. We find that (1) anharmonic phonon renormalization leads to strong vibrational frequency shifts which improve the agreement between simulated and experimental lattice constants; (2) these frequency shifts lead to a significant increase in lattice thermal conductivity (κl) because of reduced phonon scattering phase space; and (3) four-phonon scatterings are responsible for severe reduction in κl on top of three-phonon scatterings, making κl consistent with experiments. Our results suggest that the predicted κl and its temperature dependence without cons...

Subfields: Materials Chemistry

View Paper: https://www.semanticscholar.org/paper/ada579d4d4761dcc1a4458f06994f31f973a6bdf

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In Materials Chemistry

1. C. Hua
2. S. Lee
3. X. Ruan
4. L. Lindsay
5. T. Ala‐Nissila
6. Haikuan Dong
7. Zezhu Zeng
8. Zheyong Fan

Citations in the corpus

• Survey of ab initio phonon thermal transport (2018, background): “This method has been used to examine thermal transport in PbS, PbSe, and PbTe [87] and LiH and LiF [56].”
• Neuroevolution machine learning potentials: Combining high accuracy and low cost in atomistic simulations and application to heat transport (2021, methodology): “…with the NEP potential, from BTE calculations with the GAP-SOAP potential considering both three-phonon and four-phonon scat-terings [59], from BTE-DFT calculations considering three-phonon scattering only or both three-phonon and four-phonon scatterings [90], and from experiments [91, 92].”