High-Throughput Study of Lattice Thermal Conductivity in Binary Rocksalt and Zinc Blende Compounds including Higher-Order Anharmonicity

Yi Xia*, Vinay I. Hegde, Koushik Pal, Xia Hua, Dale Gaines, Shane Patel, Jiangang He, Muratahan Aykol, Chris Wolverton*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

125 Scopus citations

Abstract

Thermal transport phenomena are ubiquitous and play a critical role in the performance of various microelectronic and energy-conversion devices. Binary rocksalt and zinc blende compounds, despite their rather simple crystal structures, exhibit an extraordinary range of lattice thermal conductivity (κL) spanning over 3 orders of magnitude. A comprehensive understanding of the underlying heat transfer mechanism through the development of microscopic theories is therefore of fundamental importance, yet it remains elusive because of the challenges arising from explicitly treating higher-order anharmonicity. Recent theoretical and experimental advances have revealed the essential role of quartic anharmonicity in suppressing heat transfer in zinc blende boron arsenide (BAs) with ultrahigh κL. However, critical questions concerning the general effects of higher-order anharmonicity in the broad classes and chemistries of binary solids are still unanswered. Using our recently developed high-throughput phonon framework based on first-principles density functional theory calculations, we systematically investigate the lattice dynamics and thermal transport properties of 37 binary compounds with rocksalt and zinc blende structures at room temperature, with a particular focus on unraveling the impacts of quartic anharmonicity on κL. Our advanced theoretical model for computing κL embraces current state-of-the-art methods, featuring a complete treatment of quartic anharmonicity for both phonon frequencies and lifetimes at finite temperatures, as well as contributions from off-diagonal terms in the heat-flux operator. We find the impacts of quartic anharmonicity on κL to be strikingly different in rocksalt and zinc blende compounds, owing to the countervailing effects on finite-temperature-induced shifts in phonon frequencies and scattering rates. By correlating κL with the phonon scattering phase space, we outline a qualitative but efficient route to assess the importance of four-phonon scattering from harmonic phonon calculations. Among notable examples, in zinc blende HgTe, we identify an unprecedented sixfold reduction in κL due to four-phonon scattering, which dominates over the three-phonon scattering in the acoustic region at room temperature. We also demonstrate a possible breakdown of the phonon gas model in rocksalt AgCl, wherein the phonon states are significantly broadened due to strong intrinsic anharmonicity, inducing off-diagonal contributions to κL comparable to the diagonal ones. The deep physical insights gained in this work can be used to guide the rational design of thermal management materials.

Original languageEnglish (US)
Article number041029
JournalPhysical Review X
Volume10
Issue number4
DOIs
StatePublished - Nov 10 2020

Funding

The authors acknowledge financial support received from (i) Toyota Research Institute (TRI) through the Accelerated Materials Design and Discovery program (development of high-throughput framework for lattice dynamics and thermal conductivity calculations), (ii) the Department of Energy, Office of Science, Basic Energy Sciences under Grant No. DE-SC0014520 (theory of anharmonic phonons), and (iii) the U.S. Department of Commerce and National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) under Grant No. 70NANB14H012 (DFT calculations). This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy (U.S. Department of Energy Contract No. DE-AC02-05CH11231) and the Extreme Science and Engineering Discovery Environment (National Science Foundation Contract No. ACI-1548562).

ASJC Scopus subject areas

  • General Physics and Astronomy

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