Authors: Yi Xia | Vinay I. Hegde | Koushik Pal | Xia Hua | Dale Gaines | Shane Patel | Jiangang He | Muratahan Aykol | Chris Wolverton
Source: Physical Review X (article, 2020-11-10)
Field: Materials Science — Materials Chemistry

High-Throughput Study of Lattice Thermal Conductivity in Binary Rocksalt and Zinc Blende Compounds Including Higher-Order Anharmonicity 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 ( L ) 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 L . 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 L . Our advanced theoretical model for computing L 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 L to be strikingly different in rocksalt and zinc blende compounds, owing to the countervailing effects on finitetemperature-induced shifts in phonon frequencies and scattering rates. By correlating L 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 L 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 L 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. Anharmonicity ; Condensed matter physics ; Phonon ; Quartic function ; Thermal conductivity ; Materials science ; Lattice (music) ; Physics ; Thermodynamics ; Mathematics Thermal properties of materials ; Advanced Thermoelectric Materials and Devices ; Machine Learning in Materials Science