High-Throughput Study of Lattice Thermal Conductivity Including Higher-Order Anharmonicity

Thermal transport phenomena are ubiquitous and play a critical role in the performance of various microelectronic and energy-conversion devices. 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 many 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 a large number of compounds, 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 illustrate the physical insights gained from studies of a large number of binary rocksalt and zincblende compounds, Tl3VSe4, and Cu12Sb4S13.