Accurate first-principles prediction of lattice thermal conductivity(κ_(L))remains challenging in identifying materials with extreme thermal behavior.While the harmonic approximation with threephonon scattering(HA+3p...Accurate first-principles prediction of lattice thermal conductivity(κ_(L))remains challenging in identifying materials with extreme thermal behavior.While the harmonic approximation with threephonon scattering(HA+3ph)is now routine,reliableκ_(L)prediction often requires higher-order anharmonic effects,including self-consistent phonon renormalization,three-and four-phonon scattering,and off-diagonal heat flux(SCPH+3,4ph+OD).We present a state-of-the-art highthroughput workflow that unifies these effects and apply it to 773 cubic and tetragonal crystals spanning diverse chemistries and structures.From 562 dynamically stable compounds,weassess the hierarchical impacts of higher-order anharmonicity.For around 60%of materials,HA+3ph predictions closely match those from SCPH+3,4ph+OD.SCPH generally increasesκ_(L),by over 8 times in extreme cases,whereas four-phonon scattering universally suppressesκ_(L),sometimes to 15%of the HA+3ph value.Off-diagonal contributions are negligible in high-κ_(L)systems but can rival diagonal terms in highly anharmonic low-κ_(L)compounds.We highlight four case studies,Rb_(2)TlAlH_(6),Cu_(3)VSe_(4),CuBr,and KTlCl_(4),that exhibit distinct extreme behaviors.This work delivers not only a robust workflow for high-fidelityκ_(L)dataset but also a quantitative framework to determine when higher-order effects are essential.The hierarchy ofκ_(L)results,from the HA+3ph to SCPH+3,4ph+OD level,offers a scalable,interpretable route to discovering next-generation extreme thermal materials.展开更多
基金support from the U.S. Department of Energy, Office of Science Basic Energy Sciences under grant DE-SC0024256. H. L. and Y. X. acknowledge the support from the US National Science Foundation through awards DMR-2317008+3 种基金. Y. X. also acknowledges the support from the Faculty Development Program at Portland State University. C.W. acknowledges support from the National Science Foundation (NSF) through award 2311203Z. L. and C. W. acknowledge computational resources from the National Energy Research Scientific Computing Center (NERSC) through award ERCAP0031557This research was supported in part through the computational resources and staff contributions provided for the Quest high performance computing facility at Northwestern University which is jointly supported by the Office of the Provost, the Office for Research, and Northwestern University Information Technology. We acknowledge the computing resources provided by Bridges2 at Pittsburgh Supercomputing Center (PSC) through allocations mat220006p, mat220008p, and dmr160027p from the Advanced Cyber-infrastructure Coordination Ecosystem: ServicesSupport (ACCESS) program, which is supported by National Science Foundation grants 2138259, 2138286, 2138307, 2137603, and 2138296.
文摘Accurate first-principles prediction of lattice thermal conductivity(κ_(L))remains challenging in identifying materials with extreme thermal behavior.While the harmonic approximation with threephonon scattering(HA+3ph)is now routine,reliableκ_(L)prediction often requires higher-order anharmonic effects,including self-consistent phonon renormalization,three-and four-phonon scattering,and off-diagonal heat flux(SCPH+3,4ph+OD).We present a state-of-the-art highthroughput workflow that unifies these effects and apply it to 773 cubic and tetragonal crystals spanning diverse chemistries and structures.From 562 dynamically stable compounds,weassess the hierarchical impacts of higher-order anharmonicity.For around 60%of materials,HA+3ph predictions closely match those from SCPH+3,4ph+OD.SCPH generally increasesκ_(L),by over 8 times in extreme cases,whereas four-phonon scattering universally suppressesκ_(L),sometimes to 15%of the HA+3ph value.Off-diagonal contributions are negligible in high-κ_(L)systems but can rival diagonal terms in highly anharmonic low-κ_(L)compounds.We highlight four case studies,Rb_(2)TlAlH_(6),Cu_(3)VSe_(4),CuBr,and KTlCl_(4),that exhibit distinct extreme behaviors.This work delivers not only a robust workflow for high-fidelityκ_(L)dataset but also a quantitative framework to determine when higher-order effects are essential.The hierarchy ofκ_(L)results,from the HA+3ph to SCPH+3,4ph+OD level,offers a scalable,interpretable route to discovering next-generation extreme thermal materials.
