Sponsor
Z.L. and C.W. acknowledge 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. Y. X. also acknowledges the support from the Faculty Development Program at Portland State University. C.W. acknowledges support fromtheNational Science Foundation (NSF) through award 2311203.Z. L. andC. W.acknowledge computational resources from the National Energy Research Scientific Computing Center (NERSC) through award ERCAP0031557. This research was supported in part throughthe computational resources andstaff contributionsprovidedfor the Quest high performance computing facility at NorthwesternUniversity 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: Services & Support (ACCESS) program, which is supported by National Science Foundation grants 2138259, 2138286, 2138307, 2137603, and 2138296.
Published In
Npj Computational Materials
Document Type
Article
Publication Date
2-1-2026
Subjects
Crystal lattices, Chemistry and Materials Science, Computational Intelligence, Conductivity, Crystals Cubic lattice Datasets Dynamic stability First principles Heat conductivity Heat flux Heat transfer Materials Science Mathematical and Computational Engineering Mathematical and Computational Physics, Mathematical Modeling and Industrial Mathematics, Phonons, Predictions
Abstract
Accurate first-principles prediction of lattice thermal conductivity (κ L) remains challenging in identifying materials with extreme thermal behavior. While the harmonic approximation with three-phonon scattering (HA + 3ph) is now routine, reliable κ 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 high-throughput workflow that unifies these effects and apply it to 773 cubic and tetragonal crystals spanning diverse chemistries and structures. From 562 dynamically stable compounds, we assess 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 increases κ L, by over 8 times in extreme cases, whereas four-phonon scattering universally suppresses κ 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, Rb2TlAlH6, Cu3VSe4, CuBr, and KTlCl4, that exhibit distinct extreme behaviors. This work delivers not only a robust workflow for high-fidelity κ L dataset but also a quantitative framework to determine when higher-order effects are essential. The hierarchy of κ L results, from the HA + 3ph to SCPH + 3, 4ph + OD level, offers a scalable, interpretable route to discovering next-generation extreme thermal materials.
Rights
Open Access
This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License, which permits any non-commercial use, sharing, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if you modified the licensed material. You do not have permission under this licence to share adapted material derived from this article or parts of it. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s CreativeCommons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/bync- nd/4.0/. © The Author(s) 2025
DOI
10.1038/s41524-025-01920-y
Persistent Identifier
https://archives.pdx.edu/ds/psu/44459
Publisher
Springer Science and Business Media LLC
Citation Details
Li, Z., Lee, H., Wolverton, C., & Xia, Y. (2025). High-throughput computational framework for high-order anharmonic thermal transport in cubic and tetragonal crystals. Npj Computational Materials, 12(1).