Ultralow glass-like lattice thermal conductivity in crystalline materials is crucial for enhancing energy conversion efficiency in thermoelectrics and thermal insulators. We introduce a universal descriptor for thermal conductivity that relies only on the atomic number in the primitive cell and the sound velocity, enabling fast and scalable materials screening. Coupled with high-throughput workflows and universal machine learning potentials, we identify the candidate materials with ultralow thermal conductivity from over 25, 000 materials. We further validate this approach by experimentally confirming record-low thermal conductivity values of 0.15-0.16 W/m·K from 170 to 400 K in the halide metal CsAg2I3. Combining inelastic neutron scattering with first-principles calculations, we attribute the ultralow thermal conductivity to the intrinsically small sound velocity, strong anharmonicity, and structural complexity. Our work illustrates how a universal descriptor, combined with high-throughput screening, machine-learning potential and experiment, enables the efficient discovery of materials with ultralow thermal conductivity.

CRISMAT CNRS Normandie Univ ENSICAEN UNICAEN Caen France

FZU Institute of Physics of the Czech Academy of Sciences Cukrovarnická 10 112 Prague Czech Republic

Institute Laue Langevin 71 avenue des Martyrs CS 20156 Grenoble Cedex 9 France

MOE Key Laboratory of Materials Physics and Chemistry under Extraordinary Conditions School of Physical Science and Technology Northwestern Polytechnical University Xi'an China

ShanghaiTech Laboratory for Topological Physics and School of Physical Science and Technology ShanghaiTech University Shanghai China

Thayer School of Engineering Dartmouth College Hanover NH USA

Université de Lorraine CNRS IJL Nancy France

Zobrazit více v PubMed

Bell, L. E. Cooling, heating, generating power, and recovering waste heat with thermoelectric systems. PubMed DOI

Padture, N. P., Gell, M. & Jordan, E. H. Thermal barrier coatings for gas-turbine engine applications. PubMed DOI

Qian, X., Zhou, J. & Chen, G. Phonon-engineered extreme thermal conductivity materials. PubMed DOI

Shi, Y., Assoud, A., Ponou, S., Lidin, S. & Kleinke, H. A new material with a composite crystal structure causing ultralow thermal conductivity and outstanding thermoelectric properties: Tl PubMed DOI

Peng, W., Petretto, G., Rignanese, G.-M., Hautier, G. & Zevalkink, A. An unlikely route to low lattice thermal conductivity: small atoms in a simple layered structure. DOI

Christensen, M. et al. Avoided crossing of rattler modes in thermoelectric materials. PubMed DOI

Li, C. W. et al. Orbitally driven giant phonon anharmonicity in SnSe. DOI

Skelton, J. M. et al. Anharmonicity in the high-temperature Cmcm phase of SnSe: soft modes and three-phonon interactions. PubMed DOI

Pal, K., He, J. & Wolverton, C. Bonding hierarchy gives rise to high thermoelectric performance in layered Zintl compound BaAu2P4. DOI

Mukhopadhyay, S. et al. Two-channel model for ultralow thermal conductivity of crystalline Tl PubMed DOI

Acharyya, P. et al. Glassy thermal conductivity in Cs PubMed DOI PMC

Gibson, Q. D. et al. Low thermal conductivity in a modular inorganic material with bonding anisotropy and mismatch. PubMed DOI

Shen, X. et al. Amorphous-like ultralow thermal transport in crystalline argyrodite Cu PubMed DOI PMC

Simoncelli, M., Marzari, N. & Mauri, F. Unified theory of thermal transport in crystals and glasses. DOI

Xia, Y., Ozoliņš, V. & Wolverton, C. Microscopic mechanisms of glasslike lattice thermal transport in cubic Cu PubMed DOI

Hanus, R. et al. Uncovering design principles for amorphous-like heat conduction using two-channel lattice dynamics. DOI

Xia, Z. et al. Realizing intrinsically ultralow and glass-like thermal transport via chemical bonding engineering. PubMed DOI PMC

Li, F. et al. Long-range anion correlations mediating dynamic anharmonicity and contributing to glassy thermal conductivity in well-ordered K PubMed DOI

Zheng, J. et al. Effects of high-order anharmonicity on anomalous lattice dynamics and thermal transport in fully filled skutterudite YbFe DOI

Yang, J., Jain, A. & Ong, W.-L. Inter-channel conversion between population-/coherence-channel dictates thermal transport in MAPbI3 crystals. DOI

Knoop, F., Purcell, T. A. R., Scheffler, M. & Carbogno, C. Anharmonicity in thermal insulators: an analysis from first principles. PubMed DOI

Zeng, Z. et al. Pushing thermal conductivity to its lower limit in crystals with simple structures. PubMed DOI PMC

Slack G. A. The Thermal Conductivity of Nonmetallic Crystals. In: Ehrenreich H., Seitz F., Turnbull D. (eds).

Callaway, J. Model for lattice thermal conductivity at low temperatures. DOI

Xia, Y. et al. A unified understanding of minimum lattice thermal conductivity. PubMed DOI PMC

Wang, X. et al. An interpretable formula for lattice thermal conductivity of crystals. DOI

Agne, M. T., Hanus, R. & Snyder, G. J. Minimum thermal conductivity in the context of diffuson-mediated thermal transport. DOI

Batatia, I. et al. A foundation model for atomistic materials chemistry. PubMed DOI

Chen, C. & Ong, S. P. A universal graph deep learning interatomic potential for the periodic table. PubMed DOI

Deng, B. et al. CHGNet as a pretrained universal neural network potential for charge-informed atomistic modelling. DOI

H. Yang. et al. MatterSim: a deep learning atomistic model across elements, temperatures and pressures.

Jain, A. et al. Commentary: the materials project: a materials genome approach to accelerating materials innovation. DOI

Li, W. et al. Low sound velocity contributing to the high thermoelectric performance of Ag PubMed DOI PMC

Simoncelli, M., Marzari, N. & Mauri, F. Wigner formulation of thermal transport in solids.

Peierls, R. Zur kinetischen Theorie der Wärmeleitung in Kristallen. DOI

Slack, G. A., Tanzilli, R. A., Pohl, R. O. & Vandersande, J. W. The intrinsic thermal conductivity of AIN. DOI

Ward, A., Broido, D. A., Stewart, D. A. & Deinzer, G. Ab initio theory of the lattice thermal conductivity in diamond. DOI

Steigmeier, E. F. & Kudman, I. Acoustical-optical phonon scattering in Ge, Si, and III-V compounds. DOI

Xiao, Y. et al. Origin of low thermal conductivity in SnSe. DOI

Zhang, J. et al. Direct observation of one-dimensional disordered diffusion channel in a chain-like thermoelectric with ultralow thermal conductivity. PubMed DOI PMC

Misra, S. et al. Reduced phase space of heat-carrying acoustic phonons in single-crystalline InTe. DOI

Zhu, J. et al. Vacancies tailoring lattice anharmonicity of Zintl-type thermoelectrics. PubMed DOI PMC

Acharyya, P. et al. Extended antibonding states and phonon localization induce ultralow thermal conductivity in low dimensional metal halide. DOI

Li, J. et al. First-principles studies of atomic dynamics in tetrahedrite thermoelectrics. DOI

Shen, X. et al. High-temperature structural and thermoelectric study of argyrodite Ag PubMed DOI

Li, F. et al. Overdamped phonon diffusion and nontrivial electronic structure leading to a high thermoelectric figure of merit in KCu PubMed DOI

Morelli, D. T., Jovovic, V. & Heremans, J. P. Intrinsically minimal thermal conductivity in Cubic I-V-VI PubMed DOI

Slack, G. A. Nonmetallic crystals with high thermal conductivity. DOI

Zheng, J. et al. Anharmonicity-induced phonon hardening and phonon transport enhancement in crystalline perovskite BaZrO DOI

Zheng, J. et al. Unravelling ultralow thermal conductivity in perovskite Cs DOI

Anderson, O. L. A simplified method for calculating the debye temperature from elastic constants. DOI

Lee, W. et al. Ultralow thermal conductivity in all-inorganic halide perovskites. PubMed DOI PMC

Cheng, R., Wang, C., Ouyang, N., Shen, X. & Chen, Y. Strong crystalline thermal insulation induced by extended antibonding states. PubMed DOI PMC

Hull, S. & Berastegui, P. Crystal structures and ionic conductivities of ternary derivatives of the silver and copper monohalides—II: ordered phases within the (AgX) DOI

Yao, M.-M. et al. Lead-Free Halide CsAg DOI

Jouini N., Guen L., Tournoux M. Structure Cristalline De Cscu2i3. (Springer, 1980).

Acharyya, P. et al. Intrinsically ultralow thermal conductivity in Ruddlesden–Popper 2D perovskite Cs PubMed DOI

Bhui, A. et al. Intrinsically low thermal conductivity in the n-Type vacancy-ordered double perovskite Cs DOI

Xie, H. et al. All-inorganic halide perovskites as potential thermoelectric materials: dynamic cation off-centering induces ultralow thermal conductivity. PubMed DOI

Shen, X. et al. Soft phonon mode triggering fast Ag diffusion in superionic argyrodite Ag PubMed DOI

Zheng J. et al. Wave-like tunneling of phonons dominates glass-like thermal transport in quasi-1D copper halide CsCu

Ioffe A., Regel A. Non-crystalline, amorphous, and liquid electronic semiconductors.

Elbaz, G. A. et al. Phonon speed, not scattering, differentiates thermal transport in lead halide perovskites. PubMed DOI

Rodríguez-Carvajal, J. Recent advances in magnetic structure determination by neutron powder diffraction. DOI

Roisnel, T. & Rodríquez-Carvajal, J. WinPLOTR: a windows tool for powder diffraction pattern analysis. DOI

Gemmi, M. et al. 3D electron diffraction: the nanocrystallography revolution. PubMed DOI PMC

Smeets, S., Zou, X. & Wan, W. Serial electron crystallography for structure determination and phase analysis of nanocrystalline materials. PubMed DOI PMC

Palatinus, L. et al. Specifics of the data processing of precession electron diffraction tomography data and their implementation in the program PETS2.0. PubMed DOI

Petříček V., Palatinus L., Plášil J., Dušek M. Jana2020 – a new version of the crystallographic computing system Jana.

Arnold, O. et al. Mantid—Data analysis and visualization package for neutron scattering and μ SR experiments. DOI

Hohenberg, P. & Kohn, W. Inhomogeneous electron gas. DOI

Kresse, G. & Furthmüller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. PubMed DOI

Blöchl, P. E. Projector augmented-wave method. PubMed DOI

Perdew, J. P. et al. Restoring the density-gradient expansion for exchange in solids and surfaces. PubMed DOI

Perdew, J. P., Burke, K. & Wang, Y. Generalized gradient approximation for the exchange-correlation hole of a many-electron system. PubMed DOI

Hellman, O. & Abrikosov, I. A. Temperature-dependent effective third-order interatomic force constants from first principles. DOI

Kim, D. S. et al. Nuclear quantum effect with pure anharmonicity and the anomalous thermal expansion of silicon. PubMed DOI PMC

Shulumba, N., Hellman, O. & Minnich, A. J. Lattice thermal conductivity of polyethylene molecular crystals from first-principles including nuclear quantum effects. PubMed DOI

Errea, I., Calandra, M. & Mauri, F. Anharmonic free energies and phonon dispersions from the stochastic self-consistent harmonic approximation: application to platinum and palladium hydrides. DOI

Tadano, T., Gohda, Y. & Tsuneyuki, S. Anharmonic force constants extracted from first-principles molecular dynamics: applications to heat transfer simulations. PubMed DOI

Tadano, T. & Tsuneyuki, S. Self-consistent phonon calculations of lattice dynamical properties in cubic SrTiO DOI

Hellman, O., Abrikosov, I. A. & Simak, S. I. Lattice dynamics of anharmonic solids from first principles. DOI

Nelson, L. J., Hart, G. L. W., Zhou, F. & Ozoliņš, V. Compressive sensing as a paradigm for building physics models. DOI

Tadano, T. & Tsuneyuki, S. Quartic anharmonicity of rattlers and its effect on lattice thermal conductivity of clathrates from first principles. PubMed DOI

Feng, T. & Ruan, X. Quantum mechanical prediction of four-phonon scattering rates and reduced thermal conductivity of solids. DOI

Han, Z., Yang, X., Li, W., Feng, T. & Ruan, X. FourPhonon: an extension module to ShengBTE for computing four-phonon scattering rates and thermal conductivity. DOI

Tamura, S. -i Isotope scattering of dispersive phonons in Ge. DOI

Allen, P. B. & Feldman, J. L. Thermal conductivity of disordered harmonic solids. PubMed DOI

Li, W., Carrete, J., A. Katcho, N. & Mingo, N. ShengBTE: a solver of the Boltzmann transport equation for phonons. DOI

Ganose, A. M. et al. Atomate2: modular workflows for materials science. PubMed DOI PMC

Shen X., Guilmeau E., Koza M. M., Weber F. Lattice dynamics and Ag diffusion in Ag

Momma, K. & Izumi, F. VESTA: a three-dimensional visualization system for electronic and structural analysis. DOI