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Liquid-like thermal conduction in intercalated layered crystalline solids

Nature Materials volume 17, pages 226–230 (2018)Cite this article

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Abstract

As a generic property, all substances transfer heat through microscopic collisions of constituent particles1. A solid conducts heat through both transverse and longitudinal acoustic phonons, but a liquid employs only longitudinal vibrations2,3. As a result, a solid is usually thermally more conductive than a liquid. In canonical viewpoints, such a difference also serves as the dynamic signature distinguishing a solid from a liquid. Here, we report liquid-like thermal conduction observed in the crystalline AgCrSe2. The transverse acoustic phonons are completely suppressed by the ultrafast dynamic disorder while the longitudinal acoustic phonons are strongly scattered but survive, and are thus responsible for the intrinsically ultralow thermal conductivity. This scenario is applicable to a wide variety of layered compounds with heavy intercalants in the van der Waals gaps, manifesting a broad implication on suppressing thermal conduction. These microscopic insights might reshape the fundamental understanding on thermal transport properties of matter and open up a general opportunity to optimize performances of thermoelectrics.

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Fig. 1: Structures and phase transition.
Fig. 2: Thermally populated occupational disorder of Ag atoms.
Fig. 3: Experimental and theoretical results of phonons.
Fig. 4: Suppression of TA phonons.
Fig. 5: Controllable occupational orders in A+TM3+X2−2.

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Acknowledgements

We acknowledge the award of beam time from the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory, via proposal IPTS-13971, from SPring-8 via proposal no. 2015B1070, and from J-PARC via proposal no. 2012P0906. H.W. and R.Q.W. were supported by DOE-BES (grant no. DE-FG02-05ER46237) and the computer simulations were supported by the National Energy Research Scientific Computing Center (NERSC). Ames Laboratory is operated for the US Department of Energy by Iowa State University under contract no. DE-AC02-07CH11358. D.W. and J.Q.H. were supported by the Natural Science Foundation of Guangdong Province (grant no. 2015A030308001) and the leading talents programme of Guangdong Province (grant no. 00201517). H.L.Y. and Y.C. acknowledge the research computing facilities offered by ITS, HKU. We thank M. Kofu for the fruitful discussion.

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Authors and Affiliations

  1. J-PARC Center, Japan Atomic Energy Agency, Tokai, Ibaraki, Japan

    B. Li, Y. Kawakita, T. Kikuchi, K. Shibata & K. Nakajima

  2. Department of Physics and Astronomy, University of California, Irvine, California, USA

    H. Wang & R. Q. Wu

  3. Ames Laboratory and Department of Physics and Astronomy, Iowa State University, Ames, Iowa, USA

    Q. Zhang & D. Vaknin

  4. Jülich Center for Neutron Science, Forschungszentrum Jülich GmbH, Jülich, Germany

    M. Feygenson

  5. Department of Mechanical Engineering, The University of Hong Kong, Hong Kong SAR, China

    H. L. Yu & Y. Chen

  6. Department of Physics, Southern University of Science and Technology (SUSTech), Shenzhen, China

    D. Wu & J. Q. He

  7. SPring-8, Japan Synchrotron Radiation Research Institute, Sayo, Hyogo, Japan

    K. Ohara

  8. Neutron Science and Technology Center, Comprehensive Research Organization for Science and Society (CROSS), Tokai, Ibaraki, Japan

    T. Yamada

  9. Hebei Key Lab of Optic-electronic Information and Materials, The College of Physics Science and Technology, Hebei University, Baoding, China

    X. K. Ning

  10. Department of Chemistry, Northwestern University, Evanston, Illinois, USA

    M. G. Kanatzidis

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  1. B. Li
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Contributions

B.L. and H.W. planned the project. Q.Z., D.V., D.W. and J.Q.H. synthesized two samples. D.W. and J.Q.H. carried out thermoelectric measurements. X.K.N. measured the low-temperature specific heat and carried out transmission electron microscopy observation. For the sample made by Q.Z. and D.V., M.F. performed neutron powder diffraction measurements, B.L., Y.K. and K.O. collected X-ray scattering data, and B.L., Y.K., T.K., K.S., T.Y. and K.N. performed inelastic neutron scattering measurements. H.W., H.L.Y., Y.C. and R.Q.W. performed theoretical calculations. B.L., H.W., J.Q.H. and M.G.K. interpreted all results and wrote the manuscript with discussion and input from all coauthors.

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Correspondence to B. Li, H. Wang, J. Q. He or M. G. Kanatzidis.

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Li, B., Wang, H., Kawakita, Y. et al. Liquid-like thermal conduction in intercalated layered crystalline solids. Nature Mater 17, 226–230 (2018). https://doi.org/10.1038/s41563-017-0004-2

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