High frequency atomic tunneling yields ultralow and glass-like thermal conductivity in chalcogenide single crystals

Bo Sun, Shanyuan Niu, Raphael P. Hermann, Jaeyun Moon, Nina Shulumba, Katharine Page, Boyang Zhao, Arashdeep S. Thind, Krishnamurthy Mahalingam, JoAnna Milam-Guerrero, Ralf Haiges, Matthew Mecklenburg, Brent C. Melot, Young-Dahl Jho, Brandon M. Howe, Rohan Mishra, Ahmet Alatas, Barry Winn, Michael E. Manley (), Jayakanth Ravichandran () and Austin J. Minnich ()
Additional contact information
Bo Sun: California Institute of Technology
Shanyuan Niu: University of Southern California
Raphael P. Hermann: Oak Ridge National Laboratory
Jaeyun Moon: California Institute of Technology
Nina Shulumba: California Institute of Technology
Katharine Page: Oak Ridge National Laboratory
Boyang Zhao: University of Southern California
Arashdeep S. Thind: Washington University in St. Louis
Krishnamurthy Mahalingam: Air Force Research Laboratory
JoAnna Milam-Guerrero: University of Southern California
Ralf Haiges: University of Southern California
Matthew Mecklenburg: University of Southern California
Brent C. Melot: University of Southern California
Young-Dahl Jho: Gwangju Institute of Science and Technology
Brandon M. Howe: Air Force Research Laboratory
Rohan Mishra: Washington University in St. Louis
Ahmet Alatas: Argonne National Laboratory
Barry Winn: Oak Ridge National Laboratory
Michael E. Manley: Oak Ridge National Laboratory
Jayakanth Ravichandran: University of Southern California
Austin J. Minnich: California Institute of Technology

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract Crystalline solids exhibiting glass-like thermal conductivity have attracted substantial attention both for fundamental interest and applications such as thermoelectrics. In most crystals, the competition of phonon scattering by anharmonic interactions and crystalline imperfections leads to a non-monotonic trend of thermal conductivity with temperature. Defect-free crystals that exhibit the glassy trend of low thermal conductivity with a monotonic increase with temperature are desirable because they are intrinsically thermally insulating while retaining useful properties of perfect crystals. However, this behavior is rare, and its microscopic origin remains unclear. Here, we report the observation of ultralow and glass-like thermal conductivity in a hexagonal perovskite chalcogenide single crystal, BaTiS3, despite its highly symmetric and simple primitive cell. Elastic and inelastic scattering measurements reveal the quantum mechanical origin of this unusual trend. A two-level atomic tunneling system exists in a shallow double-well potential of the Ti atom and is of sufficiently high frequency to scatter heat-carrying phonons up to room temperature. While atomic tunneling has been invoked to explain the low-temperature thermal conductivity of solids for decades, our study establishes the presence of sub-THz frequency tunneling systems even in high-quality, electrically insulating single crystals, leading to anomalous transport properties well above cryogenic temperatures.

Date: 2020
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DOI: 10.1038/s41467-020-19872-w

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