Glassy thermal conductivity in Cs3Bi2I6Cl3 single crystal

Paribesh Acharyya, Tanmoy Ghosh, Koushik Pal, Kewal Singh Rana, Moinak Dutta, Diptikanta Swain, Martin Etter, Ajay Soni, Umesh V. Waghmare and Kanishka Biswas ()
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Paribesh Acharyya: New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR)
Tanmoy Ghosh: New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR)
Koushik Pal: Theoretical Science Unit, Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR)
Kewal Singh Rana: Indian Institute of Technology Mandi
Moinak Dutta: New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR)
Diptikanta Swain: Institute of Chemical Technology-IndianOil Odisha Campus
Martin Etter: Deutsches Elektronen-Synchrotron (DESY)
Ajay Soni: Indian Institute of Technology Mandi
Umesh V. Waghmare: Theoretical Science Unit, Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR)
Kanishka Biswas: New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR)

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract As the periodic atomic arrangement of a crystal is made to a disorder or glassy-amorphous system by destroying the long-range order, lattice thermal conductivity, κL, decreases, and its fundamental characteristics changes. The realization of ultralow and unusual glass-like κL in a crystalline material is challenging but crucial to many applications like thermoelectrics and thermal barrier coatings. Herein, we demonstrate an ultralow (~0.20 W/m·K at room temperature) and glass-like temperature dependence (2–400 K) of κL in a single crystal of layered halide perovskite, Cs3Bi2I6Cl3. Acoustic phonons with low cut-off frequency (20 cm−1) are responsible for the low sound velocity in Cs3Bi2I6Cl3 and make the structure elastically soft. While a strong anharmonicity originates from the low energy and localized rattling-like vibration of Cs atoms, synchrotron X-ray pair-distribution function evidence a local structural distortion in the Bi-halide octahedra and Cl vacancy. The hierarchical chemical bonding and soft vibrations from selective sublattice leading to low κL is intriguing from lattice dynamical perspective as well as have potential applications.

Date: 2022
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DOI: 10.1038/s41467-022-32773-4

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