Anomalous thermal transport under high pressure in boron arsenide
Suixuan Li,
Zihao Qin,
Huan Wu,
Man Li,
Martin Kunz,
Ahmet Alatas,
Abby Kavner and
Yongjie Hu ()
Additional contact information
Suixuan Li: University of California, Los Angeles
Zihao Qin: University of California, Los Angeles
Huan Wu: University of California, Los Angeles
Man Li: University of California, Los Angeles
Martin Kunz: Lawrence Berkeley National Laboratory
Ahmet Alatas: Argonne National Laboratory
Abby Kavner: University of California, Los Angeles
Yongjie Hu: University of California, Los Angeles
Nature, 2022, vol. 612, issue 7940, 459-464
Abstract:
Abstract High pressure represents extreme environments and provides opportunities for materials discovery1–8. Thermal transport under high hydrostatic pressure has been investigated for more than 100 years and all measurements of crystals so far have indicated a monotonically increasing lattice thermal conductivity. Here we report in situ thermal transport measurements in the newly discovered semiconductor crystal boron arsenide, and observe an anomalous pressure dependence of the thermal conductivity. We use ultrafast optics, Raman spectroscopy and inelastic X-ray scattering measurements to examine the phonon bandstructure evolution of the optical and acoustic branches, as well as thermal conductivity under varied temperatures and pressures up to 32 gigapascals. Using atomistic theory, we attribute the anomalous high-pressure behaviour to competitive heat conduction channels from interactive high-order anharmonicity physics inherent to the unique phonon bandstructure. Our study verifies ab initio theory calculations and we show that the phonon dynamics—resulting from competing three-phonon and four-phonon scattering processes—are beyond those expected from classical models and seen in common materials. This work uses high-pressure spectroscopy combined with atomistic theory as a powerful approach to probe complex phonon physics and provide fundamental insights for understanding microscopic energy transport in materials of extreme properties.
Date: 2022
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DOI: 10.1038/s41586-022-05381-x
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