Controlling phonon lifetimes via sublattice disordering in $\mathrm{Ag}\mathrm{Bi}{\mathrm{Se}}_{2}$

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Controlling phonon lifetimes via sublattice disordering in $Ag Bi {Se}_{2}$

J. L. Niedziela, D. Bansal, J. Ding, T. Lanigan-Atkins, C. Li, A. F. May, H. Wang, J. Y. Y. Lin, D. L. Abernathy, G. Ehlers, A. Huq, D. Parshall, J. W. Lynn, and O. Delaire

Phys. Rev. Materials 4, 105402 – Published 12 October 2020

Abstract

Understanding and controlling microscopic heat transfer mechanisms in solids is critical to material design in numerous technological applications. Yet, the current understanding of thermal transport in semiconductors and insulators is limited by the difficulty in directly measuring individual phonon lifetimes and mean free paths, and studying their dependence on the microscopic state of the material. Here we report our measurements of microscopic phonon scattering rates in $Ag Bi {Se}_{2}$ , which exhibits a controllable, reversible change directly linked to microstructure evolution near a reversible structural phase transition, that directly impacts the thermal conductivity. We demonstrate a steplike doubling of phonon scattering rates resultant from the cation disordering at the structural transition. To rationalize the neutron scattering data, we leverage a stepwise approach to account for alterations to the thermal conductivity that are imparted by distinct scattering mechanisms. These results highlight the potential of tunable microstructures housed in a stable crystal matrix to provide a practical route to tailor phonon scattering to optimize thermal transport properties.

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Received 20 April 2020
Accepted 4 August 2020

DOI:https://doi.org/10.1103/PhysRevMaterials.4.105402

Physics Subject Headings (PhySH)

Acoustic phonons Lattice thermal conductivity Lifetimes & widths Microstructure Optical phonons Phonons Thermal conductivity

Disordered systems Functional materials Thermoelectrics

Density functional theory First-principles calculations Inelastic neutron scattering Neutron diffraction Time-of-flight neutron spectroscopy

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

J. L. Niedziela ^1,2,3,*, D. Bansal ², J. Ding², T. Lanigan-Atkins², C. Li⁴, A. F. May ¹, H. Wang¹, J. Y. Y. Lin ⁵, D. L. Abernathy ⁵, G. Ehlers⁵, A. Huq⁵, D. Parshall⁶, J. W. Lynn ⁶, and O. Delaire ^2,7,†

¹Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
²Department of Mechanical Engineering and Materials Science, Duke University, Durham, North Carolina 27708, USA
³Nuclear Nonproliferation Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
⁴Materials Science and Engineering, Department of Mechanical Engineering, University of California, Riverside, California 92521, USA
⁵Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
⁶NIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, Maryland 20899, USA
⁷Department of Physics and Department of Chemistry, Duke University, Durham, North Carolina 27708, USA

^*niedzielajl@ornl.gov
^†olivier.delaire@duke.edu

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Vol. 4, Iss. 10 — October 2020

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Physical Review Materials

Controlling phonon lifetimes via sublattice disordering in AgBiSe2

J. L. Niedziela, D. Bansal, J. Ding, T. Lanigan-Atkins, C. Li, A. F. May, H. Wang, J. Y. Y. Lin, D. L. Abernathy, G. Ehlers, A. Huq, D. Parshall, J. W. Lynn, and O. Delaire

Phys. Rev. Materials 4, 105402 – Published 12 October 2020

Abstract

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Controlling phonon lifetimes via sublattice disordering in $Ag Bi {Se}_{2}$