Breaking Rayleigh's Law with Spatially Correlated Disorder to Control Phonon Transport

S. Thébaud, L. Lindsay, T. Berlijn

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3 Scopus citations

Abstract

Controlling thermal transport in insulators and semiconductors is crucial for many technological fields such as thermoelectrics and thermal insulation, for which a low thermal conductivity (κ) is desirable. A major obstacle for realizing low κ materials is Rayleigh's law, which implies that acoustic phonons, which carry most of the heat, are insensitive to scattering by point defects at low energy. We demonstrate, with large scale simulations on tens of millions of atoms, that isotropic long-range spatial correlations in the defect distribution can dramatically reduce phonon lifetimes of important low-frequency heat-carrying modes, leading to a large reduction of κ - potentially an order of magnitude at room temperature. We propose a general and quantitative framework for controlling thermal transport in complex functional materials through structural spatial correlations, and we establish the optimal functional form of spatial correlations that minimize κ. We end by briefly discussing experimental realizations of various correlated structures.

Original languageEnglish
Article number026301
JournalPhysical Review Letters
Volume131
Issue number2
DOIs
StatePublished - Jul 14 2023

Funding

We thank German Samolyuk for helpful discussions. This research was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. We used resources of the Compute and Data Environment for Science (CADES) at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC05-00OR22725.

FundersFunder number
CADESDE-AC05-00OR22725
Data Environment for Science
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Division of Materials Sciences and Engineering

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