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  • Open Access

Lattice thermal transport from phonon spectra beyond perturbation theory

Zezhu Zeng1,*, Michele Simoncelli2, and David E. Manolopoulos1

  • 1Physical and Theoretical Chemistry Laboratory, Department of Chemistry, University of Oxford, Oxford OX1 3QZ, United Kingdom
  • 2Department of Applied Physics and Applied Mathematics, Columbia University, New York, New York 10027, USA

  • *Contact author: zezhu.zeng@chem.ox.ac.uk
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Phys. Rev. B 114, 204303 – Published 9 October, 2026

DOI: https://doi.org/10.1103/bjh1-xb7z

Abstract

We develop a molecular dynamics framework to compute the mode-resolved phonon spectral density from classical correlations of an annihilation-like phonon variable. For harmonic oscillators, classical molecular dynamics exactly reproduces the corresponding quantum Kubo-transformed correlator, providing the basis for extension to anharmonic systems. Using PbTe as a benchmark and Cs3Bi2I6Cl3 as a strongly anharmonic test case, we show that the method captures both quasiparticle and non-Lorentzian spectra beyond perturbative quasiparticle theory, while yielding thermal conductivity in good agreement with experiment. This framework provides a classical molecular dynamics route to mode-resolved phonon spectral densities for spectral Wigner heat transport in strongly anharmonic solids above their Debye temperatures.

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Outline

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Phys. Rev. B 114, 204303– Published 9 October, 2026
  • Received 21 April 2026
  • Revised 27 July 2026
  • Accepted 18 September 2026
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