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Origin of reduced thermal conduction by native point defects in PbTe: Perturbed molecular dynamics with neural network potential

Tatsuya Yokoi1,*, Susumu Fujii2,3,†, Yu Ogura1, and Katsuyuki Matsunaga1,3

  • *Contact author: yokoi@mp.pse.nagoya-u.ac.jp
  • †Contact author: fujii.susumu.878@m.kyushu-u.ac.jp
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Phys. Rev. B 112, 024111 – Published 24 July, 2025

DOI: https://doi.org/10.1103/1175-sd2m

Abstract

Native point defects are fundamental building blocks of defect engineering in thermoelectric materials. However, it remains unclear which changes induced by point defects reduce lattice thermal conductivity κl at the atomic level. This study develops a neural-network potential (NNP) trained on density functional theory data for lead telluride (PbTe) and applies it to equilibrium and perturbed molecular dynamics (PMD) simulations. Isolated Pb and Te vacancies, antisites, interstitials and Schottky pairs are examined using sufficiently large supercells. The NNP is shown to reproduce harmonic and anharmonic vibrational properties and to accurately predict potential energy and atomic forces at finite temperatures. NNP-based PMD simulations reveal that local thermal transport near defects varies significantly depending on the defect type, exhibiting the lowest κl for interstitial Pb. Atom-resolved κl of point defects and their neighboring atoms correlate with the integrated absolute difference in vibrational density of states between those atoms and bulk atoms. This trend appears even within the harmonic approximation, which neglects anharmonic contributions. This suggests that the difference between the harmonic potential energies of pristine and defect-containing PbTe plays a central role in reducing κl, by modifying the force field around point defects through the second-order force constant. In contrast, atomic displacements around point defects show a weak correlation with atom-resolved κl and thus may not be a suitable metric for predicting κl of defect-containing PbTe, although relevant quantities are assumed to affect κl in conventional analytical models. The present NNP enables us to analyze physical quantities accessible via molecular simulations with high accuracy and to understand the underlying mechanisms of thermal transport reduction by point defects, without relying on analytical models.

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Phys. Rev. B 112, 024111– Published 24 July, 2025
  • Received 27 March 2025
  • Revised 13 May 2025
  • Accepted 15 July 2025
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