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    Cation disorder in AgSbTe2 leads to glasslike ultralow lattice thermal conductivity

    Soongyu Kwon1,2, Sung Yi1, Soongkeun Hyun2, James M. Hodges3, and Yi Xia1,*

    • *Contact author: yxia@pdx.edu, yimaverickxia@gmail.com

    Phys. Rev. Applied 26, 014052 – Published 17 July, 2026

    DOI: https://doi.org/10.1103/vcln-3c8m

    Abstract

    Thermoelectric efficiency benefits from suppressing lattice thermal conductivity (κl), yet the microscopic origin of the glasslike ultralow κl in AgSbTe2 remains debated. Here we combine first-principles simulation of anharmonic lattice dynamics with the unified theory of thermal transport to quantify how Ag-Sb cation disorder controls heat conduction. We find that compared with cation-ordered L11 and D4 phases, disordered structures exhibit a strongly reduced κl across a wide temperature range [approximately equal to 0.48  W/(m K) at 300 K] and a much weaker temperature dependence (∝T−0.40). Our detailed analysis of the phonon spectrum and mode-resolved transport properties reveals that cation disorder disrupts the Te-centered octahedral network, softens phonons, lowers group velocities, and enhances low-frequency scattering, thus dramatically suppressing the diagonal (particlelike) contribution [approximately equal to 0.07  W/(m K)] while making the off-diagonal (wavelike) term dominant. Moreover, we performed a statistical analysis of κl of 434 dynamically stable cation-disordered configurations, which reveals a robust positive correlation between κl and the average frequency of acoustic modes. In addition, acoustic softening further correlates with increased Ag and Te participation and reduced participation ratios, indicating disorder-induced localization of heat-carrying modes. These results identify cation-disorder-driven localization and low-frequency scattering as key to the phonon-glass behavior of AgSbTe2, and suggest disorder engineering as a route to tune κl in multication thermoelectrics.

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