Cation disorder in leads to glasslike ultralow lattice thermal conductivity
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 (), yet the microscopic origin of the glasslike ultralow in 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 and D4 phases, disordered structures exhibit a strongly reduced across a wide temperature range [approximately equal to at 300 K] and a much weaker temperature dependence (). 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 ] while making the off-diagonal (wavelike) term dominant. Moreover, we performed a statistical analysis of of 434 dynamically stable cation-disordered configurations, which reveals a robust positive correlation between 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 , and suggest disorder engineering as a route to tune in multication thermoelectrics.