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Understanding lattice dynamics and thermal transport mechanisms in cubic hybrid organic–inorganic perovskites remain challenging due to strong anharmonicity and phase transitions. Here, we investigate the thermal transport behavior in benchmark cubic hybrid perovskite FAPbI3 by coupling first principles-based anharmonic lattice dynamics with a linearized Wigner transport equation. Using the Temperature-Dependent Effective Potential (TDEP) method, we stabilize the negative soft modes, primarily dominated by organic FA+ cations. Our calculations predict an ultra-low thermal conductivity of ~ 0. 63\, W{m}^-1{K}^-1 at 300 K, following a temperature dependence of T−0. 740. Contrary to common assumptions, we find that the PbI31- units, rather than FA+ cations, dominate thermal resistance. Furthermore, we demonstrate that anharmonic force constants are highly temperature-sensitive, relying on 0-K force constants significantly underestimates thermal conductivity. Our study not only elucidates the microscopic mechanisms governing thermal transport in FAPbI3 but also provides a robust framework for modeling heat conduction in hybrid organic-inorganic compounds.
Zheng et al. (Thu,) studied this question.