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Hybrid organic-inorganic perovskites (HOIPs) have become an important classof semiconductors for solar cells and other optoelectronic applications.Electron-phonon coupling plays a critical role in all optoelectronic devices,and although the lattice dynamics and phonon frequencies of HOIPs have beenwell studied, little attention has been given to phonon lifetimes. We reportthe first high-precision measurements of acoustic phonon lifetimes in thehybrid perovskite methylammonium lead iodide (MAPI), using inelastic neutronspectroscopy to provide high energy resolution and fully deuterated singlecrystals to reduce incoherent scattering from hydrogen. Our measurements revealextremely short lifetimes on the order of picoseconds, corresponding tonanometer mean free paths and demonstrating that acoustic phonons are unable todissipate heat efficiently. Lattice-dynamics calculations using ab-initiothird-order perturbation theory indicate that the short lifetimes stem fromstrong three-phonon interactions and a high density of low-energy opticalphonon modes related to the degrees of freedom of the organic cation. Suchshort lifetimes have significant implications for electron-phonon coupling inMAPI and other HOIPs, with direct impacts on optoelectronic devices both in thecooling of hot carriers and in the transport and recombination of band edgecarriers. These findings illustrate a fundamental difference between HOIPs andconventional photovoltaic semiconductors and demonstrate the importance ofunderstanding lattice dynamics in the effort to develop metal halide perovskiteoptoelectronic devices.

Acoustic Phonon Lifetimes Limit Thermal Transport in Methylammonium Lead Iodide