Transient Suppression of Carrier Mobility Due to Hot Optical Phonons in Lead Bromide Perovskites.

In lead halide perovskites, owing to the strong Fröhlich coupling, carrier dynamics that governs the optoelectronic performance is greatly affected by the lattice vibrations. In this emerging class of materials, injected hot carriers quickly relax by emitting optical phonons, and if this process is sufficiently fast, hot optical phonons can be generated, which may in turn hamper the carrier transport. However, the transient interaction between hot phonons and carriers has not yet been investigated. Herein, we identified the transient absorption feature of hot phonons in lead bromide perovskites and then extracted the hot-phonon dynamics. The hot-phonon decay mechanism was uncovered by temperature-dependent measurements. The hot-phonon decay in lead bromide perovskites was an order of magnitude faster than that in GaAs, attributed to the large anharmonicity arising from the lattice softness and structural fluctuation. The carrier mobility was also transiently suppressed by hot phonons, and the mobility recovery was accompanied by the decay of hot phonons.