Ultrafast carrier thermalization in lead iodide perovskite probed with two-dimensional electronic spectroscopy

In band-like semiconductors, charge carriers form a thermal energy distribution rapidly after optical excitation. In hybrid lead halide perovskites, the cooling of such thermal distributions has been reported to occur on timescales of ~300 fs via carrier-phonon scattering. However, the initial step of build-up of a thermal Boltzmann distribution proved difficult to resolve with conventional pump-probe techniques due to the requirement of high resolution both in time and in energy. Here, we use two-dimensional electronic spectroscopy with sub-10fs resolution to directly observe the initial carrier interactions that lead to the formation of a thermal carrier distribution. We find that thermalization occurs dominantly via carrier-carrier scattering and report the dependence of carrier scattering rates on excess energy and carrier density. We report carrier thermalization times in the range from 8 to 85 fs. These fast scattering processes limit the electronic coherence times in lead halide perovskite semiconductors.

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