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The surface chemistry and inter-connectivity within perovskite nanocrystalsplay a critical role in determining the electronic interactions. They manifestin the Coulomb screening of electron-hole correlations and the carrierrelaxation dynamics, among other many-body processes. Here, we characterize thecoupling between the exciton and free carrier states close to the band-edge ina ligand-free formamidinium lead bromide nanocrystal assembly viatwo-dimensional coherent spectroscopy. The optical signatures observed in thiswork show: (i) a nonlinear spectral lineshape reminiscent of Fano-likeinterference that evidences the coupling between discrete electronic states anda continuum, (ii) symmetric excited state absorption cross-peaks that suggestthe existence of a coupled exciton-carrier excited state, and (iii) ultrafastcarrier thermalization and exciton formation. Our results highlight thepresence of coherent coupling between exciton and free carriers, particularlyin the sub-100 femtosecond timescales.

Exciton-carrier coupling in a metal halide perovskite nanocrystal assembly probed by two-dimensional coherent spectroscopy