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Hybrid organic-inorganic semiconductors feature complex lattice dynamics dueto the ionic character of the crystal and the softness arising fromnon-covalent bonds between molecular moieties and the inorganic network. Herewe establish that such dynamic structural complexity in a prototypicaltwo-dimensional lead iodide perovskite gives rise to the coexistence of diverseexcitonic resonances, each with a distinct degree of polaronic character. Bymeans of high-resolution resonant impulsive stimulated Raman spectroscopy, weidentify vibrational wavepacket dynamics that evolve along differentconfigurational coordinates for distinct excitons and photocarriers. Employingdensity functional theory calculations, we assign the observed coherentvibrational modes to various low-frequency ($\lesssim 50$\,cm$^{-1}$) opticalphonons involving motion in the lead-iodide layers. We thus conclude thatdifferent excitons induce specific lattice reorganizations, which aresignatures of polaronic binding. This insight on the energetic/configurationallandscape involving globally neutral primary photoexcitations may be relevantto a broader class of emerging hybrid semiconductor materials.

Phonon coherences reveal the polaronic character of excitons in two-dimensional lead-halide perovskites