The optical response of 2D layered perovskites is composed of multiple equally-spaced spectral features, often interpreted as phonon replicas, separated by an energy Δ ≃ 15−40 meV, depending upon the compound. We show that the characteristic energy spacing, seen in both absorption and emission, is correlated with a substantial scattering response above ≃200 cm−1 (≃25 meV) observed in resonant Raman. This peculiar high-frequency signal, which dominates both Stokes and anti-Stokes regions of the scattering spectra, possess the characteristic spectral fingerprints of polarons. Notably, its spectral position is shifted away from the Rayleigh line, with a tail on the high energy side. The internal structure of the polaron consists of a series of equidistant signals separated by 25-32 cm−1 (3-4 meV), depending upon the compound, forming a polaron vibronic progression. The observed progression is characterized by a large Huang-Rhys factor (S >6) for all of the 2D layered perovskites investigated here, indicative of a strong charge carrier – lattice coupling.
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