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Two-dimensional (2D) perovskites with general formula $APbX_4$ are attractingincreasing interest as solution processable, white-light emissive materials.Recent studies have shown that their broadband emission is related to theformation of intra-gap color centers; however, the nature and dynamics of theemissive species have remained elusive. Here we show that the broadbandphotoluminescence of the 2D perovskites $(EDBE)PbCl_4$ and $(EDBE)PbBr_4$ stemsfrom the localization of small polarons within the lattice distortion field.Using a combination of spectroscopic techniques and first-principlescalculations, we infer the formation of ${Pb_2}^{3+}$, $Pb^{3+}$, and ${X_2}^-$(where X=Cl or Br) species confined within the inorganic perovskite framework.Due to strong Coulombic interactions, these species retain their originalexcitonic character and form self-trapped polaron-excitons acting as radiativecolor centers. These findings are expected to be applicable to a broad class ofwhite-light emitting perovskites with large polaron relaxation energy.

Polaron Self-localization in White-light Emitting Hybrid Perovskites