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Layered perovskites: sharp edges and excitons

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Layered perovskites: sharp edges and excitons

Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites
J.-C. Blancon, H. Tsai, W. Nie, C. C. Stoumpos, L. Pedesseau, C. Katan, M. Kepenekian, C. M. M. Soe, K. Appavoo, M. Y. Sfeir, S. Tretiak, P. M. Ajayan, M. G. Kanatzidis, J. Even, J. J. Crochet, A. D. Mohite
Science 2017, DOI: 10.1126/science.aal4211

Understanding and controlling charge and energy flow in state-of-the-art semiconductor quantum-wells has enabled high-efficiency optoelectronic devices. Two-dimensional Ruddlesden-Popper perovskites are solution-processed quantum-wells wherein the band gap can be tuned by varying the perovskite layer thickness, which modulates the effective electron-hole confinement. We report that, counterintuitive to classical quantum-confined systems where photo-generated electrons and holes are strongly bound by Coulomb interactions or excitons, the photo-physics of thin films made of Ruddlesden-Popper perovskites with a thickness exceeding two perovskite crystal-units (>1.3 nanometers) is dominated by lower energy states associated with the local intrinsic electronic structure of the edges of the perovskite layers. These states provide a direct pathway for dissociating excitons into longer-lived free-carriers that significantly improve the performance of optoelectronic devices.

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