@article{3d3df13275374379b196017eec035c1f,
title = "Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites",
abstract = "Understanding and controlling charge and energy flow in state-of-the-art semiconductor quantum wells has enabled high-efficiency optoelectronic devices. Two-dimensional (2D) 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 photogenerated electrons and holes are strongly bound by Coulomb interactions or excitons, the photophysics 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 substantially improve the performance of optoelectronic devices.",
author = "Blancon, {J. C.} and H. Tsai and W. Nie and Stoumpos, {C. C.} and L. Pedesseau and C. Katan and M. Kepenekian and Soe, {C. M.M.} and K. Appavoo and Sfeir, {M. Y.} and S. Tretiak and Ajayan, {P. M.} and Kanatzidis, {M. G.} and J. Even and Crochet, {J. J.} and Mohite, {A. D.}",
note = "Funding Information: The work at Los Alamos National Laboratory (LANL) was supported by the LANL Laboratory Directed Research and Development (LDRD) program (J.-C.B., W.N., S.T., and A.D.M.) and was partially performed at the Center for Nonlinear Studies. The work was conducted, in part, at the Center for Integrated Nanotechnologies (CINT), a U.S. Department of Energy (DOE), Office of Science user facility. Work at Northwestern University was supported by grant SC0012541 from the U.S. DOE, Office of Science. The work in France was supported by Cellule Energie du CNRS (SOLHYBTRANS Project) and University of Rennes 1 (Action Incitative, D{\'e}fis Scientifique Emergents 2015). This research used resources of the Center for Functional Nanomaterials, which is a U.S. DOE Office of Science facility, at Brookhaven National Laboratory under contract no. DE-SC0012704. J.-C.B., A.D.M., and J.J.C. conceived the idea, designed the experiments, and wrote the manuscript. H.T. and W.N. fabricated thin films and performed all device measurements and analysis. J.E., C.K., and S.T. analyzed the data and performed Heyd-Scuseria-Ernzerhof screened-exchange hybrid functional calculations with support from M.K. and L.P. and provided insight into the mechanisms. M.G.K., C.C.S., and C.M.M.S. developed the chemistry for the synthesis of phase-pure crystals and provided insight into the chemical origin of the edge states. M.S. and K.A. performed several complementary measurements to provide insight into the mechanisms and to validate the observed findings. P.M.A. provided insights into the origin of edge states. All authors contributed to this work, read the manuscript, and agree to its contents, and all data are reported in the main text and supplementary materials.",
year = "2017",
month = mar,
day = "24",
doi = "10.1126/science.aal4211",
language = "English (US)",
volume = "355",
pages = "1288--1292",
journal = "Science",
issn = "0036-8075",
publisher = "American Association for the Advancement of Science",
number = "6331",
}