TY - JOUR
T1 - Edge stabilization in reduced-dimensional perovskites
AU - Na Quan, Li
AU - Ma, Dongxin
AU - Zhao, Yongbiao
AU - Voznyy, Oleksandr
AU - Yuan, Haifeng
AU - Bladt, Eva
AU - Pan, Jun
AU - García de Arquer, F. Pelayo
AU - Sabatini, Randy
AU - Piontkowski, Zachary
AU - Emwas, Abdul Hamid
AU - Todorović, Petar
AU - Quintero-Bermudez, Rafael
AU - Walters, Grant
AU - Fan, James Z.
AU - Liu, Mengxia
AU - Tan, Hairen
AU - Saidaminov, Makhsud I.
AU - Gao, Liang
AU - Li, Yiying
AU - Anjum, Dalaver H.
AU - Wei, Nini
AU - Tang, Jiang
AU - McCamant, David W.
AU - Roeffaers, Maarten B.J.
AU - Bals, Sara
AU - Hofkens, Johan
AU - Bakr, Osman M.
AU - Lu, Zheng Hong
AU - Sargent, Edward H.
N1 - Funding Information:
This publication is based in part on work supported by an award (KUS-11-009-21) from the King Abdullah University of Science and Technology (KAUST), by the Ontario Research Fund Research Excellence Program, by the Ontario Research Fund (ORF), by the Natural Sciences and Engineering Research Council (NSERC) of Canada, and by the US Department of Navy, Office of Naval Research (Grant Award No. N00014-17-1-2524). H.Y. acknowledges the Research Foundation-Flanders (FWO Vlaanderen) for a postdoctoral fellowship. E.B. gratefully acknowledges financial support by the Research Foundation-Flanders (FWO Vlaanderen). S.B. acknowledges financial support from European Research Council (ERC Starting Grant #815128-REALNANO). M.B.J.R. and J.H. acknowledge the Research Foundation-Flanders (FWO, Grants G.0962.13, G.0B39.15, AKUL/11/14 and G0H6316N), KU Leuven Research Fund (C14/15/053) and the European Research Council under the European Union’s Seventh Framework Programme (FP/2007-2013)/ERC Grant Agreement No. [307523], ERC-Stg LIGHT to M.B.J.R. DFT calculations were performed on the IBM BlueGene Q supercomputer with support from the Southern Ontario Smart Computing Innovation Platform (SOSCIP). M.I.S. acknowledges the Banting Postdoctoral Fellowship program from the Natural Sciences and Engineering Research Council of Canada (NSERC). H.T. acknowledges the Netherlands Organisation for Scientific Research (NWO) for a Rubicon grant (680-50-1511).
Publisher Copyright:
© 2020, The Author(s).
PY - 2020/12/1
Y1 - 2020/12/1
N2 - Reduced-dimensional perovskites are attractive light-emitting materials due to their efficient luminescence, color purity, tunable bandgap, and structural diversity. A major limitation in perovskite light-emitting diodes is their limited operational stability. Here we demonstrate that rapid photodegradation arises from edge-initiated photooxidation, wherein oxidative attack is powered by photogenerated and electrically-injected carriers that diffuse to the nanoplatelet edges and produce superoxide. We report an edge-stabilization strategy wherein phosphine oxides passivate unsaturated lead sites during perovskite crystallization. With this approach, we synthesize reduced-dimensional perovskites that exhibit 97 ± 3% photoluminescence quantum yields and stabilities that exceed 300 h upon continuous illumination in an air ambient. We achieve green-emitting devices with a peak external quantum efficiency (EQE) of 14% at 1000 cd m−2; their maximum luminance is 4.5 × 104 cd m−2 (corresponding to an EQE of 5%); and, at 4000 cd m−2, they achieve an operational half-lifetime of 3.5 h.
AB - Reduced-dimensional perovskites are attractive light-emitting materials due to their efficient luminescence, color purity, tunable bandgap, and structural diversity. A major limitation in perovskite light-emitting diodes is their limited operational stability. Here we demonstrate that rapid photodegradation arises from edge-initiated photooxidation, wherein oxidative attack is powered by photogenerated and electrically-injected carriers that diffuse to the nanoplatelet edges and produce superoxide. We report an edge-stabilization strategy wherein phosphine oxides passivate unsaturated lead sites during perovskite crystallization. With this approach, we synthesize reduced-dimensional perovskites that exhibit 97 ± 3% photoluminescence quantum yields and stabilities that exceed 300 h upon continuous illumination in an air ambient. We achieve green-emitting devices with a peak external quantum efficiency (EQE) of 14% at 1000 cd m−2; their maximum luminance is 4.5 × 104 cd m−2 (corresponding to an EQE of 5%); and, at 4000 cd m−2, they achieve an operational half-lifetime of 3.5 h.
UR - https://www.scopus.com/pages/publications/85077680403
U2 - 10.1038/s41467-019-13944-2
DO - 10.1038/s41467-019-13944-2
M3 - Article
C2 - 31924790
AN - SCOPUS:85077680403
SN - 2041-1723
VL - 11
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 170
ER -