Abstract
A major efficiency limit for solution-processed perovskite optoelectronic devices, for example light-emitting diodes, is trap-mediated non-radiative losses. Defect passivation using organic molecules has been identified as an attractive approach to tackle this issue. However, implementation of this approach has been hindered by a lack of deep understanding of how the molecular structures influence the effectiveness of passivation. We show that the so far largely ignored hydrogen bonds play a critical role in affecting the passivation. By weakening the hydrogen bonding between the passivating functional moieties and the organic cation featuring in the perovskite, we significantly enhance the interaction with defect sites and minimize non-radiative recombination losses. Consequently, we achieve exceptionally high-performance near-infrared perovskite light-emitting diodes with a record external quantum efficiency of 21.6%. In addition, our passivated perovskite light-emitting diodes maintain a high external quantum efficiency of 20.1% and a wall-plug efficiency of 11.0% at a high current density of 200 mA cm−2, making them more attractive than the most efficient organic and quantum-dot light-emitting diodes at high excitations.
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The data that support the plots within this paper and other findings of this study are available from the corresponding authors upon reasonable request.
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Acknowledgements
We thank O. Inganäs, T.C. Sum, S.S. Lim, J. Zhang, W. Tress, W. Chen, Y. Puttisong, Y.T. Gong, C.Y. Kuang and C. Deibel for useful discussions. This work is supported by the ERC Starting Grant (717026), the National Basic Research Program of China (973 Program, grant number 2015CB932200), the National Natural Science Foundation of China (61704077, 51572016, 51721001, 61634001, 61725502, 91733302 and U1530401), the Joint Research Program between China and the European Union (2016YFE0112000), the Natural Science Foundation of Jiangsu Province (BK20171007), the National Key Research and Development Program of China (grant number 2016YFB0700700), the European Commission Marie Skłodowska-Curie Actions (691210), the Swiss National Science Foundation (CR23I2-162828), Nanyang Technological University start-up grant M4081924, and the Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linköping University (Faculty Grant SFO-Mat-LiU no. 2009-00971). The TEM measurements were performed at the Facility for Analysis, Characterization, Testing and Simulation (FACTS) in Nanyang Technological University, Singapore. A.P. and T.B. acknowledge financial support from the ERC Consolidator grant SOPHY (grant agreement number 771528). A.P. and A.J.B. acknowledge the project PERSEO-‘Perovskite-based solar cells: towards high efficiency and long-term stability’ (Bando PRIN 2015-Italian Ministry of University and Scientific Research (MIUR) Decreto Direttoriale 4 novembre 2015 n. 2488, project number 20155LECAJ) for funding. W.X. is a Wenner-Gren Postdoc Fellow; F.G. is a Wallenberg Academy Fellow.
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F.G. and W.X. conceived the idea and designed the experiments; W.X. performed the experiments and analysed the data under the supervision of F.G. and W.H.; Q.H. performed first-principles calculations on the molecular passivation under the supervision of L.-M.L.; Y.M., Z.C.Y., H.W., X.S. and Z.B.Y. contributed to device fabrication and measurements; Y.M. performed fluence-dependent PLQY and TCSPC measurements and analysed the data under the supervision of J.W. and W.H.; Y.M. and J.W. cross-checked the device performance at Nanjing Tech University; S.B. and Z.C.Y. synthesized and modified the ZnO nanocrystals and contributed to the device development; C.B. performed the TAS measurements and analysed the data; Z.H. performed the FTIR measurements and analysed the data; X.L. performed XPS tests and analysed the data; E.T. prepared the STEM specimen using FIB and performed the STEM imaging under the supervision of M.D.; T.B. and A.J.B. performed the transient absorption measurements and analysed the data under the supervision of A.P.; M.K. performed the ToF-SIMS measurements and analysed the data; J.-M.L., M.F., K.U. and W.Z. contributed to the data analysis; W.X. and F.G. wrote the manuscript; S.B., J.W. and A.P. provided revisions to the manuscript; F.G. supervised the project. All authors discussed the results and commented on the manuscript.
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F.G. and W.X. have filed a patent application related to this work (application no. SE1950272-3).
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Xu, W., Hu, Q., Bai, S. et al. Rational molecular passivation for high-performance perovskite light-emitting diodes. Nat. Photonics 13, 418–424 (2019). https://doi.org/10.1038/s41566-019-0390-x
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DOI: https://doi.org/10.1038/s41566-019-0390-x
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