Abstract
Perovskite solar cells (PSCs) with an inverted structure (often referred to as the p–i–n architecture) are attractive for future commercialization owing to their easily scalable fabrication, reliable operation and compatibility with a wide range of perovskite-based tandem device architectures1,2. However, the power conversion efficiency (PCE) of p–i–n PSCs falls behind that of n–i–p (or normal) structure counterparts3,4,5,6. This large performance gap could undermine efforts to adopt p–i–n architectures, despite their other advantages. Given the remarkable advances in perovskite bulk materials optimization over the past decade, interface engineering has become the most important strategy to push PSC performance to its limit7,8. Here we report a reactive surface engineering approach based on a simple post-growth treatment of 3-(aminomethyl)pyridine (3-APy) on top of a perovskite thin film. First, the 3-APy molecule selectively reacts with surface formamidinium ions, reducing perovskite surface roughness and surface potential fluctuations associated with surface steps and terraces. Second, the reaction product on the perovskite surface decreases the formation energy of charged iodine vacancies, leading to effective n-type doping with a reduced work function in the surface region. With this reactive surface engineering, the resulting p–i–n PSCs obtained a PCE of over 25 per cent, along with retaining 87 per cent of the initial PCE after over 2,400 hours of 1-sun operation at about 55 degrees Celsius in air.
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The data that support the findings of this study are available from the corresponding authors on reasonable request.
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Acknowledgements
The work was partially supported by the US Department of Energy under contract number DE-AC36-08GO28308 with Alliance for Sustainable Energy, Limited Liability Company (LLC), the Manager and Operator of the National Renewable Energy Laboratory. We acknowledge the support on first-principle calculations, surface reaction analysis, synthesis of 3-APyI2 and optoelectronic characterizations (for example, transient reflection and time-resolved microwave conductivity), from the Center for Hybrid Organic–Inorganic Semiconductors for Energy (CHOISE), an Energy Frontier Research Center funded by the Office of Basic Energy Sciences, Office of Science within the US Department of Energy. A portion of the research was performed using computational resources sponsored by the Department of Energy’s Office of Energy Efficiency and Renewable Energy and located at the National Renewable Energy Laboratory. We acknowledge the support on 3-APy surface treatment and the corresponding device fabrication and characterizations from DE-FOA-0002064 and award number DE-EE0008790, and the support on the general device and thin-film perovskite fabrication and characterizations from the Advanced Perovskite Cells and Modules programme of the National Center for Photovoltaics, funded by the US Department of Energy, Office of Energy Efficiency and Renewable Energy, Solar Energy Technologies Office. This work was also supported in part by the California Energy Commission EPIC programme, EPC-19-004. We acknowledge the use of facilities and instrumentation at the UC Irvine Materials Research Institute (IMRI), which is supported in part by the National Science Foundation through the UC Irvine Materials Research Science and Engineering Center (DMR-2011967). XPS and UPS were performed in part using instrumentation funded in part by the National Science Foundation Major Research Instrumentation Program under grant number CHE-1338173. We thank I. Tran for assistance with collecting the XPS and UPS data; and S. M. Rowland and L. M. Laurens for conducting the mass spectrometry measurements and structure assignments at the NREL Bioenergy Science Technologies directorate. The views expressed in the article do not necessarily represent the views of the DOE or the US Government.
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Q.J., J.T. and K.Z. conceived the idea. K.Z. supervised the projects and process. Q.J. fabricated perovskite films and devices and conducted X-ray diffraction, scanning electron microscopy, and ultraviolet–visible and stability measurements. J.T. was involved in material and device design and analysis. Y.X. carried out the DFT calculation, with help from X.W., under the supervision of Y.Y. R.A.K. and B.W.L. were involved in surface reaction study and relevant analysis. S.P.D. performed XPS and UPS measurements and analysis under the guidance of D.P.F. C.X. performed AFM and KPFM characterizations and analysis. R.A.S. conducted the transient reflection measurement and analysis under the guidance of M.C.B. D.K. performed the photoluminescence characterization and analysis. M.P.H. prepared the 3-APy halide salts. R.T. helped to work on device stability test under the supervision of J.J.B. B.W.L. conducted the time-resolved microwave conductivity measurement and analysis. Q.J. and K.Z. wrote the first draft of the manuscript. All authors discussed the results and contributed to the revisions of the manuscript.
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Jiang, Q., Tong, J., Xian, Y. et al. Surface reaction for efficient and stable inverted perovskite solar cells. Nature 611, 278–283 (2022). https://doi.org/10.1038/s41586-022-05268-x
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DOI: https://doi.org/10.1038/s41586-022-05268-x
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