Abstract
The fabrication of scalable all-perovskite tandem solar cells is considered an attractive route to commercialize perovskite photovoltaic modules1. However, the certified efficiency of 1-cm2-scale all-perovskite tandem solar cells lags behind their small-area (approximately 0.05-cm2) counterparts2,3. This performance deficit originates from inhomogeneity in wide-bandgap (WBG) perovskite solar cells (PSCs) at a large scale. The inhomogeneity is known to be introduced at the bottom interface and within the perovskite bulk itself4,5. Here we uncover another crucial source for the inhomogeneity—the top interface formed during the deposition of the electron transport layer (ETL; C60). Meanwhile, the poor ETL interface is also a notable limitation of device performance. We address this issue by introducing a mixture of 4-fluorophenethylamine (F-PEA) and 4-trifluoromethyl-phenylammonium (CF3-PA) to create a tailored 2D perovskite layer (TTDL), in which F-PEA forms a 2D perovskite at the surface, reducing contact losses and inhomogeneity, and CF3-PA enhances charge extraction and transport. As a result, we demonstrate a high open-circuit voltage (Voc) of 1.35 V and an efficiency of 20.5% in 1.77-eV WBG PSCs at a square-centimetre scale. By stacking with a narrow-bandgap (NBG) perovskite subcell, we report 1.05-cm2 all-perovskite tandem cells delivering 28.5% (certified 28.2%) efficiency, the highest reported so far. Our work showcases the importance of treating the top perovskite/ETL contact for upscaling PSCs.
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All data are available in the main text or the supplementary materials. Further data are available from the corresponding author on request.
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Acknowledgements
This work was financially supported by the National Key R&D Program of China (2022YFB4200304), National Natural Science Foundation of China (T2325016, U21A2076, 61974063, 62125402, 62321166653, 62305150, 52302327), Natural Science Foundation of Jiangsu Province (BE2022021, BE2022026, BK20202008, BK20190315, BK20232022), Fundamental Research Funds for the Central Universities (0213/14380206, 0205/14380252), Frontiers Science Center for Critical Earth Material Cycling Fund (DLTD2109) and the ‘GeoX’ Interdisciplinary Research Funds for the Frontiers Science Center for Critical Earth Material Cycling, Nanjing University and Program for Innovative Talents and Entrepreneur in Jiangsu. C.C. acknowledges the support of a Marshall Scholarship, Winton Scholarship and the Cambridge Trust. Y.H., a Japan Society for the Promotion of Science (JSPS) Overseas Research Fellow, acknowledges the financial support from the JSPS. M.I.S. is grateful to Canada Research Chairs Program (CRC-2019-00297) for operational support. We acknowledge the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (HYPERION, grant agreement no. 756962) and the Engineering and Physical Sciences Research Council (EPSRC) (grant agreement no. EP/V027131/1). S.D.S. acknowledges the Royal Society and Tata Group (grant no. UF150033). Grazing-incidence wide-angle X-ray scattering experiments were carried out at beamline 02U2, Shanghai Synchrotron Radiation Facility (SSRF). Calculations were performed in part at the High Performance Computing Center of Jilin University.
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H.T. conceived and directed the overall project. Y.W., R.L. and C.L. fabricated all the devices and conducted the characterization. A.D.B. and H.T.N. performed the photoluminescence and electroluminescence imaging characterization. H.S., X.Z., H.L., P.W., H.G., H.Z., X.L. and L.L. helped with the device fabrication and material characterization. W.S. and Y.N. performed the atomic force microscopy imaging characterization. C.C. performed the intensity-dependent quasi-Fermi level splitting measurements and pseudo-J–V analysis under the supervision of S.D.S. M.L. and C.X. performed the atomic Kelvin probe force microscopy imaging characterization. X.W., K.Z. and L.Z. performed the first-principles calculations. Y.W., X.W., Y.H., M.I.S., S.D.S., L.Z. and H.T. wrote the manuscript. All authors read and commented on the manuscript.
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H.T. is the founder, chief scientific officer and chairman of Renshine Solar Co. Ltd., a company that is commercializing perovskite photovoltaics. S.D.S. is a co-founder of Swift Solar. The other authors declare no competing interests.
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Wang, Y., Lin, R., Liu, C. et al. Homogenized contact in all-perovskite tandems using tailored 2D perovskite. Nature 635, 867–873 (2024). https://doi.org/10.1038/s41586-024-08158-6
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DOI: https://doi.org/10.1038/s41586-024-08158-6
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