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Nature Materials (2025)
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Achieving a well-controlled electron-selective layer is critical for the device scalability and performance of perovskite solar cells. While phenyl-C61-butyric acid methyl ester (PCBM) is a promising electron-selective material in inverted perovskite solar cells, its dimerization under environmental stress accelerates the material degradation and complicates producing high-quality PCBM layers, thereby compromising device long-term operational stability and scale-up fabrication. Here we investigated the PCBM molecular stacking on perovskite surfaces, finding that the variability in perovskite surface termination leads to orientation and distribution heterogeneity of the PCBM layer, resulting in undesirable dimerization. To address this, we developed a molecular dopant for suppressing PCBM dimer formation, achieving a certified efficiency of 26.4% in laboratory-scale devices and 25.3% in 1 cm2 devices. Furthermore, these devices maintained 93% of their initial power conversion efficiency after 1,500 h of ageing at 85 °C following the ISOS L-2I protocol.
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The data that support the findings of this study are available from the corresponding authors upon request.
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This research was financially supported by the CAS Project for Young Scientists in Basic Research (grant number YSBR-102), the National Key R&D programme of China (grant number 2021YFB3800102) and the National Natural Science Foundation of China (grant numbers 52302324, 52272252, U22A20142 and 62204108). J.Y. acknowledges the support from the Director’s Fund of Hefei Institutes of Physical Science (grants numbers YZJJ-GGZX-2022-01 and YZJJ202304-CX). N.-G.P. acknowledges financial support through grants from the National Research Foundation of Korea, which is funded by the Korean Ministry of Science and ICT under contract NRF-2021R1A3B1076723 (Research Leader Program). J.L. acknowledges the support from the National Natural Science Foundation of China (grant number 22303053). We thank the XPS group and scanning electron microscopy group of the Instruments Center for Physical Science, University of Science and Technology of China for its vigorous support on the work in this article. X.L., J.L. and Y.Z. thank the Center for Computational Science and Engineering at Southern University of Science and Technology and Hoffmann Institute of Advanced Materials at Shenzhen Polytechnic University for providing the computing resources.
These authors contributed equally: Zheng Liang, Huifen Xu, Zhenda Huang, Xia Lei, Jiajiu Ye.
Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei, People’s Republic of China
Zheng Liang, Huifen Xu, Zhenda Huang, Jiajiu Ye, Boyuan Liu, Shirui Weng, Yuli Tao, Hui Zhang, Feng Chen, Liangbao Yang & Xu Pan
University of Science and Technology of China, Hefei, People’s Republic of China
Zheng Liang, Huifen Xu, Zhenda Huang, Boyuan Liu, Wenjing Chen, Xue Wang, Yuli Tao, Hui Zhang, Wanting Liu, Hongmin Zhou, Shangfeng Yang & Zhengguo Xiao
School of Chemical Engineering and Center for Antibonding Regulated Crystals, Sungkyunkwan University, Suwon, Republic of Korea
Zheng Liang, Yalan Zhang, Sang-Uk Lee & Nam-Gyu Park
SKKU Institute of Energy Science and Technology, Sungkyunkwan University, Suwon, Republic of Korea
Zheng Liang, Yalan Zhang, Sang-Uk Lee & Nam-Gyu Park
Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, People’s Republic of China
Xia Lei, Peide Zhu, Yaru Li, Jie Zeng, Jiufeng Dong & Baomin Xu
Hoffman Institute of Advanced Materials, Shenzhen Polytechnic University, Shenzhen, People’s Republic of China
Xia Lei & Jingbai Li
IMD3-Photovoltaics, Forschungszentrum Jülich, Jülich, Germany
Jiajiu Ye & Thomas Kirchartz
Sustainable Energy and Environment Thrust, Function Hub, The Hong Kong University of Science and Technology (Guangzhou), Guangzhou, People’s Republic of China
Yong Zhang
School of Renewable Energy, Hohai University, Changzhou, People’s Republic of China
Yunxiao Liao & Yong Ding
Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore, Singapore
Xiangbin Cai
i-Lab, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou, People’s Republic of China
Hongzhen Lin
Aerospace Information Research Institute, Chinese Academy of Sciences, Beijing, People’s Republic of China
Guoning Xu
ChangZhou S.C Exact Equipment Co., Changzhou, People’s Republic of China
Jiang Sheng
Faculty of Engineering and CENIDE, University of Duisburg-Essen, Duisburg, Germany
Thomas Kirchartz
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Z.L., J.Y. and X.P. conceived the main idea of this work; J.Y., X.P. and N.-G.P. oversaw the administration of this project; J.L., Z.L. and Y.Z. conceptualized and analysed the theoretical study; Z.L., H.X., Z.H. and B.L. fabricated devices and performed photovoltaic measurements; X.L. performed the MD simulations and DFT calculations under the supervision of J.L; Z.L. contributed to or assisted with subsequent experimental characterizations and data analysis. P.Z., Y. Li, J.Z. and J.D. synthesized the perovskite materials and performed the electrical characterizations under supervision of Y.Z. and B.X; W.C. performed optoelectronic characterization under supervision of Z.X; X.W. contributed to the methodology design under supervision of S.Y; Y.L. completed the preparation and testing of large area PSMs under supervision of Y.D. and J.S; S.W. contributed to the ARPR analysis under supervision of L.Y; Y.T. and H.Z. synthesized the additive chemicals under supervision of J.Y. and X.P; X.C. and H.Zh. performed electron microscope analysis; W.L. and Y.Zh. performed the XPS and UPS analysis; S.-U.L. and contributed to the analysis and discussion of activation energy and band alignment. H.L. performed the SFG analysis; T.K. contributed to the discussion of the mechanism; G.X., J.L., Y.Z., J.Y., B.X., X.P. and N.-G.P. secured the funding for this project; Z.L., H.X. and J.Y. wrote the original draft J.L., Y.Z., S.Y., B.X., Z.X., T.K., Y.Y., X.P. and N.-G.P. revised the paper; all authors discussed the results and commented on the paper.
Correspondence to Jiajiu Ye, Yong Zhang, Jingbai Li, Xu Pan or Nam-Gyu Park.
The authors declare no competing interests.
Nature Materials thanks Xiong Li, Yixin Zhao and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
PL spectra of a, the bare perovskite (PVSK) and separately coated with FIBA (PVSK/FIBA) and b, perovskite films with bare PCBM (Ref) and FIBA-treated PCBM (FIBA).
FIBA concentration varied from 5 wt% to 25 wt%.
Energetic level (Ea’) relative to perovskite VBM, as extracted from C-ω-T measurements.
Statistical data of detailed photovoltaic parameters, including a, VOC, b, JSC, c, FF and d, PCE of a series devices treated with various FIBA concentrations. Extended Data Fig. 4 presents a box plot showing the mean, the median (as a central line), the 25th to 75th percentile range as the box, and whiskers extending to 1.5 times the interquartile range.
a, EQE results of the reference and FIBA devices. b, Plot of the first-order derivative of EQE measurements, indicating the bandgap of the perovskite materials.
Optical microscopy images of the a, reference and b, FIBA devices at the metal electrodes region after stability testing under ISOS D-2I. The scale bars represent 100 μm.
Optical microscopy images of the a, reference and b, FIBA devices at the metal electrodes region after stability testing under ISOS L-3. The scale bars represent 50 μm.
Supplementary Figs. 1–55, Tables 1–7, Notes 1–5 and references.
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Liang, Z., Xu, H., Huang, Z. et al. Suppression of PCBM dimer formation in inverted perovskite solar cells. Nat. Mater. (2025). https://doi.org/10.1038/s41563-025-02368-7
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