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Organic solar cells with 20.82% efficiency and high tolerance of active layer thickness through crystallization sequence manipulation

Nature Materials volume 24, pages 444–453 (2025)Cite this article

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Abstract

Printing of large-area solar panels necessitates advanced organic solar cells with thick active layers. However, increasing the active layer thickness typically leads to a marked drop in the power conversion efficiency. Here we developed an organic semiconductor regulator, called AT-β2O, to tune the crystallization sequence of the components in active layers. When adding AT-β2O in the donor (D18-Cl) and acceptor (N3) blend, N3 crystallizes behind D18-Cl, and this phenomenon is different from the co-crystallization observed in binary D18-Cl:N3 blends. This manipulation of crystallization dynamics is favourable to form bulk-heterojunction-gradient vertical phase separation in the active layer accompanied by the high crystallinity of the acceptor and balanced charge carrier mobilities in thick films. The resultant single-junction organic solar cells exhibited a certified power conversion efficiency of over 20%, as well as demonstrated exceptional adaptability across the active layer thicknesses (100–400 nm) and remarkable universality. Such breakthroughs enable large-area modules with a certified power conversion efficiency of 18.04%.

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Fig. 1: Molecular structures and single-crystal structures acquired through X-ray crystallographic analysis.
Fig. 2: Crystallinity and deposit dynamics characterization.
Fig. 3: Film-depth-dependent phase separation.
Fig. 4: Film crystallization dynamics characterization.
Fig. 5: Photovoltaic performance of the devices.
Fig. 6: Large-area OSC modules and device stability.

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Data availability

The experimental data that support the findings of this paper are available within the Article and its Supplementary Information. The other findings of this study are available from the corresponding author upon reasonable request. Source data are provided with this paper.

Code availability

The codes used to analyse the data in this study are available from the corresponding author upon reasonable request.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (grant nos 52325307, 52273188, 22309129 and 22075194), Department of Science and Technology of Jiangsu Province (grant no. BE2022023), the National Postdoctoral Program for Innovative Talents (grant no. BX20220221), the China Postdoctoral Science Foundation (grant no. 2023M732530), Sichuan Science and Technology Program (grant no. 2023NSFSC0990), the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD), Collaborative Innovation Center of Suzhou Nano Science and Technology and the Key Laboratory of Polymeric Materials Design and Synthesis for Biomedical Function, Soochow University. R.Z. thanks C. Zhu for the GIWAXS measurement at beamline 7.3.3 at the Advanced Light Source, Lawrence Berkeley National Laboratory, supported by the Director, Office of Science, Office of Basic Energy Sciences, US Department of Energy, under contract no. DE-AC02-05CH11231. We thank Y. Chen (Beijing Synchrotron Radiation Facility) and L. Wang (Beijing Zhongke Wanyuan Technology) for the in situ GIWAXS experiments. We also acknowledge support from the Suzhou Sunflex New Energy Company and State Key Lab of Luminescent Materials and Devices, South China University of Technology.

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Authors and Affiliations

  1. Laboratory of Advanced Optoelectronic Materials, Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, China

    Haiyang Chen, Yuting Huang, Hongyu Mou, Junyuan Ding, Weijie Chen, Juan Zhu, Qinrong Cheng, Hao Gu, Xiaoxiao Wu, Tianjiao Zhang, Yingyi Wang, Yaowen Li & Yongfang Li

  2. Department of Physics, Chemistry and Biology (IFM), Linköping University, Linköping, Sweden

    Rui Zhang & Feng Gao

  3. Institute of Polymer Optoelectronic Materials and Devices State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou, China

    Jiadong Zhou & Zengqi Xie

  4. Department of Chemistry, Zhejiang University, Hangzhou, China

    Zukun Wang & Haiming Zhu

  5. College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu, China

    Hongxiang Li

  6. Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou, China

    Yaowen Li & Yongfang Li

  7. State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials, Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, China

    Yaowen Li

  8. Beijing National Laboratory for Molecular Sciences; CAS Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing, China

    Yongfang Li

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Contributions

Yaowen Li conceived and supervised the project. H.C. developed the new material AT-β2O. H.C., Y.H., H.M. and H.G. fabricated the devices. J. Zhou and Z.X. grew the single crystal and analysed the single-crystal structure of AT-β2O. H.C., Y.H., J.D., Q.C., J. Zhu, X.W., T.Z., H.L. and Y.W. participated in the characterizations of materials and devices. Z.W. and H.Z. conducted the pump-fluence-dependent TA spectroscopy measurements. H.C., R.Z., W.C, F.G., Yaowen Li and Yongfang Li contributed to the result analysis. H.C. and Yaowen Li wrote the manuscript. Yaowen Li and Yongfang Li revised the project. All authors discussed the results and commented on the final manuscript.

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Correspondence to Yaowen Li.

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Chen, H., Huang, Y., Zhang, R. et al. Organic solar cells with 20.82% efficiency and high tolerance of active layer thickness through crystallization sequence manipulation. Nat. Mater. 24, 444–453 (2025). https://doi.org/10.1038/s41563-024-02062-0

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