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Nature Photonics (2026)
The popular and effective top-surface mixed-dimensional heterojunction in n–i–p perovskite photovoltaics is frequently ineffective in p–i–n architectures due to the intrinsic p-type character of most reported two-dimensional (2D) or low-dimensional perovskites. Here we deploy electronic engineering to realize the p– to n–type transition in 2D Ruddlesden–Popper perovskites through molecular dipole tuning and chemically designable n-type defects. Parahalogenated piperidine derivatives induce a favourable p– to n–type transition in 2D perovskites, thereby improving energy-level alignment at the perovskite–electron transport layer interface. This tailored band alignment effectively reduces interfacial energy barriers, suppresses non-radiative recombination losses for wide-bandgap perovskites and enhances stability. Notably, p–i–n wide-bandgap (~1.68 eV) perovskite solar cells with an n-type 2D capping layer exhibit more than 100 mV enhancement in open-circuit voltage, resulting in a certified power conversion efficiency of 33.64% when integrated with industrial 110-μm-thick Czochralski heterojunction silicon. Furthermore, such monolithic perovskite/silicon tandem cells retain 92% of their initial efficiency after 1,100 h of continuous operation under maximum-power-point tracking. Our chemical design of p– to n–type transition for 2D perovskite establishes a molecular-level strategy for optimizing interfacial energetics towards high-performance perovskite/silicon tandem photovoltaics.
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All data supporting the findings of this study are available in the main text or the Supplementary Information.
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We acknowledge BL02U2 beamline of the Shanghai Synchrotron Radiation Facility (SSRF) for assistance with GIWAXS measurements and the Instrumental Analysis Center of Shanghai Jiao Tong University and the School of Environmental Science and Engineering for assistance with characterizations. We thank H. Yang, T. Zhu and S. Hong from Shanghai Ideaoptics Co., Ltd. for kind assistance in PLQY measurements, and B. Zhu from the National Center of Inspection on Solar Photovoltaic Products Quality for helpful discussion of tandem-cell measurements.
This work was financially supported by the National Natural Science Foundation of China (NSFC) under grant nos. 22220102002 (Y.Z.), 52203334 (Y.M.), 22522903 (Y. Chen), 52403330 (Yao Wang) and 22409130 (B.L.); the Shanghai Science and Technology Innovation Action Plan under grant no. 24DZ3001203 (B.L.); the Shanghai Science and Technology Commission Program under grant no. 25DZ3001902 (Y.M.); and the Shanghai Jiao Tong University 2030 Initiative under grant no. WH510363004/003 (Y.M.).
These authors contributed equally: Jiahao Guo, Zeyu Zhang, Zhen Jia.
School of Environmental Science and Engineering, Frontiers Science Center for Transformative Molecules, State Key Laboratory of Green Papermaking and Resource Recycling, Shanghai Jiao Tong University, Shanghai, China
Jiahao Guo, Fang Liu, Menglei Feng, Wenji Zhan, Haifei Wang, Kanrui Jiang, Yuetian Chen, Yanfeng Miao & Yixin Zhao
Future Photovoltaic Research Center, Global Institute of Future Technology, Shanghai Jiao Tong University, Shanghai, China
Zeyu Zhang, Yao Wang, Bowei Li, Yanming Wang & Yixin Zhao
Chint New Energy Technology Co. Ltd., Haining, China
Zhen Jia & Zijia Li
School of Materials Science and Engineering, Jilin University, Changchun, China
Xiaoyu Wang
UM-SJTU Joint Institute, Shanghai Jiao Tong University, Shanghai, China
Yide Chang
Shanghai Non-carbon Energy Conversion and Utilization Institute, Shanghai, China
Yao Wang, Yuetian Chen, Yanfeng Miao, Bowei Li & Yixin Zhao
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Y.Z., Z.L., Yanming Wang and B.L. directed and supervised the project. Y.Z. conceptualized the research idea and designed the experimental framework. J.G., M.F., H.W. and Z.J. prepared and characterized the films and devices. F.L. contributed to synthesizing the X-PDI spacers and characterizing the perovskite films. B.L. characterized the PLQY. Z.Z., Y. Chang and Yanming Wang conducted DFT calculation. W.Z. conducted the EQEEL measurements. J.G. and K.J. contributed to the TEM measurements. J.G., B.L., Z.Z., X.W., Y. Chen, Yao Wang, Y.M. and Y.Z. drafted, revised and finalized the paper. All the authors revised the paper.
Correspondence to Bowei Li, Yanming Wang, Zijia Li or Yixin Zhao.
Y.Z., J.G., B.L., Yao Wang, Y.M. and Y. Chen are inventors on a patent application (CN202511692493.4) related to this work submitted by Shanghai Jiao Tong University. The other authors declare no competing interests.
Nature Photonics thanks the anonymous reviewers for their contribution to the peer review of this work.
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Supplementary Figs. 1–39, Tables 1–8 and References 1–17.
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Guo, J., Zhang, Z., Jia, Z. et al. Modulating p–n transition of two-dimensional perovskites for efficient and stable perovskite/Si tandem photovoltaics. Nat. Photon. (2026). https://doi.org/10.1038/s41566-026-01979-z
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DOI: https://doi.org/10.1038/s41566-026-01979-z
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