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Nature Materials volume 24, pages 1626–1634 (2025)
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The cathode interfacial layer (CIL) critically influences electron extraction and charge recombination, thereby playing a pivotal role in organic solar cells (OSCs). However, most state-of-the-art CILs are constrained by limited conductivity, high recombination and poor morphology, which collectively hinder device efficiency and stability. Here we report an inorganic–organic hybrid CIL (AZnO-F3N), developed by a dual-component synergy strategy, which integrates organic material PNDIT-F3N with two-dimensional amorphous zinc oxide. This design leverages the synergistic interactions between two-dimensional amorphous zinc oxide and PNDIT-F3N, resulting in reduced interfacial defect, enhanced conductivity and improved film uniformity. OSCs incorporating the AZnO-F3N CIL exhibit more efficient charge extraction and transport, along with reduced recombination. Consequently, a D18:L8-BO-based binary OSC achieves an efficiency of 20.6%. The introduction of BTP-eC9 as the third component further elevates the efficiency to 21.0% (certified as 20.8%). Moreover, the CIL demonstrates versatility across various active layers, thick-film configuration and flexible devices, underscoring its great potential to advance OSC technology.
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Source data are provided with this paper. The remaining data are available from the corresponding authors upon reasonable request.
The codes used to analyse the data in this study are available from the corresponding authors upon reasonable request.
Cheng, P., Li, G., Zhan, X. & Yang, Y. Next-generation organic photovoltaics based on non-fullerene acceptors. Nat. Photon. 12, 131–142 (2018).
Liu, Y. et al. Recent progress in organic solar cells (part I material science). Sci. China Chem. 65, 224–268 (2022).
Article CAS Google Scholar
Hou, J., Inganäs, O., Friend, R. H. & Gao, F. Organic solar cells based on non-fullerene acceptors. Nat. Mater. 17, 119–128 (2018).
Article CAS PubMed Google Scholar
Guan, S. et al. Self-assembled interlayer enables high-performance organic photovoltaics with power conversion efficiency exceeding 20%. Adv. Mater. 36, 2400342 (2024).
Article CAS Google Scholar
Jiang, Y. et al. Non-fullerene acceptor with asymmetric structure and phenyl-substituted alkyl side chain for 20.2% efficiency organic solar cells. Nat. Energy 9, 975–986 (2024).
Article CAS Google Scholar
Li, C. et al. Highly efficient organic solar cells enabled by suppressing triplet exciton formation and non-radiative recombination. Nat. Commun. 15, 8872 (2024).
Article CAS PubMed PubMed Central Google Scholar
He, R. et al. Improving interface quality for 1-cm2 all-perovskite tandem solar cells. Nature 618, 80–86 (2023).
Article CAS PubMed Google Scholar
Li, Y. et al. Flexible silicon solar cells with high power-to-weight ratios. Nature 626, 105–110 (2024).
Article CAS PubMed Google Scholar
Benduhn, J. et al. Intrinsic non-radiative voltage losses in fullerene-based organic solar cells. Nat. Energy 2, 17053 (2017).
Article CAS Google Scholar
Green, M. A. Solar cell fill factors: general graph and empirical expressions. Solid-State Electron. 24, 788–789 (1981).
Article CAS Google Scholar
Jiang, K. et al. Suppressed recombination loss in organic photovoltaics adopting a planar–mixed heterojunction architecture. Nat. Energy 7, 1076–1086 (2022).
Article Google Scholar
Zhang, X. et al. High fill factor organic solar cells with increased dielectric constant and molecular packing density. Joule 6, 444–457 (2022).
Article CAS Google Scholar
Zhu, L. et al. Single-junction organic solar cells with over 19% efficiency enabled by a refined double-fibril network morphology. Nat. Mater. 21, 656–663 (2022).
Article CAS PubMed Google Scholar
Zeng, R. et al. All-polymer organic solar cells with nano-to-micron hierarchical morphology and large light receiving angle. Nat. Commun. 14, 4148 (2023).
Article CAS PubMed PubMed Central Google Scholar
Li, C. et al. Non-fullerene acceptors with branched side chains and improved molecular packing to exceed 18% efficiency in organic solar cells. Nat. Energy 6, 605–613 (2021).
Article CAS Google Scholar
Yuan, J. et al. Single-junction organic solar cell with over 15% efficiency using fused-ring acceptor with electron-deficient core. Joule 3, 1140–1151 (2019).
Article CAS Google Scholar
Bai, Q. et al. Recent progress in low-cost noncovalently fused-ring electron acceptors for organic solar cells. Aggregate 3, e281 (2022).
Article CAS Google Scholar
Tada, A., Geng, Y., Wei, Q., Hashimoto, K. & Tajima, K. Tailoring organic heterojunction interfaces in bilayer polymer photovoltaic devices. Nat. Mater. 10, 450–455 (2011).
Article CAS PubMed Google Scholar
Li, C. et al. Achieving record-efficiency organic solar cells upon tuning the conformation of solid additives. J. Am. Chem. Soc. 144, 14731–14739 (2022).
Article CAS PubMed PubMed Central Google Scholar
Song, C. K. et al. ‘Supersaturated’ self-assembled charge-selective interfacial layers for organic solar cells. J. Am. Chem. Soc. 136, 17762–17773 (2014).
Article CAS PubMed Google Scholar
Wu, Z. et al. n-Type water/alcohol-soluble naphthalene diimide-based conjugated polymers for high-performance polymer solar cells. J. Am. Chem. Soc. 138, 2004–2013 (2016).
Article CAS PubMed Google Scholar
Qin, F. et al. Robust metal ion-chelated polymer interfacial layer for ultraflexible non-fullerene organic solar cells. Nat. Commun. 11, 4508 (2020).
Article CAS PubMed PubMed Central Google Scholar
Ouyang, X., Peng, R., Ai, L., Zhang, X. & Ge, Z. Efficient polymer solar cells employing a non-conjugated small-molecule electrolyte. Nat. Photon. 9, 520–524 (2015).
Article CAS Google Scholar
Yao, J. et al. Cathode engineering with perylene-diimide interlayer enabling over 17% efficiency single-junction organic solar cells. Nat. Commun. 11, 2726 (2020).
Article CAS PubMed PubMed Central Google Scholar
Yu, Z. et al. Hot-substrate deposition of hole- and electron-transport layers for enhanced performance in perovskite solar cells. Adv. Energy Mater. 8, 1701659 (2018).
Article Google Scholar
Zhang, G. et al. NiOx nanoparticles hole-transporting layer regulated by ionic radius-controlled doping and reductive agent for organic solar cells with efficiency of 19.18%. Adv. Mater. 36, 2310630 (2024).
Article CAS Google Scholar
Leijtens, T., Lim, J., Teuscher, J., Park, T. & Snaith, H. J. Charge density dependent mobility of organic hole-transporters and mesoporous TiO2 determined by transient mobility spectroscopy: implications to dye-sensitized and organic solar cells. Adv. Mater. 25, 3227–3233 (2013).
Article CAS PubMed Google Scholar
He, Z. et al. Enhanced power-conversion efficiency in polymer solar cells using an inverted device structure. Nat. Photon. 6, 591–595 (2012).
Article Google Scholar
Zhao, C. et al. An organic–inorganic hybrid electrolyte as a cathode interlayer for efficient organic solar cells. Angew. Chem. Int. Ed. 60, 8526–8531 (2021).
Article CAS Google Scholar
Zhang, Y. et al. Organic–inorganic hybrid cathode interlayer materials for efficient organic solar cells. Sustain. Energy Fuels 6, 4115–4129 (2022).
Article CAS Google Scholar
Li, S. et al. Achieving over 18% efficiency organic solar cell enabled by a ZnO-based hybrid electron transport layer with an operational lifetime up to 5 years. Angew. Chem. Int. Ed. 61, e202207397 (2022).
Article CAS Google Scholar
Baek, S.-W. et al. Enhancing the internal quantum efficiency and stability of organic solar cells via metallic nanofunnels. Adv. Energy Mater. 5, 1501393 (2015).
Article Google Scholar
Jiang, Q. et al. Surface passivation of perovskite film for efficient solar cells. Nat. Photon. 13, 460–466 (2019).
Article CAS Google Scholar
Chen, Z. et al. Simplified fabrication of high-performance organic solar cells through the design of self-assembling hole-transport molecules. Joule 8, 1723–1734 (2024).
Article CAS Google Scholar
Xin, Y. et al. Multiarmed aromatic ammonium salts boost the efficiency and stability of inverted organic solar cells. J. Am. Chem. Soc. 146, 3363–3372 (2024).
Article CAS PubMed Google Scholar
Fiori, G. et al. Electronics based on two-dimensional materials. Nat. Nanotechnol. 9, 768–779 (2014).
Article CAS PubMed Google Scholar
Wen, X. et al. Tetrahydroxy-perylene bisimide embedded in a zinc oxide thin film as an electron-transporting layer for high-performance non-fullerene organic solar cells. Angew. Chem. Int. Ed. 58, 13051–13055 (2019).
Article CAS Google Scholar
Sun, Y., Seo, J. H., Takacs, C. J., Seifter, J. & Heeger, A. J. Inverted polymer solar cells integrated with a low-temperature-annealed sol-gel-derived ZnO film as an electron transport layer. Adv. Mater. 23, 1679–1683 (2011).
Article CAS PubMed Google Scholar
Li, Y. et al. An n-n heterojunction configuration for efficient electron transport in organic photovoltaic devices. Adv. Funct. Mater. 33, 2209728 (2023).
Article CAS Google Scholar
Xia, Y. et al. Molecular doping inhibits charge trapping in low-temperature-processed ZnO toward flexible organic solar cells. ACS Appl. Mater. Interfaces 13, 14423–14432 (2021).
Article CAS PubMed Google Scholar
Chen, S. et al. Inverted polymer solar cells with reduced interface recombination. Adv. Energy Mater. 2, 1333–1337 (2012).
Article CAS Google Scholar
Latham, K. G., Simone, M. I., Dose, W. M., Allen, J. A. & Donne, S. W. Synchrotron based NEXAFS study on nitrogen doped hydrothermal carbon: insights into surface functionalities and formation mechanisms. Carbon 114, 566–578 (2017).
Article CAS Google Scholar
Zubavichus, Y., Shaporenko, A., Korolkov, V., Grunze, M. & Zharnikov, M. X-ray absorption spectroscopy of the nucleotide bases at the carbon, nitrogen, and oxygen K-edges. J. Phys. Chem. B 112, 13711–13716 (2008).
Article CAS PubMed Google Scholar
Mendoza-Sánchez, B. & Gogotsi, Y. Synthesis of two-dimensional materials for capacitive energy storage. Adv. Mater. 28, 6104–6135 (2016).
Article PubMed Google Scholar
Daboczi, M. et al. Origin of open-circuit voltage losses in perovskite solar cells investigated by surface photovoltage measurement. ACS Appl. Mater. Interfaces 11, 46808–46817 (2019).
Article CAS PubMed Google Scholar
Meng, H. et al. Inhibition of halide oxidation and deprotonation of organic cations with dimethylammonium formate for air-processed p–i–n perovskite solar cells. Nat. Energy 9, 536–547 (2024).
Article CAS Google Scholar
Tang, R. et al. Hydrothermal deposition of antimony selenosulfide thin films enables solar cells with 10% efficiency. Nat. Energy 5, 587–595 (2020).
Article CAS Google Scholar
Shockley, W. & Queisser, H. J. Detailed balance limit of efficiency of p-n junction solar cells. J. Appl. Phys. 32, 510–519 (1961).
Article CAS Google Scholar
Schön, J. H., Kloc, C., Siegrist, T., Laquindanum, J. & Katz, H. E. Charge transport in anthradithiophene single crystals. Org. Electron. 2, 165–169 (2001).
Article Google Scholar
Abdi-Jalebi, M. et al. Charge extraction via graded doping of hole transport layers gives highly luminescent and stable metal halide perovskite devices. Sci. Adv. 5, eaav2012 (2019).
Article CAS PubMed PubMed Central Google Scholar
Wang, F. et al. Monolithically-grained perovskite solar cell with Mortise-Tenon structure for charge extraction balance. Nat. Commun. 14, 3216 (2023).
Article CAS PubMed PubMed Central Google Scholar
Wang, R. et al. Charge separation from an intra-moiety intermediate state in the high-performance PM6:Y6 organic photovoltaic blend. J. Am. Chem. Soc. 142, 12751–12759 (2020).
Article CAS PubMed Google Scholar
Marcus, R. A. Chemical and electrochemical electron-transfer theory. Annu. Rev. Phys. Chem. 15, 155–196 (1964).
Article CAS Google Scholar
Zhao, H., Chen, X., Wang, G., Qiu, Y. & Guo, L. Two-dimensional amorphous nanomaterials: synthesis and applications. 2D Mater. 6, 032002 (2019).
Article CAS Google Scholar
Li, F. et al. Dual-phase super-strong and elastic ceramic. ACS Nano 13, 4191–4198 (2019).
Article CAS PubMed Google Scholar
Nai, J., Tian, Y., Guan, X. & Guo, L. Pearson’s principle inspired generalized strategy for the fabrication of metal hydroxide and oxide nanocages. J. Am. Chem. Soc. 135, 16082–16091 (2013).
Article CAS PubMed Google Scholar
Xiong, H. et al. General room-temperature Suzuki–Miyaura polymerization for organic electronics. Nat. Mater. 23, 695–702 (2024).
Article CAS PubMed Google Scholar
Song, J. et al. Solid additive engineering enables high-efficiency and eco-friendly all-polymer solar cells. Matter 5, 4047–4059 (2022).
Article CAS Google Scholar
Song, J. et al. High-efficiency organic solar cells with low voltage loss induced by solvent additive strategy. Matter 4, 2542–2552 (2021).
Article CAS Google Scholar
Gu, X. et al. High-efficiency and low-energy-loss organic solar cells enabled by tuning conformations of dimeric electron acceptors. CCS Chem. 5, 2576–2588 (2023).
Article CAS Google Scholar
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We acknowledge financial support from the National Natural Science Foundation of China (52450063, 52473200, 52120105006 and 51532001), the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB0520103), National Key R&D Program of China (no. 2024YFB3614300), the International Partnership Program of the Chinese Academy of Sciences (124GJHZ2023079MI), the Fundamental Research Funds for the Central Universities and the University of Chinese Academy of Sciences. A portion of this work is based on the data obtained at BSRF-1W1A. We gratefully acknowledge the cooperation of the beamline scientists at BSRF-1W1A beamline and also thank BL10B in NSRL for characterizations by synchrotron radiation.
These authors contributed equally: Congqi Li, Yunhao Cai, Pengfei Hu.
College of Materials Science and Opto-Electronic Technology Center of Materials Science and Optoelectronics Engineering CAS Center for Excellence in Topological Quantum Computation CAS Key Laboratory of Vacuum Physics, University of Chinese Academy of Sciences, Beijing, China
Congqi Li, Yunhao Cai, Meng Zhang, Jikai Lv, Meng Zhang, Qijie Lin, Jiarui Wang, Xin Zhang, Xiaoyi Li & Hui Huang
School of Chemistry, Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology, Beijing Advanced Innovation Center for Biomedical Engineering, Beihang University, Beijing, China
Pengfei Hu, Tao Liu & Lin Guo
Research Institute of Aero-Engine, Beihang University, Beijing, China
Pengfei Hu
School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Key Laboratory of Electrical Insulation and Thermal Aging, Shanghai Jiao Tong University, Shanghai, China
Lei Zhu, Rui Zeng, Fei Han, Ming Zhang & Feng Liu
Beijing National Laboratory for Molecular Sciences, Huairou Research Center, Institute of Chemistry, Chinese Academy of Sciences, Beijing, China
Yuanxin Ma & Zihao Xu
School of Materials Science & Engineering, Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Key Laboratory of Organic Integrated Circuits, Ministry of Education, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin University, Tianjin, China
Dexia Han & Long Ye
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Center of Smart Materials and Devices School of Chemistry, Chemical Engineering and Life Science, Wuhan University of Technology, Wuhan, China
Jingwen Xu & Jianlong Xia
Center for Advanced Low-Dimension Materials State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and Engineering, Donghua University, Shanghai, China
Na Yu & Zheng Tang
School of Physics, State Key Laboratory of Crystal Materials, Shandong University, Jinan, China
Jiawei Qiao & Xiaotao Hao
School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, China
Qian Peng
School of Chemical Engineering and Technology, State Key Laboratory of Chemical Engineering and Low-Carbon Technology, Tianjin University, Tianjin, China
Hui Huang
The International Joint Institute of Tianjin University, Fuzhou, China
Hui Huang
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H.H. and Y.C. developed the concept and conceived the idea. Y.C., L.G. and H.H. supervised and directed this project. C.L. fabricated and characterized the devices and carried out detailed characterizations. P.H., T.L. and Meng Zhang (https://orcid.org/0009-0004-9866-3749) synthesized the 2D A-ZnO. Z.X., Y.M., J. Xu and J. Xia provided the transient absorption spectra results and corresponding analysis. L.Z., R.Z., Ming Zhang, F.H. and F.L. provided the morphology measurement and corresponding analysis. Meng Zhang (https://orcid.org/0009-0000-4058-8927) and X.L. conducted the first-principles calculation and related analysis. J.L. and Q.P. provided the energy-level-related calculation and corresponding analysis. D.H. and L.Y. fabricated the IS-OSCs devices and provided the related data. Q.L. and J.W. carried out the TPV, TPC and Mott–Schottky-related characterization and analysed the data. N.Y. and Z.T. provided the energy loss results. J.Q. and X.H. provided the fluorescence lifetime imaging microscopy and time-resolved photoluminescence results. C.L., Y.C., P.H., F.L., L.G. and H.H. organized the paper. All authors discussed the results and commented on the paper.
Correspondence to Yunhao Cai, Lin Guo or Hui Huang.
The authors declare no competing interests.
Nature Materials thanks the anonymous reviewers for their contribution to the peer review of this work.
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Supplementary Figs. 1–48, Tables 1–14, Notes 1–9 and Methods.
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Li, C., Cai, Y., Hu, P. et al. Organic solar cells with 21% efficiency enabled by a hybrid interfacial layer with dual-component synergy. Nat. Mater. 24, 1626–1634 (2025). https://doi.org/10.1038/s41563-025-02305-8
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