Manipulating Hierarchical Aggregation Structure <italic style="font-style: italic">via</italic> Film-forming Kinetics Enables Organic Photovoltaics over 20% Efficiency

Qin-Sheng Li; Hou-Dong Mao; Lin Wen; Li-Fu Zhang; Zhao Qin; Jia-You Zhang; Dou Luo; Li-Cheng Tan; Yi-Wang Chen

doi:10.1007/s10118-026-3702-x

Your Location：

Home >

Browse articles >

Manipulating Hierarchical Aggregation Structure via Film-forming Kinetics Enables Organic Photovoltaics over 20% Efficiency

RESEARCH ARTICLE | Updated：2026-07-02

- Manipulating Hierarchical Aggregation Structure via Film-forming Kinetics Enables Organic Photovoltaics over 20% Efficiency
- Manipulating Hierarchical Aggregation Structure via Film-forming Kinetics Enables Organic Photovoltaics over 20% Efficiency
- Chinese Journal of Polymer Science 2026年44卷页码：1-9
- Affiliations：
  
  a.College of Chemistry and Chemical Engineering/Film Energy Chemistry for Jiangxi Provincial Key Laboratory (FEC)/Institute of Polymers and Energy Chemistry (IPEC), Nanchang University, Nanchang 330031, China
  b.Zhuhai College of Science and Technology, Zhuhai 519040, China
  c.Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of the Ministry of Education, Jiangxi Normal University, Nanchang 330022, China
- Author bio：
  
  tanlicheng@ncu.edu.cn
- Funds：
  
  Y. C. thanks the National Natural Science Foundation of China (No. 52333006) for their support. L. Z. would like to thank the National Natural Science Foundation of China (No. 52303232) and Jiangxi Provincial Natural Science Foundation (Nos. 20242BAB20184 and 2025BAC240409). L. T. thanks the National Natural Science Foundation of China for their support (No. 52373186). D. L. thanks the National Natural Science Foundation of China (No. 22509176) for their support.;The authors declare no interest conflict.Electronic supplementary information (ESI) is available free of charge in the online version of this article at http://doi.org/10.1007/s10118-026-3702-x.The data that support the findings of this study are available from the corresponding author upon reasonable request.
- DOI：10.1007/s10118-026-3702-x
  中图分类号：
- 收稿：2026-02-08，
  
  录用：2026-04-04，
  
  网络首发：2026-07-02，
  
  纸质出版：2026-06
- Accepted：
Scan QR Code
Li, Q. S.; Mao, H. D.; Wen, L.; Zhang, L. F.; Qin, Z.; Zhang, J. Y.; Luo, D.; Tan, L. C.; Chen, Y. W. Manipulating hierarchical aggregation structure via film-forming kinetics enables organic photovoltaics over 20% efficiency. Chinese J. Polym. Sci. https://doi.org/10.1007/s10118-026-3702-x

Qin-Sheng Li, Hou-Dong Mao, Lin Wen, et al. Manipulating Hierarchical Aggregation Structure via Film-forming Kinetics Enables Organic Photovoltaics over 20% Efficiency[J/OL]. Chinese Journal of Polymer Science, 2026, 441-9. DOI: 10.1007/s10118-026-3702-x.
Li, Q. S.; Mao, H. D.; Wen, L.; Zhang, L. F.; Qin, Z.; Zhang, J. Y.; Luo, D.; Tan, L. C.; Chen, Y. W. Manipulating hierarchical aggregation structure via film-forming kinetics enables organic photovoltaics over 20% efficiency. Chinese J. Polym. Sci. https://doi.org/10.1007/s10118-026-3702-x DOI：

Qin-Sheng Li, Hou-Dong Mao, Lin Wen, et al. Manipulating Hierarchical Aggregation Structure via Film-forming Kinetics Enables Organic Photovoltaics over 20% Efficiency[J/OL]. Chinese Journal of Polymer Science, 2026, 441-9. DOI: 10.1007/s10118-026-3702-x. DOI：

摘要

Abstract

The non-equilibrium dynamics of solvent evaporation and polymer diffusion induce vertical crystallization differences in the donor film

which pose great challenges to the precise control of the ideal vertical phase morphology in pseudo-planar heterojunction (PPHJ) organic photovoltaics (OPVs). In this study

the Peclet number (Pe) was first proposed as a predictive parameter to evaluate the correlation between solvent evaporation and the vertical gradient distribution morphology of the active layer during the film-forming process. This further directs the regulation of the hierarchical aggregation structure and vertical crystallization behavior of the polymer donor

thereby inducing ordered donor/acceptor interpenetration and ultimately achieving the construction of active layers with controllable heterojunction architectures. Depth-dependent light absorption spectroscopy and

in situ

depth-dependent fluorescence intensity measurements confirmed that Pe is about 1 can induce vertical crystallization differences in various polymer donors to form a PPHJ active layer with an ideal vertical gradient distribution morphology. Consequently

the toluene-processed PPHJ devic

e achieved competitive power conversion efficiencies of 20.07%/16.86% (0.04/16.94 cm

)

via

blade coating technology.

关键词

Keywords

references

Wang, S.; Zhong, W.; Huang, F. Recent advancements in stretchable polymer optoelectronics. Acta Polymeric Sinica (in Chinese) 2024 , 55 , 1091−1110..

Jiang Y., Sun S., Xu R.;, Liu F., Miao X., Ran G., Liu K., Yi Y., Zhang W., Zhu X. Nonfullerene acceptor with asymmetric structure and phenyl-substituted alkyl side chain for 20.2% efficiency organic solar cells. Nat. Energy 2024 , 9 , 975−986..

Sun, R.; Yuan, X.; Yang, X.; Wu, Y.; Shao, Y.; Wu, X.; Brabec, C. J.; Min, J. Cost-efficient recycling of organic photovoltaic devices. Joule 2024 , 8 , 2523−2538..

Lu, X.; Liu, Y.; Tian, R.; Liu, X.; Wang, Y.; Zhou, Y. Enhanced moisture and thermal stability of transparent electrodes via cross-linking for large-area flexible organic photovoltaic modules. Energy Environ. Sci. 2025 , 18 , 2426−2435..

Baran, D.; Ashraf, R. S.; Hanifi, D. A.; Abdelsamie, M.; Gasparini, N.; Röhr, J. A.; Holliday, S.; Wadsworth, A.; Lockett, S.; Neophytou, M.; Emmott, CJM.; Nelson, J.; Brabec, CJ.; Amassian, A.; Salleo, A.; Kirchartz, T.; Durrant, J. R.; McCulloch, I. Reducing the efficiency-stability-cost gap of organic photovoltaics with highly efficient and stable small-molecule acceptor ternary solar cells. Nat. Mater. 2017 , 16 , 363−369..

Cui Y., Wang Y., Bergqvist J., Yao H., Xu Y., Gao B., Yang C., Zhang S., Inganäs O., Gao F., Hou J. Wide-gap nonfullerene acceptor enabling high-performance organic photovoltaic cells for indoor applications. Nat. Energy 2019 , 4 , 768−775..

Classen, A.; Chochos, CL.; Lüer, L.; Gregoriou, VG.; Wortmann, J.; Osvet, A.; Forberich, K.; McCulloch, I.; Heumüller, T.; Brabec, CJ. Role of exciton lifetime in charge generation in organic solar cells at negligible energy level offsets. Nat. Energy 2020 , 5 , 711−719..

Maimaris, M.; Pettipher, AJ.; Azzouzi, M.; Walke, DJ.; Zheng, X.; Gorodetsky, A.; Dong, Y.; Tuladhar, PS.; Crespo, H.; Nelson, J.; Tisch, JWG.; Bakulin, AA. Sub-10-fs observation of bound exciton formation in organic optoelectronic devices. Nat. Commun. 2022 , 13 , 4949..

Zhang, L.; Mao, H.; Huang, L.; Hu, L.; Wang, X.; Tan, L.; Chen, Y. Achieving improved stability and minimal nonradiative recombination loss for over 18% binary organic photovoltaics via a versatile interfacial regulation strategy. Sci. China Chem. 2022 , 65 , 1623−1633..

[Hu, H.; Jin, Z.; Ge, J.; Shen, C.; Xie, L.; Song, W.; Ye, Q.; Ding, P.; Li, J.; Han, C.; Yu, X.; Liu, Q.; Ge, Z. 17.68% Efficiency nonhalogenated solvent-processed organic solar cell modules driven by seed crystal strategy. Adv. Mater . 2025 , 37 , 2420308..

Jia, L.; Wu, M.; Ru, M.; Li, Y.; Li, S.; Xia, C.; Zhao, W. Sustainable organic solar cells via renewable biomass and circular recycling. Matter 2025 , 8 , 102291..

Li, Y.; Guo, Y.; Chen, Z.; Zhan, L.; He, C.; Bi, Z.; Yao, N.; Li, S.; Zhou, G.; Yi, Y.; Yang, Y (Michael). Zhu H., Ma W., Gao F., Zhang F., Zuo L., Chen H. Mechanism study on organic ternary photovoltaics with 18.3% certified efficiency: from molecule to device. Energy Environ. Sci. 2022 , 15 , 855−865..

[Ma, R.; Luo, Z.; Zhang, Y. Organic solar cells: beyond 20%. Sci. China Mater . 2025 , 68 . 1689−1701..

[Cheng, B.; Xia, X.; Fu, Z. Achieving 20.9% efficiency organic solar cell enabled by dual-additive-targeted engineering. Sci. China Chem . 2026 , 69 . 1869−1870..

Bai, Y.; Li, S.; Wang, Q. Simultaneous enhancement of efficiency, stability, and stretchability in binary polymer solar cells with a three-dimensional aromatic core tethered tetrameric acceptor. Natl. Sci. Rev. 2025 , 12 , nwaf019..

Cheng, F.; Lai, S.; Zhang, Y.; Xue, L.; Xia, X.; Zhu, P.; Lu, X.; Liao, X.; Chen, Y. Random terpolymer based on simple siloxane-functionalized thiophene unit enabling high-performance non-fullerene organic solar cells. Chinese J. Polym. Sci. 2024 , 42 , 311−321..

He C., Pan Y., Lu G., Wu B., Xia X., Ma C., Chen Z., Zhu H., Lu X., Ma W., Zuo L., Chen H. Versatile sequential casting processing for highly efficient and stable binary organic photovoltaics. Adv. Mater. 2022 , 34 , 2203379..

Jia, Z.; Pan, J.; Chen, X.; Li, Y.; Liu, T.; Zhu, H.; Yao, J.; Yan, B.; Yang, Y (Michael). Eco-friendly volatile additives enable efficient large-area organic photovoltaic modules to be processed with non-halogenated solvents. Energy Environ. Sci. 2024 , 17 , 3908−3916..

Zheng, Y.; Sun, R.; Zhang, M.; Chen, Z.; Peng, Z.; Wu, Q.; Yuan, X.; Yu, Y.; Wang, T.; Wu, Y.; Hao, X.; Lu, G.; Ade, H.; Min, J. Baseplate temperature-dependent vertical composition gradient in pseudo-bilayer films for printing non-fullerene organic solar cells. Adv. Energy Mater. 2021 , 11 , 2102135..

[Zhou, J.; Man, X.; Jiang, Y.; Doi, M. Structural formation in soft matter solutions induced by solvent evaporation. Adv. Mater . 2017 , 29 , 1703769..

Routh, AF.; Zimmerman, WB. Distribution of particles during solvent evaporation from films. Chem. Eng. Sci. 2004 , 59 , 2961..

[Luo, X.; Yang, W.; Lin, Y.; Wu, J.; Zhang, X.; Peng, F.; Z hong, W.; Qiao, X.; Li, N.; Ma, D.; Ying, L.; Improving efficiency of organic photovoltaics by manipulating critical concentration of polymer in bulk-heterojunction solution. Adv. Funct. Mater . 2024 , 34 , 2409323..

Zeng, R.; Zhang, M.; Wang, X.; Zhu, L.; Hao, B.; Zhong,W.; Zhou, G.; Deng, J.; Tan, S.; Zhuang, J.; Han, F.; Zhang, A.; Zhou, Z.; Xue, X.; Xu, S.; Xu, J.; Liu, Y.; Lu, H.; Wu, X.; Wang, C.; Fink, Z.; RussII, T.; Jing, H.; Zhang, Y.; Bo, Z.; Liu, F. Achieving 19% efficiency in non-fused-ring electron acceptor solar cells via solubility control of donor and acceptor crystallization. Nat. Energy 2024 , 9 , 1117−1128..

Zhang, B.; Chen, W.; Chen, H.; Zeng, G.; Zhang, R.; Li, H.; Wang, Y.; Gu, X.; Sun, W.; Gu, H.; Gao, F.; Li, Y.; Li, Y. Rapid solidification for green solvent-processed large-area organic solar modules with > 16% efficiency. Energy Environ. Sci. 2024 , 17 , 2935−2944..

Wen L.; Mao H.; Ban M.; Tan L.; Zhang J.; Qin Z.; Zhang L.; Chen Y. Constructing controlled vertical gradient morphology in pseudo-planar heterojunction organic photovoltaics via self-assembled interface orthogonal strategy. Adv. Mater. 2025 , 37 , 2503813..

[Fu, Z.; Qiao, J.; Cui, F.; Zhang, W.; Wang, L.; Lu, P.; Yin, H.; Du, X.; Qin, W.; Hao, X. π–π Stacking modulation via polymer adsorption for long exciton diffusion in high-efficiency thick-film organic solar cells. Adv. Mater . 2024 , 36 , 2313532..

Fu, Z.; He, W.; Yao, Y.; Qiu, Z.; Chen, H.; Li, C.; Wang, K.; Zhang, Q.; Kwok, R. K.; Tang, B. Z.; Fu, Q. Pursuing phase transitions of a concentrated polymer solution by in situ fluorescence measurements based on aggregation-induced emission. J. Phys. Chem. Lett. 2022 , 13 , 9855−9861..

Wen, L.; Mao, H.; Zhang, L.; Zhang, J.; Qin, Z.; Tan, L.; Chen, Y. Achieving the desired pseudoplanar heterojunction organic solar cells via binary-dilution strategy. Adv. Mater. 2024 , 36 , 2308159..

Xue, J.; Zhao, H. Lin, B.; Wang, Y.; Zhu, Q.; Lu, G.; Wu, B.; Bi, Z.; Zhou, X.; Zhao, C.; Lu, G.; Zhou, K.; Ma, W. Nonhalogenated dual-slot die processing enables high-efficiency organic solar cells. Adv. Mater. 2022 , 34 , 2202659..

Li, S.; He, C.; Chen, T.; Zheng, J.; Sun, R.; Fang, J.; Chen, Y.; Pan, Y.; Yan, K.; Li, C-Z.; Shi, M.; Zuo, L.; Ma, C. Q.; Min, J.; Liu, Y.; Ch en, H. Refined molecular microstructure and optimized carrier management of multicomponent organic photovoltaics toward 19.3% certified efficiency. Energy Environ. Sci. 2023 , 16 , 2262−2273..

Wei, Y.; Zhou, X.; Cai, Y. High-performance as-cast organic solar cells enabled by a refined double-fibril network morphology and improved dielectric constant of the active layer. Adv. Mater. 2024 , 36 , 2403294..

Wang, T.; Brédas, J. L. Organic photovoltaics: understanding the preaggregation of polymer donors in solution and its morphological impact. J. Am. Chem. Soc. 2021 , 143 , 1822−1835..

Liang, Q.; Jiao, X.; Yan, Y.; Xie, Z.; Lu, G.; Liu, J.; Han, Y. Separating crystallization process of p3ht and o-idtbr to construct highly crystalline interpenetrating network with optimized vertical phase separation. Adv. Funct. Mater. 2019 , 29 , 1807591..

Zhang, J.; Mao, H.; Zhou, K.; Zhang, L.; Luo, D.; Wang, P.; Ye, L.; Chen, Y. Polymer-entangled spontaneous pseudo-planar heterojunction for constructing efficient flexible organic solar cells. Adv. Mater. 2024 , 36 , 2309379..

Gao, W.; Ma, R.; Dela Peña, T. A.; Yan, C.; Li, H.; Li, M.; Wu, J.; Cheng, P.; Zhong, C.; Wei, Z.; Jen, AK-Y.; Li, G. Efficient all-small-molecule organic solar cells processed with non-halogen solvents. Nat. Commun. 2024 , 15 , 1946..

Zhong, W.; Zhang, M.; Freychet, G.; Su, G. M.; Ying, L.; Huang, F.; Cao, Y.; Zhang, Y.; Wang, C.; Liu, F. Decoupling complex multi-length-scale morphology in non-fullerene photovoltaics with nitrogen k-edge resonant soft X-ray scattering. Adv. Mater. 2022 , 34 , 2107316..

Cui, F.; Qiao, J.; Xu, Y.; Fu, Z.; Gui,, R.; Zhang, C.; Zhou, R.; Ye, L.; Du, X.; Chen, F.; Hao, X.; Yan, H.; Yin, H. Using an external electric field to tune active layer morphology enabling high-efficiency organic solar cells via ambient blade coating. Sci. Adv. 2024 , 10 , eado5460..

Wang, C.; Ma, X.; Deng, D.; Zhang, H.; Sun, R.; Zhang, J.; Zhang, L.; Wu, M.; Min, J.; Zhang, Z-G.; Wei, Z. Giant dimeric donors for all-giant oligomer organic solar cells with efficiency over 16% and superior photostability. Nat. Commun. 2024 , 15 , 8494..

Lu, L.; Chen, W.; Xu, T.; Yu, L. High-performance t ernary blend polymer solar cells involving both energy transfer and hole relay processes. Nat. Commun. 2015 , 6 , 7327..

[Zhang, G.; Chen, X. K.; Xiao, J. Delocalization of exciton and electron wavefunctions in non-fullerene acceptor molecules enables efficient organic solar cells. Nat. Commun . 2020 , 11 , 3943..

浏览量

Downloads

CSCD

文章被引用时，请邮件提醒。

Submit

工具集

关联资源

Scaling Behaviors of Polymers on Lipid Membranes: Coupling of Polymer Chain Dynamics and Surface Thermal Fluctuations

A Low Reorganization Energy and Two-dimensional Acceptor with Four End Units for Organic Solar Cells with Low Eloss

Hypercrosslinked Porous Organic Polymers from Tetraaniline and Anthraquinone for High-capacitance, Long-life Supercapacitors

Ultralong Sodium Alginate-based Room/High-temperature Phosphorescence Materials with Color-tunability and Flexibility

Microenvironment Responsive Polymeric Nitric Oxide Releasing Micelles for Enhancing Eradication of Methicillin-resistant Staphylococcus aureus Biofilm

Manipulating Hierarchical Aggregation Structure via Film-forming Kinetics Enables Organic Photovoltaics over 20% Efficiency

Manipulating Hierarchical Aggregation Structure via Film-forming Kinetics Enables Organic Photovoltaics over 20% Efficiency

DOI：10.1007/s10118-026-3702-x

摘要

Abstract

关键词

Keywords

references