Achieving 20.1% Efficiency in Organic Solar Cells Through Interconnected Fibrillar Networks via Local Molecular Stacking

Junying Wu , Wanqing You , Xuanang Luo , Xiaojing Wang , Zhiyuan Yang , Junhao Zeng , Jingchuan Chen , Cheng Wang , Lei Ying , Wenkai Zhong , Zhicai He , Yong Cao

Aggregate ›› 2026, Vol. 7 ›› Issue (3) : e70305

PDF (8827KB)
Aggregate ›› 2026, Vol. 7 ›› Issue (3) :e70305 DOI: 10.1002/agt2.70305
RESEARCH ARTICLE
Achieving 20.1% Efficiency in Organic Solar Cells Through Interconnected Fibrillar Networks via Local Molecular Stacking
Author information +
History +
PDF (8827KB)

Abstract

The performance of organic solar cells (OSCs) is governed by how molecular packing evolves into interconnected networks that facilitate exciton dissociation and charge transport. Using an all-small-molecule blend DR3TSBDT:Y6 as a model system, we study how local molecular stacking evolves into performance-relevant morphology during solvent vapor annealing (SVA) and subsequent thermal annealing (TA). SVA promotes end-to-end stacking of amorphous acceptors to form interconnected fibrils, while TA compacts inter-fibril spacing without disrupting favorable local order. Such molecular-to-morphological refinements broaden light absorption, enhance charge transport, and markedly improve device efficiency. Extending this approach to additional blend systems (D18:Y6, D18:L8-BO, and DR3TSBDT:L8-BO) yields similar structural evolution and performance gains, with the D18:L8-BO system achieving up to 20.10% PCE. Our study establishes control over local stacking in amorphous acceptors into fibrillar networks as a general and effective route to realize high-performance OSCs.

Keywords

amorphous / molecular stacking / morphology / organic solar cells / post-treatments

Cite this article

Download citation ▾
Junying Wu, Wanqing You, Xuanang Luo, Xiaojing Wang, Zhiyuan Yang, Junhao Zeng, Jingchuan Chen, Cheng Wang, Lei Ying, Wenkai Zhong, Zhicai He, Yong Cao. Achieving 20.1% Efficiency in Organic Solar Cells Through Interconnected Fibrillar Networks via Local Molecular Stacking. Aggregate, 2026, 7 (3) : e70305 DOI:10.1002/agt2.70305

登录浏览全文

4963

注册一个新账户 忘记密码

References

[1]

J. Zhang, X. Duan, X. Li, et al., “Achieving 20% Efficiency in Binary Organic Solar Cells With Suppressed Non-Radiative Recombination via Triphenylamine Halides,” Energy & Environmental Science 18 (2025): 5378-5388.

[2]

H. Chen, Y. Huang, R. Zhang, et al., “Organic Solar Cells With 20.82% Efficiency and High Tolerance of Active Layer Thickness Through Crystallization Sequence Manipulation,” Nature Materials 24 (2025): 444-453.

[3]

C. Li, J. Song, H. Lai, et al., “Non-Fullerene Acceptors With High Crystallinity and Photoluminescence Quantum Yield Enable >20% Efficiency Organic Solar Cells,” Nature Materials 24 (2025): 433-443.

[4]

H. Mou, Y. Yin, H. Chen, et al., “Transient Dipole Strategy Boosts Highly Oriented Self-Assembled Monolayers for Organic Solar Cells Approaching 21% Efficiency,” Journal of the American Chemical Society 147 (2025): 21241-21251.

[5]

J. Wang, Y. Xie, K. Chen, H. Wu, J. M. Hodgkiss, and X. Zhan, “Physical Insights Into Non-Fullerene Organic Photovoltaics,” Nature Reviews Physics 6 (2024): 365-381.

[6]

Y. Sun, L. Wang, C. Guo, et al., “π-Extended Nonfullerene Acceptor for Compressed Molecular Packing in Organic Solar Cells to Achieve Over 20% Efficiency,” Journal of the American Chemical Society 146 (2024): 12011-12019.

[7]

D. Li, N. Deng, Y. Fu, et al., “Fibrillization of Non-Fullerene Acceptors Enables 19% Efficiency Pseudo-Bulk Heterojunction Organic Solar Cells,” Advanced Materials 35 (2023): 2208211.

[8]

H. M. Kwon, S. V. Barma, L. Zuo, et al., “Highly Efficient Organic Solar Cells Based on S,N-Heteroacene Non-Fullerene Acceptors,” Chemistry of Materials 30 (2018): 5429-5434.

[9]

M. Deng, X. Xu, Y. Duan, L. Yu, R. Li, and Q. Peng, “Y-Type Non-Fullerene Acceptors With Outer Branched Side Chains and Inner Cyclohexane Side Chains for 19.36% Efficiency Polymer Solar Cells,” Advanced Materials 35 (2023): 2210760.

[10]

F. Sun, J. Wu, B. Cheng, et al., “Constructing Continuous Acceptor Fibrillar Networks and Achieving Uniform Phase Separation via Polymer-Assisted Morphology Control for 20.3% Efficiency Additive-Free Organic Solar Cells,” Energy & Environmental Science 18 (2025): 7071-7081.

[11]

L. Zhu, M. Zhang, J. Xu, et al., “Single-Junction Organic Solar Cells With Over 19% Efficiency Enabled by a Refined Double-Fibril Network Morphology,” Nature Materials 21 (2022): 656-663.

[12]

W. Zhong, S. Wang, and F. Liu, “Unlocking Functional Potentials: Nanofibril Networks in Organic Semiconductors,” Advanced Nanocomposites 2 (2025): 124-147.

[13]

M. Zhou, C. Liao, Y. Duan, et al., “19.10% Efficiency and 80.5% Fill Factor Layer-by-Layer Organic Solar Cells Realized by 4-Bis(2-Thienyl)Pyrrole-2,5-Dione Based Polymer Additives for Inducing Vertical Segregation Morphology,” Advanced Materials 35 (2023): 2208279.

[14]

F. Qi, L. O. Jones, K. Jiang, et al., “Regiospecific N -Alkyl Substitution Tunes the Molecular Packing of High-Performance Non-Fullerene Acceptors,” Materials Horizons 9 (2022): 403-410.

[15]

Z. Li, J. Xie, W. Wang, et al., “Achieving 19.6% Efficiency in Organic Photovoltaics Through Guest-Polymer Assisted Morphological Fibrillization,” Energy & Environmental Science 18 (2025): 3026-3035.

[16]

X. Zhang, X. Li, X. Kong, et al., “Fine-Tuning of Molecular Self-Assembly Morphology via Synergistic Ternary Copolymerization and Side Chain Optimization of Low-Cost Polymer Donors toward Efficient Organic Solar Cells,” Advanced Materials 37 (2025): 2503325.

[17]

L. Xue, Q. Xie, W. Xie, et al., “Precise Side-Chain Engineering Optimizes Polymer Pre-Aggregation and Crystallinity for Efficient Organic Solar Cells with Minimized Non-Radiative Energy Loss,” Aggregate 6 (2025): e70103.

[18]

L. Ye, K. Weng, J. Xu, et al., “Unraveling the Influence of Non-Fullerene Acceptor Molecular Packing on Photovoltaic Performance of Organic Solar Cells,” Nature Communications 11 (2020): 6005.

[19]

Z. Chen, J. Ge, W. Song, et al., “20.2% Efficiency Organic Photovoltaics Employing a π-Extension Quinoxaline-Based Acceptor With Ordered Arrangement,” Advanced Materials 36 (2024): 2406690.

[20]

J. Zhou, L. Wang, C. Liu, et al., “Tuning of the Polymeric Nanofibril Geometry via Side-Chain Interaction Toward 20.1% Efficiency of Organic Solar Cells,” Journal of the American Chemical Society 146 (2024): 34998-35006.

[21]

B. Fan, W. Gao, X. Wu, et al., “Importance of Structural Hinderance in Performance-stability Equilibrium of Organic Photovoltaics,” Nature Communications 13 (2022): 5946.

[22]

Y. Fu, T. H. Lee, Y.-C. Chin, et al., “Molecular Orientation-Dependent Energetic Shifts in Solution-Processed Non-Fullerene Acceptors and Their Impact on Organic Photovoltaic Performance,” Nature Communications 14 (2023): 1870.

[23]

X. Liu, Z. He, H. Wang, et al., “Unraveling Cross-Scale Fluorination Mechanisms in Non-Fullerene Acceptors for High-Efficiency Organic Photovoltaics,” Advanced Functional Materials 36 (2025): e17542.

[24]

N. Gasparini, A. Salleo, I. McCulloch, and D. Baran, “The Role of the Third Component in Ternary Organic Solar Cells,” Nature Reviews Materials 4 (2019): 229-242.

[25]

Y. Cai, Y. Li, R. Wang, et al., “A Well-Mixed Phase Formed by Two Compatible Non-Fullerene Acceptors Enables Ternary Organic Solar Cells With Efficiency Over 18.6%,” Advanced Materials 33 (2021): 2101733.

[26]

L. Zhu, M. Zhang, G. Zhou, et al., “Efficient Organic Solar Cell With 16.88% Efficiency Enabled by Refined Acceptor Crystallization and Morphology With Improved Charge Transfer and Transport Properties,” Advanced Energy Materials 10 (2020): 1904234.

[27]

C. Li, J. Zhou, J. Song, et al., “Non-Fullerene Acceptors With Branched Side Chains and Improved Molecular Packing to Exceed 18% Efficiency in Organic Solar Cells,” Nature Energy 6 (2021): 605-613.

[28]

J. Song, M. Zhang, T. Hao, et al., “Design Rules of the Mixing Phase and Impacts on Device Performance in High-Efficiency Organic Photovoltaics,” Research 2022 (2022): 9817267.

[29]

M. Ghasemi, H. Hu, Z. Peng, et al., “Delineation of Thermodynamic and Kinetic Factors That Control Stability in Non-Fullerene Organic Solar Cells,” Joule 3 (2019): 1328-1348.

[30]

K. An, W. Zhong, F. Peng, et al., “Mastering Morphology of Non-Fullerene Acceptors Towards Long-Term Stable Organic Solar Cells,” Nature Communications 14 (2023): 2688.

[31]

J. Guo, B. Qiu, X. Xia, et al., “Miscibility Regulation and Thermal Annealing Induced Hierarchical Morphology Enables High-Efficiency All-Small-Molecule Organic Solar Cells Over 17%,” Advanced Energy Materials 13 (2023): 2300481.

[32]

Q. Yue, H. Wu, Z. Zhou, M. Zhang, F. Liu, and X. Zhu, “13.7% Efficiency Small-Molecule Solar Cells Enabled by a Combination of Material and Morphology Optimization,” Advanced Materials 31 (2019): 1904283.

[33]

J. Min, X. Jiao, I. Ata, et al., “Time-Dependent Morphology Evolution of Solution-Processed Small Molecule Solar Cells During Solvent Vapor Annealing,” Advanced Energy Materials 6 (2016): 1502579.

[34]

M. Li, F. Liu, X. Wan, et al., “Subtle Balance between Length Scale of Phase Separation and Domain Purification in Small-Molecule Bulk-Heterojunction Blends Under Solvent Vapor Treatment,” Advanced Materials 27 (2015): 6296.

[35]

W. Zhu, A. P. Spencer, S. Mukherjee, et al., “Crystallography, Morphology, Electronic Structure, and Transport in Non-Fullerene/Non-Indacenodithienothiophene Polymer:Y6 Solar Cells,” Journal of the American Chemical Society 142 (2020): 14532-14547.

[36]

K. Gao, W. Deng, L. Xiao, et al., “New Insight of Molecular Interaction, Crystallization and Phase Separation in Higher Performance Small Molecular Solar Cells via Solvent Vapor Annealing,” Nano Energy 30 (2016): 639-648.

[37]

Y. Chen, K. Li, J. Zhang, et al., “Over 19% Efficiency Polymer Solar Cells Enabled by Selectively Tuning Bulkheterojunction Morphology via a Dual-Heating Strategy,” Small Methods 9 (2025): e01159.

[38]

J. Hao, Y. Feng, Q. Ma, et al., “Real-Time Probing of Morphological Evolution and Recrystallization During Solvent Annealing in Blade-Coated All-Polymer Organic Solar Cells Using In Situ X-Ray Scattering,” Advanced Science 12 (2025): e01823.

[39]

C. Cui and Y. Li, “Morphology Optimization of Photoactive Layers in Organic Solar Cells,” Aggregate 2 (2021): e31.

[40]

Y. Wang, J. Yu, R. Zhang, et al., “Origins of the Open-Circuit Voltage in Ternary Organic Solar Cells and Design Rules for Minimized Voltage Losses,” Nature Energy 8 (2023): 978-988.

[41]

Y. Li, Y. Cai, Y. Xie, et al., “A Facile Strategy for Third-Component Selection in Non-Fullerene Acceptor-Based Ternary Organic Solar Cells,” Energy & Environmental Science 14 (2021): 5009.

[42]

L. J. A. Koster, V. D. Mihailetchi, R. Ramaker, and P. W. M. Blom, “Light Intensity Dependence of Open-Circuit Voltage of Polymer:Fullerene Solar Cells,” Applied Physics Letters 86 (2005): 123509.

[43]

A. K. K. Kyaw, D. H. Wang, V. Gupta, et al., “Intensity Dependence of Current-Voltage Characteristics and Recombination in High-Efficiency Solution-Processed Small-Molecule Solar Cells,” ACS Nano 7 (2013): 4569-4577.

[44]

V. D. Mihailetchi, L. J. A. Koster, J. C. Hummelen, and P. W. M. Blom, “Photocurrent Generation in Polymer-Fullerene Bulk Heterojunctions,” Physical Review Letter 93 (2004): 216601.

[45]

W. Zhong, J. Cui, B. Fan, et al., “Enhanced Photovoltaic Performance of Ternary Polymer Solar Cells by Incorporation of a Narrow-Bandgap Nonfullerene Acceptor,” Chemistry of Materials 29 (2017): 8177-8186.

[46]

M. Stephen, K. Genevičius, G. Juška, K. Arlauskas, and R. C. Hiorns, “Charge Transport and Its Characterization Using Photo- CELIV in Bulk Heterojunction Solar Cells,” Polymer International 66 (2017): 13-25.

[47]

M. E. Ziffer, S. B. Jo, H. Zhong, et al., “Long-Lived, Non-Geminate, Radiative Recombination of Photogenerated Charges in a Polymer/Small-Molecule Acceptor Photovoltaic Blend,” Journal of the American Chemical Society 140 (2018): 9996-10008.

[48]

Y. Liu, L. Zuo, X. Shi, A. K. Y. Jen, and D. S. Ginger, “Unexpectedly Slow yet Efficient Picosecond to Nanosecond Photoinduced Hole-Transfer Occurs in a Polymer/Nonfullerene Acceptor Organic Photovoltaic Blend,” ACS Energy Letters 3 (2018): 2396-2403.

[49]

C. Huang, D. Kim, W. Yang, et al., “Amphiphilic Polymer Conetworks for Non-Fullerene Organic Solar Cells: Regulated Molecular Stacking Enables Efficient Downconversion,” Advanced Energy Materials 16 (2025): e04273.

[50]

G. Xie, J. Wang, J. Lv, et al., “Fully Locked Conjugated Backbones in Simple-Structured Polymer Donors Enabling High-Performance Organic Solar Cells,” Angewandte Chemie International Edition 137 (2025): e18567.

[51]

W. Zhang, J. Huang, J. Xu, et al., “Phthalimide Polymer Donor Guests Enable Over 17% Efficient Organic Solar Cells via Parallel-like Ternary and Quaternary Strategies,” Advanced Energy Materials 10 (2020): 2001436.

[52]

K. Jiang, J. Lu, R. J. E. Westbrook, et al., “Photoluminescent Delocalized Excitons in Donor Polymers Facilitate Efficient Charge Generation for High-Performance Organic Photovoltaics,” Nature Communications 16 (2025): 3176.

[53]

M. Zhang, L. Zhu, T. Hao, et al., “High-Efficiency Organic Photovoltaics Using Eutectic Acceptor Fibrils to Achieve Current Amplification,” Advanced Materials 33 (2021): 2007177.

[54]

Y. Wei, X. Zhou, Y. Cai, et al., “High Performance as-Cast Organic Solar Cells Enabled by a Refined Double-Fibril Network Morphology and Improved Dielectric Constant of Active Layer,” Advanced Materials 36 (2024): 2403294.

[55]

J. Song, C. Li, H. Ma, et al., “Optimizing Double-Fibril Network Morphology via Solid Additive Strategy Enables Binary All-Polymer Solar Cells With 19.50% Efficiency,” Advanced Materials 36 (2024): 2406922.

[56]

B. A. Collins, Z. Li, J. R. Tumbleston, E. Gann, C. R. McNeill, and H. Ade, “Absolute Measurement of Domain Composition and Nanoscale Size Distribution Explains Performance in PTB7:PC 71 BM Solar Cells,” Advanced Energy Materials 3 (2013): 65-74.

[57]

D. Kroh, F. Eller, K. Schötz, et al., “Identifying the Signatures of Intermolecular Interactions in Blends of PM6 With Y6 and N4 Using Absorption Spectroscopy,” Advanced Functional Materials 32 (2022): 2205711.

[58]

G. Zhang, X. K. Chen, J. Xiao, et al., “Delocalization of Exciton and Electron Wavefunction in Non-Fullerene Acceptor Molecules Enables Efficient Organic Solar Cells,” Nature Communications 11 (2020): 3943.

[59]

H. Zhang, C. Tian, Z. Zhang, et al., “Concretized Structural Evolution Supported Assembly-Controlled Film-Forming Kinetics in Slot-Die Coated Organic Photovoltaics,” Nature Communications 14 (2023): 6312.

[60]

E. Sebastian, A. M. Philip, A. Benny, and M. Hariharan, “Null Exciton Splitting in Chromophoric Greek Cross(+) Aggregate,” Angewandte Chemie International Edition 57 (2018): 15696-15701.

[61]

M. Kasha, “Energy Transfer Mechanisms and the Molecular Exciton Model for Molecular Aggregates,” Radiation Research 20 (1963): 55.

[62]

M. Kasha, H. R. Rawls, and M. A. El-Bayoumi, “The Exciton Model in Molecular Spectroscopy,” Pure and Applied Chemistry 11 (1965): 371-392.

RIGHTS & PERMISSIONS

2026 The Author(s). Aggregate published by SCUT, AIEI, and John Wiley & Sons Australia, Ltd.

PDF (8827KB)

0

Accesses

0

Citation

Detail

Sections
Recommended

/