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<p>Achieving simultaneously high open-circuit voltage (<i>V</i><sub>OC</sub>) and fill factor (FF) remains a central challenge for high-performance organic solar cells (OSCs), as excessive crystallization or energetic disorder often leads to a severe trade-off between voltage loss and charge transport. Here, we demonstrate a synergistic strategy that integrates asymmetric non-fullerene acceptor (NFA) design with additive-controlled crystallization to overcome this limitation in binary OSCs. Two asymmetric acceptors, AS-N3-4F and AS-N3-4Cl, were developed by introducing an asymmetric side-chain architecture into the N3 framework, combined with terminal halogenation. These acceptors exhibit suitable energy levels, preferred face-on orientation, and well-regulated molecular packing. By systematically comparing two widely used solvent additives, 1-chloronaphthalene (1-CN) and 1,8-diiodooctane (DIO), we reveal that asymmetric acceptor geometry fundamentally alters the crystallization response to different additives. In contrast to DIO, 1-CN effectively moderates the crystallization behavior by reducing the π-π interactions, suppressing over-crystallization, and reducing non-radiative recombination loss, leading to simultaneous enhancement of <i>V</i><sub>OC</sub> and FF without sacrificing short-circuit current density. As a result, the D18:AS-N3-4F-based device processed with 1-CN achieves a power conversion efficiency of 20.01%, with a high <i>V</i><sub>OC</sub> of 0.903 V and an excellent FF of 80.5%, whereas DIO-processed devices suffer from increased voltage loss. This work elucidates the critical interplay between asymmetric molecular design and additive-controlled crystallization, providing practical guidelines for achieving high-efficiency OSCs.</p>

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Asymmetric acceptor engineering and additive-controlled crystallization synergize to yield efficient binary organic solar cells

  • 期刊论文

  • 发表日期：

    2026年4月30日

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  • Zhenyu Chen,
  • Shanshan Qin,
  • Bowen Deng,
  • Yongchao Hu,
  • Pengfei Ding,
  • Daobin Yang,
  • Kang Wang,
  • Jingyu Shi,
  • Xuelin Wang,
  • Tao Zhang,
  • Kangqiao Ma,
  • Zaifei Ma,
  • Deping Qian,
  • Ziyi Ge

摘要

Achieving simultaneously high open-circuit voltage (VOC) and fill factor (FF) remains a central challenge for high-performance organic solar cells (OSCs), as excessive crystallization or energetic disorder often leads to a severe trade-off between voltage loss and charge transport. Here, we demonstrate a synergistic strategy that integrates asymmetric non-fullerene acceptor (NFA) design with additive-controlled crystallization to overcome this limitation in binary OSCs. Two asymmetric acceptors, AS-N3-4F and AS-N3-4Cl, were developed by introducing an asymmetric side-chain architecture into the N3 framework, combined with terminal halogenation. These acceptors exhibit suitable energy levels, preferred face-on orientation, and well-regulated molecular packing. By systematically comparing two widely used solvent additives, 1-chloronaphthalene (1-CN) and 1,8-diiodooctane (DIO), we reveal that asymmetric acceptor geometry fundamentally alters the crystallization response to different additives. In contrast to DIO, 1-CN effectively moderates the crystallization behavior by reducing the π-π interactions, suppressing over-crystallization, and reducing non-radiative recombination loss, leading to simultaneous enhancement of VOC and FF without sacrificing short-circuit current density. As a result, the D18:AS-N3-4F-based device processed with 1-CN achieves a power conversion efficiency of 20.01%, with a high VOC of 0.903 V and an excellent FF of 80.5%, whereas DIO-processed devices suffer from increased voltage loss. This work elucidates the critical interplay between asymmetric molecular design and additive-controlled crystallization, providing practical guidelines for achieving high-efficiency OSCs.