<p>All-polymer solar cells (all-PSCs) have attracted significant attention owing to their excellent stability and mechanical stretchability. However, achieving high-performance all-PSCs remains challenging due to the difficulty in controlling the morphology of polymer blend films. In this study, a novel polymer donor, PBDTF-DTP, incorporating a weak electron-withdrawing yet large-dipole-moment dithienylphthalimide (DTP-2T) unit, was rationally designed and synthesized for ternary all-PSCs. Introducing PBDTF-DTP as a guest donor not only enables complementary light absorption in the active layer but also deepens the highest occupied molecular orbital level, which is beneficial for simultaneously improving the short-circuit current density (<i>J</i><sub>SC</sub>) and open-circuit voltage (<i>V</i><sub>OC</sub>). Besides, the large dipole moment of the DTP-2T unit helps to increase the dielectric constant, which suppresses non-radiative energy loss and further boosts <i>V</i><sub>OC</sub>. Notably, PBDTF-DTP exhibits a relatively higher molecular electrostatic potential than the host donor, which effectively tunes its compatibility with both the polymer donor and acceptor, thereby regulating the blend morphology and promoting the formation of a nanoscale fibrillar network within the active layer. Such well-optimized morphology facilitates more efficient charge generation and transport while suppressing charge recombination. As a result, the ternary all-PSC based on PM6:PBDTF-DTP:PYIT achieves a synergistic enhancement in <i>J</i><sub>SC</sub>, <i>V</i><sub>OC</sub>, and fill factor, yielding a remarkable power conversion efficiency of 18.01%, significantly higher than that of the binary PM6:PYIT device (15.51%). This study demonstrates that combining electrostatic potential optimization with a ternary strategy provides an effective approach to regulate the morphology of all-polymer blends and achieve high-efficiency all-PSCs.</p>

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Electrostatic regulation of high-dipole dithienophthalimide-based wide-bandgap polymer for efficient ternary all-polymer solar cells

  • Mingtao Liu,
  • Jin Li,
  • Feng Ding,
  • Yuang Fu,
  • Jinyang Yu,
  • Peipei Zhu,
  • Dan Liu,
  • Meng Tao,
  • Ruizhuo Yu,
  • Xinhui Lu,
  • Haiming Zhu,
  • Xunfan Liao,
  • Yiwang Chen

摘要

All-polymer solar cells (all-PSCs) have attracted significant attention owing to their excellent stability and mechanical stretchability. However, achieving high-performance all-PSCs remains challenging due to the difficulty in controlling the morphology of polymer blend films. In this study, a novel polymer donor, PBDTF-DTP, incorporating a weak electron-withdrawing yet large-dipole-moment dithienylphthalimide (DTP-2T) unit, was rationally designed and synthesized for ternary all-PSCs. Introducing PBDTF-DTP as a guest donor not only enables complementary light absorption in the active layer but also deepens the highest occupied molecular orbital level, which is beneficial for simultaneously improving the short-circuit current density (JSC) and open-circuit voltage (VOC). Besides, the large dipole moment of the DTP-2T unit helps to increase the dielectric constant, which suppresses non-radiative energy loss and further boosts VOC. Notably, PBDTF-DTP exhibits a relatively higher molecular electrostatic potential than the host donor, which effectively tunes its compatibility with both the polymer donor and acceptor, thereby regulating the blend morphology and promoting the formation of a nanoscale fibrillar network within the active layer. Such well-optimized morphology facilitates more efficient charge generation and transport while suppressing charge recombination. As a result, the ternary all-PSC based on PM6:PBDTF-DTP:PYIT achieves a synergistic enhancement in JSC, VOC, and fill factor, yielding a remarkable power conversion efficiency of 18.01%, significantly higher than that of the binary PM6:PYIT device (15.51%). This study demonstrates that combining electrostatic potential optimization with a ternary strategy provides an effective approach to regulate the morphology of all-polymer blends and achieve high-efficiency all-PSCs.