<p>Hole-selective self-assembled monolayers have advanced the performance of perovskite solar cells (PSCs), yet their excessive intermolecular interactions result in undesirable self-aggregation and weak interfacial contact. Here we devise a bicarbazole-based dimeric structure incorporating amide units as dual hydrogen-bond donors and acceptors to enable the formation of hydrogen-bonding networks within the molecules and with transparent conductive oxide. This design promotes homogeneous molecular arrangement and well-aligned energy levels, minimizing hole-transport loss and enhancing interfacial stability. We achieve an efficiency of 21.56% in a 1.77 eV PSC, with an open-circuit voltage of 1.35 V and a fill factor of 85.76%. This strategy is also applicable to 1.56 eV PSCs, affording efficiencies of 26.80% (certified 26.57% by current density–voltage (<i>J</i>–<i>V</i>) scan and 25.92% steady-state measured over 300 s). Most notably, the integrated all-perovskite tandem solar cell yields an efficiency of 30.19% (certified 29.38% by <i>J</i>–<i>V</i> scan and 28.40% steady state measured over 120 s).</p>

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Self-assembled molecules with hydrogen-bond networks enable efficient all-perovskite tandem solar cells

  • Deng Wang,
  • Zhixin Liu,
  • Zhi-Wen Gao,
  • Xia Lei,
  • Peide Zhu,
  • Jie Zeng,
  • Qian Li,
  • Lida Wang,
  • Zhen Zhang,
  • Meng Gu,
  • Siru He,
  • Yuqi Bao,
  • Qing Lian,
  • Jingbai Li,
  • Zonglong Song,
  • Yintai Xu,
  • Dangyuan Lei,
  • Xingzhu Wang,
  • Alex K.-Y. Jen,
  • Baomin Xu

摘要

Hole-selective self-assembled monolayers have advanced the performance of perovskite solar cells (PSCs), yet their excessive intermolecular interactions result in undesirable self-aggregation and weak interfacial contact. Here we devise a bicarbazole-based dimeric structure incorporating amide units as dual hydrogen-bond donors and acceptors to enable the formation of hydrogen-bonding networks within the molecules and with transparent conductive oxide. This design promotes homogeneous molecular arrangement and well-aligned energy levels, minimizing hole-transport loss and enhancing interfacial stability. We achieve an efficiency of 21.56% in a 1.77 eV PSC, with an open-circuit voltage of 1.35 V and a fill factor of 85.76%. This strategy is also applicable to 1.56 eV PSCs, affording efficiencies of 26.80% (certified 26.57% by current density–voltage (JV) scan and 25.92% steady-state measured over 300 s). Most notably, the integrated all-perovskite tandem solar cell yields an efficiency of 30.19% (certified 29.38% by JV scan and 28.40% steady state measured over 120 s).