<p>The performance of three-dimensional (3D) perovskite solar cells (PSCs) is predominantly limited by interfacial non-radiative recombination and instability. Although low-dimensional (LD) interlayers, particularly two-dimensional (2D) perovskites, are widely adopted for surface passivation, their heterogeneous n-values and quantum-well confinement often impede charge transport. One-dimensional (1D) perovskites offer a promising alternative due to their structural flexibility and superior passivation capabilities, yet their potential has been underexploited by challenges in controlled crystallization and ordered orientation. Here, we constructed a 3D/PDAI<sub>2</sub>/1D heterojunction through sequential deposition of propane-1,3-diammonium iodide (PDAI<sub>2</sub>) and 4-amidinopyridinium chloride (4APyCl). The pre-anchored PDAI<sub>2</sub> not only provides field-effect passivation but also templates the subsequent vertical alignment of 1D Pb–I chains assembled with 4APyCl. This configuration establishes continuous out-of-plane charge transport channels, enabling effective surface defect passivation, favorable energy-level alignment, and enhanced interfacial carrier extraction. The resulting inverted PSCs achieved a champion power conversion efficiency of 25.8% and retained 85% of the initial performance after 1000&#xa0;h of maximum power point tracking under 1-sun illumination. By demonstrating the critical role of molecular orchestration in LD interlayers, this work provides a blueprint for establishing structure–property relationships and guides the rational design of stable and efficient 3D/1D perovskite photovoltaics.</p>

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Diamine-Mediated Synergistic Engineering of Orientation and Interfacial Field of 3D/1D Heterojunctions for Efficient Perovskite Photovoltaics

  • Yaobin Li,
  • Yunxuan Cao,
  • Yu Zou,
  • Wenjin Yu,
  • Zhenhuang Su,
  • Zhuoer Cai,
  • Yueli Liu,
  • Qinyun Liu,
  • Hantao Wang,
  • Lefan Gong,
  • Yucheng Ye,
  • Rong Tang,
  • Yunan Gao,
  • Felix Thomas Eickemeyer,
  • Bo Qu,
  • Lixin Xiao,
  • Zhijian Chen

摘要

The performance of three-dimensional (3D) perovskite solar cells (PSCs) is predominantly limited by interfacial non-radiative recombination and instability. Although low-dimensional (LD) interlayers, particularly two-dimensional (2D) perovskites, are widely adopted for surface passivation, their heterogeneous n-values and quantum-well confinement often impede charge transport. One-dimensional (1D) perovskites offer a promising alternative due to their structural flexibility and superior passivation capabilities, yet their potential has been underexploited by challenges in controlled crystallization and ordered orientation. Here, we constructed a 3D/PDAI2/1D heterojunction through sequential deposition of propane-1,3-diammonium iodide (PDAI2) and 4-amidinopyridinium chloride (4APyCl). The pre-anchored PDAI2 not only provides field-effect passivation but also templates the subsequent vertical alignment of 1D Pb–I chains assembled with 4APyCl. This configuration establishes continuous out-of-plane charge transport channels, enabling effective surface defect passivation, favorable energy-level alignment, and enhanced interfacial carrier extraction. The resulting inverted PSCs achieved a champion power conversion efficiency of 25.8% and retained 85% of the initial performance after 1000 h of maximum power point tracking under 1-sun illumination. By demonstrating the critical role of molecular orchestration in LD interlayers, this work provides a blueprint for establishing structure–property relationships and guides the rational design of stable and efficient 3D/1D perovskite photovoltaics.