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<p>Charge transport and extraction in polycrystalline perovskite films are often hindered by inefficient carrier transfer across grain domain boundaries (GDBs). Herein, we present a universal post-treatment strategy leveraging supramolecular crown ether-assisted slow release and precise delivery of Rb⁺ cations to GDBs, achieving in-situ GDB bridging. The solid-state nuclear magnetic resonance (NMR), transmission electron microscopic (TEM), and time-of-flight secondary ion mass spectrometry (ToF-SIMS) analyses confirm that Rb<sup>+</sup> forms a non-perovskite phase, primarily localized at the surface and GDBs. Ultrafast time-resolved photoluminescence mapping revealed accelerated carrier diffusion across the grain boundaries for the Rb<sup>+</sup>-treated perovskite thin films which enables photo-generated charge carriers to travels over two grain domain boundaries before recombination. As a result, perovskite solar cells treated with this strategy achieved a champion efficiency of 26.02% (certified as 25.77%) and demonstrated remarkable stability, retaining 99.2% of their initial efficiency after 1300 h of continuous one-sun illumination under maximum power point tracking (ISOS-L-1I).</p>

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In-situ boundary bridging unlocks multi-grain-domain carrier diffusion in polycrystalline metal halide perovskites

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年10月1日

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  • Minhuan Wang,
  • Yanfeng Yin,
  • Pengfei Wang,
  • Wenzhe Shang,
  • Yaling Han,
  • Jing Gao,
  • Kangshuo Hui,
  • Tao Feng,
  • Ummugulsum Gunes,
  • Tristan Georges,
  • Lyndon Emsley,
  • Peng Xu,
  • Jiming Bian,
  • Jing Cao,
  • Zhehan Ying,
  • Rui Cai,
  • Jingyi Xiao,
  • Shengye Jin,
  • Xiaoqing Jiang,
  • Shaik M. Zakeeruddin,
  • Wenming Tian,
  • Likai Zheng,
  • Yantao Shi,
  • Michael Grätzel

摘要

Charge transport and extraction in polycrystalline perovskite films are often hindered by inefficient carrier transfer across grain domain boundaries (GDBs). Herein, we present a universal post-treatment strategy leveraging supramolecular crown ether-assisted slow release and precise delivery of Rb⁺ cations to GDBs, achieving in-situ GDB bridging. The solid-state nuclear magnetic resonance (NMR), transmission electron microscopic (TEM), and time-of-flight secondary ion mass spectrometry (ToF-SIMS) analyses confirm that Rb+ forms a non-perovskite phase, primarily localized at the surface and GDBs. Ultrafast time-resolved photoluminescence mapping revealed accelerated carrier diffusion across the grain boundaries for the Rb+-treated perovskite thin films which enables photo-generated charge carriers to travels over two grain domain boundaries before recombination. As a result, perovskite solar cells treated with this strategy achieved a champion efficiency of 26.02% (certified as 25.77%) and demonstrated remarkable stability, retaining 99.2% of their initial efficiency after 1300 h of continuous one-sun illumination under maximum power point tracking (ISOS-L-1I).