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

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 () and Michael Grätzel ()
Additional contact information
Minhuan Wang: Dalian University of Technology
Yanfeng Yin: Chinese Academy of Sciences
Pengfei Wang: Dalian University of Technology
Wenzhe Shang: Dalian University of Technology
Yaling Han: Dalian University of Technology
Jing Gao: Ecole Polytechnique Federale de Lausanne (EPFL)
Kangshuo Hui: Dalian University of Technology
Tao Feng: Dalian University of Technology
Ummugulsum Gunes: Ecole Polytechnique Federale de Lausanne (EPFL)
Tristan Georges: Ecole Polytechnique Federale de Lausanne (EPFL)
Lyndon Emsley: Ecole Polytechnique Federale de Lausanne (EPFL)
Peng Xu: Chinese Academy of Sciences
Jiming Bian: Dalian University of Technology
Jing Cao: Lanzhou University
Zhehan Ying: The Hong Kong University of Science and Technology (Guangzhou)
Rui Cai: Dalian University of Technology
Jingyi Xiao: Dalian University of Technology
Shengye Jin: Chinese Academy of Sciences
Xiaoqing Jiang: Ecole Polytechnique Federale de Lausanne (EPFL)
Shaik M. Zakeeruddin: Ecole Polytechnique Federale de Lausanne (EPFL)
Wenming Tian: Chinese Academy of Sciences
Likai Zheng: Ecole Polytechnique Federale de Lausanne (EPFL)
Yantao Shi: Dalian University of Technology
Michael Grätzel: Ecole Polytechnique Federale de Lausanne (EPFL)

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: Abstract 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).

Date: 2025
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DOI: 10.1038/s41467-025-63777-5

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