Boosting exciton mobility approaching Mott-Ioffe-Regel limit in Ruddlesden−Popper perovskites by anchoring the organic cation

Yiyang Gong, Shuai Yue, Yin Liang, Wenna Du, Tieyuan Bian, Chuanxiu Jiang, Xiaotian Bao, Shuai Zhang, Mingzhu Long, Guofu Zhou, Jun Yin, Shibin Deng, Qing Zhang (), Bo Wu () and Xinfeng Liu ()
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Yiyang Gong: South China Normal University
Shuai Yue: CAS Key Laboratory of Standardization and Measurement for Nanotechnology, National Center for Nanoscience and Technology
Yin Liang: Peking University
Wenna Du: CAS Key Laboratory of Standardization and Measurement for Nanotechnology, National Center for Nanoscience and Technology
Tieyuan Bian: The Hong Kong Polytechnic University, Hung Hom
Chuanxiu Jiang: CAS Key Laboratory of Standardization and Measurement for Nanotechnology, National Center for Nanoscience and Technology
Xiaotian Bao: CAS Key Laboratory of Standardization and Measurement for Nanotechnology, National Center for Nanoscience and Technology
Shuai Zhang: CAS Key Laboratory of Standardization and Measurement for Nanotechnology, National Center for Nanoscience and Technology
Mingzhu Long: South China Normal University
Guofu Zhou: South China Normal University
Jun Yin: The Hong Kong Polytechnic University, Hung Hom
Shibin Deng: Nankai University
Qing Zhang: Peking University
Bo Wu: South China Normal University
Xinfeng Liu: CAS Key Laboratory of Standardization and Measurement for Nanotechnology, National Center for Nanoscience and Technology

Nature Communications, 2024, vol. 15, issue 1, 1-8

Abstract: Abstract Exciton transport in two-dimensional Ruddlesden−Popper perovskite plays a pivotal role for their optoelectronic performance. However, a clear photophysical picture of exciton transport is still lacking due to strong confinement effects and intricate exciton-phonon interactions in an organic-inorganic hybrid lattice. Herein, we present a systematical study on exciton transport in (BA)2(MA)n−1PbnI3n+1 Ruddlesden−Popper perovskites using time-resolved photoluminescence microscopy. We reveal that the free exciton mobilities in exfoliated thin flakes can be improved from around 8 cm2 V−1 s−1 to 280 cm2V−1s−1 by anchoring the soft butyl ammonium cation with a polymethyl methacrylate network at the surface. The mobility of the latter is close to the theoretical limit of Mott-Ioffe-Regel criterion. Combining optical measurements and theoretical studies, it is unveiled that the polymethyl methacrylate network significantly improve the lattice rigidity resulting in the decrease of deformation potential scattering and lattice fluctuation at the surface few layers. Our work elucidates the origin of high exciton mobility in Ruddlesden−Popper perovskites and opens up avenues to regulate exciton transport in two-dimensional materials.

Date: 2024
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DOI: 10.1038/s41467-024-45740-y

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