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钙钛矿纳米晶体薄膜中长程激子扩散的起源:光子回收与激子跳跃

Origins of the long-range exciton diffusion in perovskite nanocrystal films: photon recycling vs exciton hopping.

作者信息

Giovanni David, Righetto Marcello, Zhang Qiannan, Lim Jia Wei Melvin, Ramesh Sankaran, Sum Tze Chien

机构信息

Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University (NTU), 21 Nanyang Link, Singapore, 637371, Singapore.

Energy Research Institute @NTU (ERI@N), Interdisciplinary Graduate School, Nanyang Technological University, 50 Nanyang Avenue, S2-B3a-01, Singapore, 639798, Singapore.

出版信息

Light Sci Appl. 2021 Jan 1;10(1):2. doi: 10.1038/s41377-020-00443-z.

Abstract

The outstanding optoelectronic performance of lead halide perovskites lies in their exceptional carrier diffusion properties. As the perovskite material dimensionality is reduced to exploit the quantum confinement effects, the disruption to the perovskite lattice, often with insulating organic ligands, raises new questions on the charge diffusion properties. Herein, we report direct imaging of >1 μm exciton diffusion lengths in CHNHPbBr perovskite nanocrystal (PNC) films. Surprisingly, the resulting exciton mobilities in these PNC films can reach 10 ± 2 cm V s, which is counterintuitively several times higher than the carrier mobility in 3D perovskite films. We show that this ultralong exciton diffusion originates from both efficient inter-NC exciton hopping (via Förster energy transfer) and the photon recycling process with a smaller yet significant contribution. Importantly, our study not only sheds new light on the highly debated origins of the excellent exciton diffusion in PNC films but also highlights the potential of PNCs for optoelectronic applications.

摘要

卤化铅钙钛矿出色的光电性能源于其卓越的载流子扩散特性。随着钙钛矿材料维度降低以利用量子限域效应,通常借助绝缘有机配体对钙钛矿晶格造成的破坏,引发了关于电荷扩散特性的新问题。在此,我们报道了在CHNHPbBr钙钛矿纳米晶体(PNC)薄膜中激子扩散长度大于1μm的直接成像。令人惊讶的是,这些PNC薄膜中产生的激子迁移率可达10±2 cm² V⁻¹ s⁻¹,这与直觉相反,比三维钙钛矿薄膜中的载流子迁移率高出几倍。我们表明,这种超长激子扩散源于高效的纳米晶体间激子跳跃(通过Förster能量转移)以及贡献较小但仍很显著的光子回收过程。重要的是,我们的研究不仅为PNC薄膜中出色激子扩散这一备受争议的起源提供了新见解,还突出了PNC在光电应用方面的潜力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e1d6/7775951/fdb9c7f741e7/41377_2020_443_Fig1_HTML.jpg

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