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Disentangling Electronic Transport and Hysteresis at Individual Grain Boundaries in Hybrid Perovskites via Automated Scanning Probe Microscopy

Cite this: ACS Nano 2023, 17, 10, 9647–9657
Publication Date (Web):May 8, 2023
https://doi.org/10.1021/acsnano.3c03363
Copyright © 2023 American Chemical Society

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    Abstract

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    Underlying the rapidly increasing photovoltaic efficiency and stability of metal halide perovskites (MHPs) is the advancement in the understanding of the microstructure of polycrystalline MHP thin film. Over the past decade, intense efforts have been aimed at understanding the effect of microstructures on MHP properties, including chemical heterogeneity, strain disorder, phase impurity, etc. It has been found that grain and grain boundary (GB) are tightly related to lots of microscale and nanoscale behavior in MHP thin films. Atomic force microscopy (AFM) is widely used to observe grain and boundary structures in topography and subsequently to study the correlative surface potential and conductivity of these structures. For now, most AFM measurements have been performed in imaging mode to study the static behavior; in contrast, AFM spectroscopy mode allows us to investigate the dynamic behavior of materials, e.g., conductivity under sweeping voltage. However, a major limitation of AFM spectroscopy measurements is that they require manual operation by human operators, and as such only limited data can be obtained, hindering systematic investigations of these microstructures. In this work, we designed a workflow combining the conductive AFM measurement with a machine learning (ML) algorithm to systematically investigate grain boundaries in MHPs. The trained ML model can extract GBs locations from the topography image, and the workflow drives the AFM probe to each GB location to perform a current–voltage (IV) curve automatically. Then, we are able to have IV curves at all GB locations, allowing us to systematically understand the property of GBs. Using this method, we discovered that the GB junction points are less conductive, potentially more photoactive, and can play critical roles in MHP stability, while most previous works only focused on the difference between GB and grains.

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    • NMF analysis of CL results (PDF)

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    Cited By

    This article is cited by 2 publications.

    1. Liu Yang, Fei Zheng, Xu Wang, Like Huang, Xiaohui Liu, Jing Zhang, Yuejin Zhu, Ziyang Hu. Influence of A-Site Composition on the Nanostructure and Electrical Properties of APbI3 Perovskite Films: Implications for Solar Cells. ACS Applied Nano Materials 2023, 6 (20) , 19443-19451. https://doi.org/10.1021/acsanm.3c04100
    2. Holland Hysmith, So Yeon Park, Jonghee Yang, Anton V. Ievlev, Yongtao Liu, Kai Zhu, Bobby G. Sumpter, Joseph Berry, Mahshid Ahmadi, Olga S. Ovchinnikova. The Role of SnO2 Processing on Ionic Distribution in Double-Cation–Double Halide Perovskites. ACS Applied Materials & Interfaces 2023, 15 (30) , 36856-36865. https://doi.org/10.1021/acsami.3c03520

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