Mapping Surface‐Defect and Ions Migration in Mixed‐Cation Perovskite Crystals

Author:

Nughays Razan O.1,Almasabi Khulud23,Nematulloev Sarvarkhodzha1,Wang Lijie1,Bian Tieyuan4,Nadinov Issatay1,Irziqat Bahaaeddin5,Harrison George T15,Fatayer Shadi5,Yin Jun4,Bakr Osman M.23,Mohammed Omar F.12ORCID

Affiliation:

1. Advanced Membranes and Porous Materials Center (AMPM) Division of Physical Science and Engineering King Abdullah University of Science and Technology Thuwal 23955‐6900 Kingdom of Saudi Arabia

2. KAUST Catalysis Center Division of Physical Sciences and Engineering King Abdullah University of Science and Technology Thuwal 23955‐6900 Kingdom of Saudi Arabia

3. Functional Nanomaterials Lab Division of Physical Sciences and Engineering King Abdullah University of Science and Technology Thuwal 23955‐6900 Kingdom of Saudi Arabia

4. Department of Applied Physics The Hong Kong Polytechnic University Kowloon Hong Kong 999077 P. R. China

5. KAUST Solar Center (KSC) Division of Physical Science and Engineering King Abdullah University of Science and Technology Thuwal 23955‐6900 Kingdom of Saudi Arabia

Abstract

AbstractSingle crystal perovskites have garnered significant attention as potential replacements for existing absorber layer materials. Despite the extensive investigations on their photoinduced charge‐carriers dynamics, most of the time‐resolved techniques focus on bulk properties, neglecting surface characteristic which plays a crucial role for their optoelectronic performance. Herein, 4D ultrafast scanning electron microscopy (4D‐USEM) is utilized to probing the photogenerated carrier transport at the first few nanometers, alongside density functional theory (DFT) to track both defect centers and ions migration. Two compositions of mixed cation are investigated: FA0.6MA0.4PbI3 and FA0.4MA0.6PbI3, interestingly, the former displays a longer lifetime compared to the latter due the presence of a higher surface‐defect centers. DFT calculations fully support that revealing samples with higher FA content have a lower energy barrier for iodide ions to migrate from the bulk to top layer, assisting in passivating surface vacancies, and a higher energy diffusion barrier to escape from surface to vacuum, resulting in fewer vacancies and longer‐lived hole–electron pairs. These findings manifest the influence of cation selection on charge carrier transport and formation of defects, and emphasize the importance of understanding ion migrations role in controlling surface vacancies to assist engineering high‐performance optoelectronic devices based on single crystal perovskites.

Funder

Hong Kong Polytechnic University

Global Collaborative Research, King Abdullah University of Science and Technology

Publisher

Wiley

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