Local A-Site Phase Segregation Leads to Cs-Rich Regions Showing Accelerated Photodegradation in Mixed-Cation Perovskite Semiconductor Films

Huang, Zixu; Jiang, Fangyuan; Song, Zhaoning; Dolia, Kshitiz; Zhu, Tao; Yan, Yanfa; Ginger, David S.

doi:10.1021/acsenergylett.4c00960

Local A-Site Phase Segregation Leads to Cs-Rich Regions Showing Accelerated Photodegradation in Mixed-Cation Perovskite Semiconductor Films

Journal Article · Fri May 31 00:00:00 EDT 2024 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.4c00960· OSTI ID:2475135

^[1]; Jiang, Fangyuan ^[1]; ^[2]; Dolia, Kshitiz ^[2]; Zhu, Tao ^[2]; ^[2]; ^[3]

University of Washington, Seattle, WA (United States)
University of Toledo, OH (United States)
University of Washington, Seattle, WA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

We use hyperspectral photoluminescence microscopy to study compositional heterogeneity and its influence on the stability of mixed-cation (formamindinium (FA) and cesium) FA_1-xCs_xPb(I_0.9Br_0.1)₃ lead halide perovskites with different Cs contents. We observe substantial microscale heterogeneity in the photoluminescence. By correlating photoluminescence maps with time-of-flight secondary ion mass spectrometry (ToF-SIMS) imaging, we show that the redder-photoluminescence regions of the perovskite film are associated with Cs-rich compositions. X-ray diffraction measurement and confocal Raman spectroscopy provide evidence for the presence of d-phase CsPbI_xBr_3-x in these regions. Photo-aging tests show that these Cs-rich clusters undergo faster photoluminescence decay than the rest of the film. These observations highlight the importance of local heterogeneities and their influence on the stability of halide perovskite semiconductors being studied for optoelectronics.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: National Science Foundation (NSF); Office of Naval Research (ONR); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office

Grant/Contract Number:: AC05-76RL01830; EE0009528

OSTI ID:: 2475135

Report Number(s):: PNNL-SA--196938

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 6 Vol. 9; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Local A-Site Phase Segregation Leads to Cs-Rich Regions Showing Accelerated Photodegradation in Mixed-Cation Perovskite Semiconductor Films

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