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ACS Publications. Most Trusted. Most Cited. Most Read
Cesium-Incorporated Triple Cation Perovskites Deliver Fully Reversible and Stable Nanoscale Voltage Response
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    Cesium-Incorporated Triple Cation Perovskites Deliver Fully Reversible and Stable Nanoscale Voltage Response
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    • Elizabeth M. Tennyson
      Elizabeth M. Tennyson
      Department of Materials Science and Engineering, University of Maryland, College Park, Maryland 20742, United States
      Institute for Research in Electronics and Applied Physics, University of Maryland, College Park, Maryland 20742, United States
    • Bart Roose
      Bart Roose
      Cavendish Laboratory, Department of Physics, University of Cambridge, JJ Thomson Avenue, CB3 0HE Cambridge, United Kingdom
      More by Bart Roose
    • Joseph L. Garrett
      Joseph L. Garrett
      Institute for Research in Electronics and Applied Physics, University of Maryland, College Park, Maryland 20742, United States
      Department of Physics, University of Maryland, College Park, Maryland 20742, United States
    • Chen Gong
      Chen Gong
      Department of Materials Science and Engineering, University of Maryland, College Park, Maryland 20742, United States
      Institute for Research in Electronics and Applied Physics, University of Maryland, College Park, Maryland 20742, United States
      More by Chen Gong
    • Jeremy N. Munday
      Jeremy N. Munday
      Institute for Research in Electronics and Applied Physics, University of Maryland, College Park, Maryland 20742, United States
      Department of Electrical and Computer Engineering, University of Maryland, College Park, Maryland 20742, United States
    • Antonio Abate
      Antonio Abate
      Helmholtz-Zentrum Berlin für Materialien und Energie, Kekuléstraße 5, 12489 Berlin, Germany
      Department of Chemical, Materials and Production Engineering, University of Naples Federico II, Piazzale Tecchio 80, 80125 Fuorigrotta, Naples, Italy
    • Marina S. Leite*
      Marina S. Leite
      Department of Materials Science and Engineering, University of Maryland, College Park, Maryland 20742, United States
      Institute for Research in Electronics and Applied Physics, University of Maryland, College Park, Maryland 20742, United States
      *E-mail: [email protected]
    Other Access OptionsSupporting Information (1)

    ACS Nano

    Cite this: ACS Nano 2019, 13, 2, 1538–1546
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    https://doi.org/10.1021/acsnano.8b07295
    Published December 26, 2018
    Copyright © 2018 American Chemical Society

    Abstract

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    Perovskite solar cells that incorporate small concentrations of Cs in their A-site have shown increased lifetime and improved device performance. Yet, the development of fully stable devices operating near the theoretical limit requires understanding how Cs influences perovskites’ electrical properties at the nanoscale. Here, we determine how the chemical composition of three perovskites (MAPbBr3, MAPbI3, and Cs-mixed) affects their short- and long-term voltage stabilities, with <50 nm spatial resolution. We map an anomalous irreversible electrical signature on MAPbBr3 at the mesoscale, resulting in local Voc variations of ∼400 mV, and in entire grains with negative contribution to the Voc. These measurements prove the necessity of high spatial resolution mapping to elucidate the fundamental limitations of this emerging material. Conversely, we capture the fully reversible voltage response of Cs-mixed perovskites, composed by Cs0.06(MA0.17FA0.83)0.94Pb(I0.83Br0.17)3, demonstrating that the desired electrical output persists even at the nanoscale. The Cs-mixed material presents no spatial variation in Voc, as ion motion is restricted. Our results show that the nanoscale electrical behavior of the perovskites is intimately connected to their chemical composition and macroscopic response.

    Copyright © 2018 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsnano.8b07295.

    • Additional TOF-SIMS depth profiles, map, and fast-KPFM scans on MAPbBr3. A plot of humidity level during KPFM experiment, light and dark KPFM results for the MAPbI3 perovskite film, and fast-KPFM results on the Cs-mixed sample (PDF)

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    Cited By

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    This article is cited by 11 publications.

    1. Vesselin Donchev, Davide Regaldo, Stefan Georgiev, Aleksandra Bojar, Mattia da Lisca, Kiril Kirilov, José Alvarez, Philip Schulz, Jean-Paul Kleider. Surface Photovoltage Study of Metal Halide Perovskites Deposited Directly on Crystalline Silicon. ACS Omega 2023, 8 (9) , 8125-8133. https://doi.org/10.1021/acsomega.2c07664
    2. Hao Zhang, Parinaz Moazzezi, Juanjuan Ren, Brett Henderson, Cristina Cordoba, Vishal Yeddu, Arthur M. Blackburn, Makhsud I. Saidaminov, Irina Paci, Stephen Hughes, Reuven Gordon. Coupling Perovskite Quantum Dot Pairs in Solution using a Nanoplasmonic Assembly. Nano Letters 2022, 22 (13) , 5287-5293. https://doi.org/10.1021/acs.nanolett.2c01222
    3. Kaiyu Wang, Qing Yao, Jie Zhang, Chenyu Shang, Changqian Li, Feitong Chen, Tianliang Zhou, Haiqing Sun, Weiwei Zhang, Huiling Zhu, Jianxu Ding. Short-Range Migration of A-Site Cations Inhibit Photoinduced Phase Segregation in FAxMAyCs1–x–yPbI3–zBrz Single Crystals. The Journal of Physical Chemistry C 2021, 125 (42) , 23050-23057. https://doi.org/10.1021/acs.jpcc.1c08346
    4. Manas Likhit Holekevi Chandrappa, Zhuoying Zhu, David P. Fenning, Shyue Ping Ong. Correlated Octahedral Rotation and Organic Cation Reorientation Assist Halide Ion Migration in Lead Halide Perovskites. Chemistry of Materials 2021, 33 (12) , 4672-4678. https://doi.org/10.1021/acs.chemmater.1c01175
    5. Elizabeth M. Tennyson, Kyle Frohna, William K. Drake, Florent Sahli, Terry Chien-Jen Yang, Fan Fu, Jérémie Werner, Cullen Chosy, Alan R. Bowman, Tiarnan A. S. Doherty, Quentin Jeangros, Christophe Ballif, Samuel D. Stranks. Multimodal Microscale Imaging of Textured Perovskite–Silicon Tandem Solar Cells. ACS Energy Letters 2021, 6 (6) , 2293-2304. https://doi.org/10.1021/acsenergylett.1c00568
    6. David Toth, Bekele Hailegnaw, Filipe Richheimer, Fernando A. Castro, Ferry Kienberger, Markus C. Scharber, Sebastian Wood, Georg Gramse. Nanoscale Charge Accumulation and Its Effect on Carrier Dynamics in Tri-cation Perovskite Structures. ACS Applied Materials & Interfaces 2020, 12 (42) , 48057-48066. https://doi.org/10.1021/acsami.0c10641
    7. Hailin Zhang, Haiyang Xu, Xu Ji, Jingkang Liang, Qiongfen Yu. Progress toward Applications of Perovskite Solar Cells. Energy & Fuels 2020, 34 (6) , 6624-6633. https://doi.org/10.1021/acs.energyfuels.0c00485
    8. Adnan Ali, Heesoo Park, Raghvendra Mall, Brahim Aïssa, Stefano Sanvito, Halima Bensmail, Abdelhak Belaidi, Fedwa El-Mellouhi. Machine Learning Accelerated Recovery of the Cubic Structure in Mixed-Cation Perovskite Thin Films. Chemistry of Materials 2020, 32 (7) , 2998-3006. https://doi.org/10.1021/acs.chemmater.9b05342
    9. Elizabeth M. Tennyson, John M. Howard, Bart Roose, Joseph L. Garrett, Jeremy N. Munday, Antonio Abate, Marina S. Leite. The Effects of Incident Photon Energy on the Time-Dependent Voltage Response of Lead Halide Perovskites. Chemistry of Materials 2019, 31 (21) , 8969-8976. https://doi.org/10.1021/acs.chemmater.9b03089
    10. Yanyan Wang, Ziyang Hu, Wenlong Yao, Cheng Yang, Houcheng Zhang, Jing Zhang, Yuejin Zhu. Heterogeneous photoresponse of individual grain in all-inorganic perovskite solar cells. Applied Physics Letters 2020, 117 (8) https://doi.org/10.1063/5.0014187
    11. Qi Dong, Lei Lei, Juliana Mendes, Franky So. Operational stability of perovskite light emitting diodes. Journal of Physics: Materials 2020, 3 (1) , 012002. https://doi.org/10.1088/2515-7639/ab60c4

    ACS Nano

    Cite this: ACS Nano 2019, 13, 2, 1538–1546
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.8b07295
    Published December 26, 2018
    Copyright © 2018 American Chemical Society

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