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Multication perovskite 2D/3D interfaces form via progressive dimensional reduction

Author

Listed:
  • Andrew H. Proppe

    (University of Toronto
    University of Toronto)

  • Andrew Johnston

    (University of Toronto)

  • Sam Teale

    (University of Toronto)

  • Arup Mahata

    (D3-Computation, Istituto Italiano di Tecnologia
    Computational Laboratory for Hybrid/Organic Photovoltaics (CLHYO), Istituto CNR di Scienze e Tecnologie Chimiche (CNR-SCITEC), Istituto CNR di Scienze e Tecnologie Molecolari (ISTM-CNR))

  • Rafael Quintero-Bermudez

    (University of Toronto)

  • Eui Hyuk Jung

    (University of Toronto)

  • Luke Grater

    (University of Toronto)

  • Teng Cui

    (Department of Mechanical and Industrial Engineering)

  • Tobin Filleter

    (Department of Mechanical and Industrial Engineering)

  • Chang-Yong Kim

    (Canadian Light Source)

  • Shana O. Kelley

    (University of Toronto
    University of Toronto)

  • Filippo Angelis

    (D3-Computation, Istituto Italiano di Tecnologia
    Computational Laboratory for Hybrid/Organic Photovoltaics (CLHYO), Istituto CNR di Scienze e Tecnologie Chimiche (CNR-SCITEC), Istituto CNR di Scienze e Tecnologie Molecolari (ISTM-CNR)
    University of Perugia
    College of Science, King Saud University)

  • Edward H. Sargent

    (University of Toronto)

Abstract

Many of the best-performing perovskite photovoltaic devices make use of 2D/3D interfaces, which improve efficiency and stability – but it remains unclear how the conversion of 3D-to-2D perovskite occurs and how these interfaces are assembled. Here, we use in situ Grazing-Incidence Wide-Angle X-Ray Scattering to resolve 2D/3D interface formation during spin-coating. We observe progressive dimensional reduction from 3D to n = 3 → 2 → 1 when we expose (MAPbBr3)0.05(FAPbI3)0.95 perovskites to vinylbenzylammonium ligand cations. Density functional theory simulations suggest ligands incorporate sequentially into the 3D lattice, driven by phenyl ring stacking, progressively bisecting the 3D perovskite into lower-dimensional fragments to form stable interfaces. Slowing the 2D/3D transformation with higher concentrations of antisolvent yields thinner 2D layers formed conformally onto 3D grains, improving carrier extraction and device efficiency (20% 3D-only, 22% 2D/3D). Controlling this progressive dimensional reduction has potential to further improve the performance of 2D/3D perovskite photovoltaics.

Suggested Citation

  • Andrew H. Proppe & Andrew Johnston & Sam Teale & Arup Mahata & Rafael Quintero-Bermudez & Eui Hyuk Jung & Luke Grater & Teng Cui & Tobin Filleter & Chang-Yong Kim & Shana O. Kelley & Filippo Angelis &, 2021. "Multication perovskite 2D/3D interfaces form via progressive dimensional reduction," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-23616-9
    DOI: 10.1038/s41467-021-23616-9
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    Cited by:

    1. Bo Li & Qi Liu & Jianqiu Gong & Shuai Li & Chunlei Zhang & Danpeng Gao & Zhongwei Chen & Zhen Li & Xin Wu & Dan Zhao & Zexin Yu & Xintong Li & Yan Wang & Haipeng Lu & Xiao Cheng Zeng & Zonglong Zhu, 2024. "Harnessing strong aromatic conjugation in low-dimensional perovskite heterojunctions for high-performance photovoltaic devices," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    2. Xiaopeng Feng & Yuhong He & Wei Qu & Jinmei Song & Wanting Pan & Mingrui Tan & Bai Yang & Haotong Wei, 2022. "Spray-coated perovskite hemispherical photodetector featuring narrow-band and wide-angle imaging," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    3. Hyungsoo Lee & Chan Uk Lee & Juwon Yun & Chang-Seop Jeong & Wooyong Jeong & Jaehyun Son & Young Sun Park & Subin Moon & Soobin Lee & Jun Hwan Kim & Jooho Moon, 2024. "A dual spin-controlled chiral two-/three-dimensional perovskite artificial leaf for efficient overall photoelectrochemical water splitting," Nature Communications, Nature, vol. 15(1), pages 1-15, December.

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