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How the Microstructure of MAPbI3 Powder Impacts Pressure-Induced Compaction and Optoelectronic Thick-Film Properties

  • Christina Witt
    Christina Witt
    Soft Matter Optoelectronics, University of Bayreuth, Bayreuth 95440, Germany
  • Nico Leupold
    Nico Leupold
    Department of Functional Materials, University of Bayreuth, Bayreuth 95440, Germany
    More by Nico Leupold
  • Philipp Ramming
    Philipp Ramming
    Soft Matter Optoelectronics, University of Bayreuth, Bayreuth 95440, Germany
  • Konstantin Schötz
    Konstantin Schötz
    Soft Matter Optoelectronics, University of Bayreuth, Bayreuth 95440, Germany
  • Ralf Moos
    Ralf Moos
    Department of Functional Materials, University of Bayreuth, Bayreuth 95440, Germany
    More by Ralf Moos
  • , and 
  • Fabian Panzer*
    Fabian Panzer
    Soft Matter Optoelectronics, University of Bayreuth, Bayreuth 95440, Germany
    *Email: [email protected]
Cite this: J. Phys. Chem. C 2022, 126, 36, 15424–15435
Publication Date (Web):September 1, 2022
https://doi.org/10.1021/acs.jpcc.2c03329
Copyright © 2022 The Authors. Published by American Chemical Society

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    Abstract

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    Within the last few years, applying pressure to improve and alter the structural and optoelectronic properties of halide perovskite thin films and powder-based thick-film pellets has emerged as a promising processing method. However, a detailed understanding of the relationship between perovskite microstructure, pressing process, and final film properties is still missing. Here, we investigate the impact of powder microstructure on the compaction processes during pressure treatment and on the final properties of powder-pressed thick films, using the model halide perovskite methylammonium lead iodide (MAPbI3). Analyzing pressure relaxations together with XRD and SEM characterizations, we find that larger powder particles result in less compact thick films with higher surface roughness. Furthermore, larger particles exhibit stronger sintered connections between individual powder particles, resulting in less crushing and particle rearrangement but in more pronounced plastic deformation during pressure treatment. Moreover, plastic deformation of the powder particles leads to a reduction of crystallite size in the final film. This reduction results in increased nonradiative, defect-associated excited state recombination, as confirmed by photoluminescence investigations. More plastic deformation also deteriorates the grain boundary quality and consequently facilitates ion migration, which is reflected in higher electrical dark conductivities of the thick films. Thus, our work elucidates how important the design of the perovskite powder microstructure is for the pressure-induced compaction behavior and for the resulting structural, optical, and electrical thick-film properties. These insights will pave the way for tailored pressure processing of halide perovskite films with improved optoelectronic properties.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpcc.2c03329.

    • Details on MAI and PbI2 precursor preparation and mechanochemical synthesis of MAPbI3 powders, including SEM images; details on pellet pressing; additional analyses of the pressure relaxations, including detailed analyses of the amplitude ratio; supplementary XRD patterns of powders and pellets; details concerning relative densities and surface roughness with values of the 100 MPa pellets; and details on optoelectronic measurements, including additional analyses of the time-resolved PL curves, extraction of Urbach energy, and an exemplary impedance spectrum with an equivalent circuit for corresponding fits (PDF)

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    Cited By

    This article is cited by 2 publications.

    1. Yihui Cai, Dominique Begin, Charles Sidhoum, Adrien Girault, Thomas Fix, Christophe Lefevre, Wissal Belayachi, Aziz Dinia, Daniele Preziosi, Mathieu Gallart, Pierre Gilliot, Eric Gros-Daillon, Ferdinand Ledee, Ovidiu Ersen, Clément Sanchez, Sylvie Begin-Colin. Mechanosynthesis of MAPbI3@Graphite Composites with Active Interfaces and Promising Photodetection Properties. Chemistry of Materials 2023, 35 (23) , 10188-10205. https://doi.org/10.1021/acs.chemmater.3c02418
    2. Christina Witt, Konstantin Schötz, Meike Kuhn, Nico Leupold, Simon Biberger, Philipp Ramming, Frank-Julian Kahle, Anna Köhler, Ralf Moos, Eva M. Herzig, Fabian Panzer. Orientation and Grain Size in MAPbI3 Thin Films: Influence on Phase Transition, Disorder, and Defects. The Journal of Physical Chemistry C 2023, 127 (22) , 10563-10573. https://doi.org/10.1021/acs.jpcc.2c08968

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