Film formation mechanisms in mixed-dimensional 2D/3D halide perovskite films revealed by in situ grazing-incidence wide-angle X-ray scattering

Creators: Hoffman, Justin M.; Hadar, Ido; Li, Xiaotong; Ke, Weijun; Vasileiadou, Eugenia S.; Strzalka, Joseph; Chen, Lin X.; Kanatzidis, Mercouri G.

Abstract

Mixed-dimensional 2D/3D hybrid halide perovskites retain the stability of 2D perovskites (formula (A′)2(A)₍ₙ₋₁₎PbₙI₍₃ₙ₊₁₎) and long diffusion lengths of the 3D materials (AMX₃), thereby affording devices with extended stability as well as state-of-the art efficiencies approaching those of the 3D materials. These films are made by spin-coating precursor solutions with an arbitrarily large average layer thickness n (⟨n⟩ > 7) to give films with both 2D and 3D phases. Although the 2D and 3D perovskite film formation mechanisms have been studied, little is understood about composite 2D/3D film formation. We used in-situ grazing-incidence wide-angle scattering with synchrotron radiation to characterize the films fabricated from precursor solutions with stoichiometries of (BA)₂(MA)₍ₙ₋₁₎PbₙI₍₃ₙ₊₁₎ (⟨n⟩ = 3, 4, 5, 7, 12, 50, and ∞ (MAPbI₃)). Four different mechanisms are seen depending on the stoichiometry in the precursor solution. Kinetic analysis shows faster and earlier growth of the solvate with increasing ⟨n⟩.

Additional Information

© 2022 Elsevier. Received 12 August 2021, Revised 6 November 2021, Accepted 28 December 2021, Available online 21 January 2022, Version of Record 14 April 2022. This work was supported by the Office of Naval Research (ONR) under grant no. N00014-20-1-2725. This project was supported in part by a fellowship award through the National Defense Science and Engineering Graduate (NDSEG) Fellowship Program, sponsored by the Air Force Research Laboratory (AFRL), the Office of Naval Research (ONR), and the Army Research Office (ARO). This research used resources of the Advanced Photon Source, a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by the Argonne National Laboratory under the contract no. DE-AC02-06CH113. L.X.C. is partially supported by the Solar Energy Photochemistry program of the US Department of Energy, Office of Science, Office of Basic Energy Sciences, through Argonne National Laboratory under contract no. DE-AC02-06CH11357. This work made use of the SPID facility of Northwestern University's NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (ShyNE) Resource (NSF ECCS-1542205), the MRSEC program (NSF DMR-1720139) at the Materials Research Center, the International Institute for Nanotechnology (IIN), the Keck Foundation, and the State of Illinois through the IIN. Author contributions. J.M.H., M.G.K., and L.X.C. conceived the idea and designed the study. J.M.H., I.H., W.K., X.L., and E.S.V. collected the data with the assistance of J.S. Then J.M.H. performed the analysis and interpretation of the data. J.M.H. and M.G.K. wrote the manuscript. All authors discussed the results and commented on the manuscript. Data and code availability. The code used in the analysis of this study is open-access and available at Zenodo: https://doi.org/10.5281/zenodo.5648076. Further information on the data and analysis will be provided by the authors upon request. For a full description of the experimental procedures including materials, data acquisition, and analysis, see the supplemental information. The authors declare no competing interests.

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