Phase Intergrowth and Structural Defects in Organic Metal Halide Ruddlesden–Popper Thin Films

Venkatesan, Naveen R.; Kennard, Rhys M.; DeCrescent, Ryan A.; Nakayama, Hidenori; Dahlman, Clayton J.; Perry, Erin E.; Schuller, Jon A.; Chabinyc, Michael L.

doi:10.1021/acs.chemmater.8b03832

Title: Phase Intergrowth and Structural Defects in Organic Metal Halide Ruddlesden–Popper Thin Films

Journal Article · 26 November 2018 · Chemistry of Materials

DOI: https://doi.org/10.1021/acs.chemmater.8b03832 · OSTI ID:1594808

^[1]; Kennard, Rhys M. ^[2]; DeCrescent, Ryan A. ^[2]; Nakayama, Hidenori ^[3];

^[2]; Perry, Erin E. ^[2];

^[2];

^[2]

Univ. of California, Santa Barbara, CA (United States); University of California, Santa Barbara
Univ. of California, Santa Barbara, CA (United States)
Mitsubishi Chemical Corporation (Japan). Electronics Materials and New Energy Lab.; Univ. of California, Santa Barbara, CA (United States)

Organic metal halide Ruddlesden–Popper phases combine the excellent optoelectronic properties of three-dimensional, bulk hybrid perovskites with superior material stability in ambient conditions. However, the thin film structure of these layered perovskites is still poorly understood, as phase purity is typically determined solely by specular X-ray diffraction. The thin film structure of these Ruddlesden–Popper phases was examined by increasingly local characterization techniques. It is difficult to assess the phase purity by purely bulk optical and diffraction measurements. From the comparison of grazing-incidence wide angle X-ray scattering (GIWAXS) patterns of cast films to expected scattering from single-crystal structures, significant in-plane disorder was observed. Spatially localized photoluminescence measurements show that films do not phase separate on the micrometer-scale. Selected area electron diffraction measurements show the intergrowth of different phases within the same thin film, consistent with previous observations seen in epitaxially-grown Ruddlesden–Popper complex oxides. Despite the presence of phase impurities that would typically be detrimental for device performance, fits to photothermal deflection spectroscopy measurements show relatively low Urbach energies of 33 meV for (C₄H₉NH₃)₂(CH₃NH₃)₂Pb₃I₁₀ and 32 meV for (C₄H₉NH₃)₂(CH₃NH₃)₃Pb₄I₁₃, indicating that the electronic properties are insensitive to the phase impurities.

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Research Organization:: Univ. of California, Santa Barbara, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-76SF00515; SC0012541

OSTI ID:: 1594808

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 23 Vol. 30; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Two‐Dimensional Halide Perovskites in Solar Cells: 2D or not 2D? Ortiz‐Cervantes, Carmen; Carmona‐Monroy, Paulina; Solis‐Ibarra, Diego ChemSusChem, Vol. 12, Issue 8 https://doi.org/10.1002/cssc.201802992	journal	March 2019
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Bright magnetic dipole radiation from two-dimensional lead-halide perovskites DeCrescent, Ryan A.; Venkatesan, Naveen R.; Dahlman, Clayton J. Science Advances, Vol. 6, Issue 6 https://doi.org/10.1126/sciadv.aay4900	journal	February 2020
Bright magnetic dipole radiation from two-dimensional lead-halide perovskites DeCrescent, Ryan A.; Venkatesan, Naveen R.; Dahlman, Clayton J. arXiv https://doi.org/10.48550/arxiv.1901.05136	preprint	January 2019

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