Controlling Solvate Intermediate Growth for Phase-Pure Organic Lead Iodide Ruddlesden–Popper (C4H9NH3)2(CH3NH3)n-1PbnI3n+1 Perovskite Thin Films

Dahlman, Clayton J.; DeCrescent, Ryan A.; Venkatesan, Naveen R.; Kennard, Rhys M.; Wu, Guang; Everest, Michael A.; Schuller, Jon A.; Chabinyc, Michael L.

doi:10.1021/acs.chemmater.9b01952

Title: Controlling Solvate Intermediate Growth for Phase-Pure Organic Lead Iodide Ruddlesden–Popper (C₄H₉NH₃)₂(CH₃NH₃)_n-1Pb_nI_3n+1 Perovskite Thin Films

Journal Article · Tue Jul 23 00:00:00 EDT 2019 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.9b01952· OSTI ID:1594806

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^[1]; Kennard, Rhys M. ^[1]; Wu, Guang ^[1]; Everest, Michael A. ^[2];

^[1];

^[1]

Univ. of California, Santa Barbara, CA (United States)
Westmont College, Santa Barbara, CA (United States)

The growth of Ruddlesden-Popper perovskite thin films is complicated by the existence of multiple crystallization pathways available to precursors in solution. During conventional thin film growth processes, such as spin-coating or blade-coating, solvents can evaporate too quickly to clearly resolve different reaction intermediates and products that form during crystallization. Here, we resolve multiple reaction products and intermediates that form during Ruddlesden-Popper phase growth by studying drop-cast precursor solutions in situ through the evolution of X-ray diffraction, photoluminescence, and optical micrographs over long timescales in a thin film geometry. We found that methylammonium-rich solvate intermediates play a crucial role in directing the bulk optical properties of the films, and form simultaneously with smaller regions of Ruddlesden-Popper phases during growth. The microstructure and optical properties of these sub-phases were characterized during growth and after annealing, revealing that discrepancies between thin film and single-crystal optical properties originate from solvate intermediates. These lower band-gap solvate-mediated minority phases dominate the optical emission spectrum by means of rapid energy migration, and contribute to sub-band-gap electronic states in photovoltaic devices. Processing routes to yield thin films with optical properties similar to single crystals of Ruddlesden-Popper phases were developed by tuning the precursor stoichiometry and deposition kinetics.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Quantum Materials for Energy Efficient Neuromorphic Computing (Q-MEEN-C); Univ. of California, Santa Barbara, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012541; SC0019273; AC02-76SF00515; AC0205CH11231

OSTI ID:: 1594806

Journal Information:: Chemistry of Materials, Vol. 31, Issue 15; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 32 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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CCDC 1950235: Experimental Crystal Structure Determination J., Dahlman, Clayton; A., DeCrescent, Ryan; R., Venkatesan, Naveen https://doi.org/10.5517/ccdc.csd.cc23gcts The current record is supplemented by this dataset	dataset	January 2019
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Title: Controlling Solvate Intermediate Growth for Phase-Pure Organic Lead Iodide Ruddlesden–Popper (C4H9NH3)2(CH3NH3)n-1PbnI3n+1 Perovskite Thin Films

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