Small Cyclic Diammonium Cation Templated (110)-Oriented 2D Halide (X = I, Br, Cl) Perovskites with White-Light Emission

Li, Xiaotong; Guo, Peijun; Kepenekian, Mikaël; Hadar, Ido; Katan, Claudine; Even, Jacky; Stoumpos, Constantinos C.; Schaller, Richard D.; Kanatzidis, Mercouri G.

doi:10.1021/acs.chemmater.9b01511

Title: Small Cyclic Diammonium Cation Templated (110)-Oriented 2D Halide (X = I, Br, Cl) Perovskites with White-Light Emission

Journal Article · Mon Apr 22 00:00:00 EDT 2019 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.9b01511· OSTI ID:1558606

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Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. Rennes, Rennes (France)
Univ. of Crete, Heraklion (Greece)
Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

Two-dimensional (2D) halide perovskites exhibit excellent potential for optoelectronics because of their outstanding physical properties and structural diversity. White-light emission is one property of 2D perovskites that originates from self-trapped excitons (STE) in the highly distorted structures. The so-called (110)-oriented 2D perovskites are generally distorted and believed to be good candidates for white-light emitting devices. Here, we report (110)-oriented 2D perovskites, C₄N₂H₁₂PbX₄ (X = I, Br, Cl), templated by the small cyclic diammonium cation, 3-aminopyrrolidinium (3APr). Structural characterization by single-crystal X-ray diffraction reveals that the distortion of the inorganic part of the structures is influenced by the stereochemical conformation of the cation between the perovskite layers. The experimental bandgaps follow the trend I < Br < Cl (2.56 eV, 3.29 eV, 3.85 eV, respectively). Density functional theory calculations reveal a weak but significant electronic band dispersion along the stacking axis, suggesting a non-negligible interlayer electronic coupling caused by the short proximity of adjacent inorganic layers. The high level of distortion results in the emergence of white-light emission, rarely seen in iodide perovskites, as well as the bromide and chloride isostructural analogues, which provides perfect platform to compare the broad emission mechanism for all three halides. The bromide and chloride perovskites show longer lifetimes and higher color rendering index (CRI) (83 and 85), relevant to solid-state lighting. Lastly, temperature-dependent PL measurements confirm that the broad emission comes from different STE mechanism for different halides, with the peak broadening persisting even at low temperature for the chloride compound.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: US Department of the Navy, Office of Naval Research (ONR); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1558606

Journal Information:: Chemistry of Materials, Vol. 31, Issue 9; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 75 works

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