Small Cyclic Diammonium Cation Templated (110)-oriented 2D Halide (X = I, Br, Cl) Perovskites with White-light Emission - Archive ouverte HAL
Article Dans Une Revue Chemistry of Materials Année : 2019

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

Résumé

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-aminopyrrolidine (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). DFT 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. 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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Dates et versions

hal-02106354 , version 1 (01-09-2020)

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Xiaotong Li, Peijun Guo, Mikaël Kepenekian, Ido Hadar, Claudine Katan, et al.. Small Cyclic Diammonium Cation Templated (110)-oriented 2D Halide (X = I, Br, Cl) Perovskites with White-light Emission. Chemistry of Materials, 2019, 31 (9), pp.3582-3590. ⟨10.1021/acs.chemmater.9b01511⟩. ⟨hal-02106354⟩
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