Organic-inorganic hybrid metal halide perovskites, an emerging class of solution processable photoactive materials, welcome a new member with a one-dimensional structure. Herein we report the synthesis, crystal structure and photophysical properties of one-dimensional organic lead bromide perovskites, C4N2H14PbBr4, in which the edge sharing octahedral lead bromide chains [PbBr4 2−]∞ are surrounded by the organic cations C4N2H14 2+ to form the bulk assembly of core-shell quantum wires. This unique one-dimensional structure enables strong quantum confinement with the formation of self-trapped excited states that give efficient bluish white-light emissions with photoluminescence quantum efficiencies of approximately 20% for the bulk single crystals and 12% for the microscale crystals. This work verifies once again that one-dimensional systems are favourable for exciton self-trapping to produce highly efficient below-gap broadband luminescence, and opens up a new route towards superior light emitters based on bulk quantum materials.
Organometal halide
perovskites have recently emerged as a highly
promising class of functional materials for a variety of applications.
The exceptional structural tunability enables these materials to possess
three- (3D), two- (2D), one- (1D), and zero-dimensional (0D) structures
at the molecular level. Remarkable progress has been realized in the
research of perovskites in recent years, focusing mainly on 3D and
2D structures but leaving low-dimensional 1D and 0D structures significantly
underexplored. Here we offer our perspective on the most exciting
developments in the low-dimensional organometal halide perovskites.
Due to the strong quantum confinement and site isolation, 1D and 0D
perovskites exhibit remarkable and useful properties that are significantly
different from those of 3D and 2D perovskites. The excitement about
the recent developments lies not only in the specific achievements
but also in what these materials represent in terms of a new paradigm
in materials design.
The synthesis and characterization is reported of (C NH ) SnBr , a novel organic metal halide hybrid with a zero-dimensional (0D) structure, in which individual seesaw-shaped tin (II) bromide anions (SnBr ) are co-crystallized with 1-butyl-1-methylpyrrolidinium cations (C NH ). Upon photoexcitation, the bulk crystals exhibit a highly efficient broadband deep-red emission peaked at 695 nm, with a large Stokes shift of 332 nm and a high quantum efficiency of around 46 %. The unique photophysical properties of this hybrid material are attributed to two major factors: 1) the 0D structure allowing the bulk crystals to exhibit the intrinsic properties of individual SnBr species, and 2) the seesaw structure enabling a pronounced excited state structural deformation as confirmed by density functional theory (DFT) calculations.
Organic-inorganic hybrid metal halide perovskites have emerged as a highly promising class of light emitters, which can be used as phosphors for optically pumped white light-emitting diodes (WLEDs). By controlling the structural dimensionality, metal halide perovskites can exhibit tunable narrow and broadband emissions from the free-exciton and self-trapped excited states, respectively. Here, we report a highly efficient broadband yellow light emitter based on zero-dimensional tin mixed-halide perovskite (CNHBr)SnBrI (x = 3). This rare-earth-free ionically bonded crystalline material possesses a perfect host-dopant structure, in which the light-emitting metal halide species (SnBrI, x = 3) are completely isolated from each other and embedded in the wide band gap organic matrix composed of CNHBr. The strongly Stokes-shifted broadband yellow emission that peaked at 582 nm from this phosphor, which is a result of excited state structural reorganization, has an extremely large full width at half-maximum of 126 nm and a high photoluminescence quantum efficiency of ∼85% at room temperature. UV-pumped WLEDs fabricated using this yellow emitter together with a commercial europium-doped barium magnesium aluminate blue phosphor (BaMgAlO:Eu) can exhibit high color rendering indexes of up to 85.
Hybrid organic-inorganic metal halide perovskites possess exceptional structural tunability, with three- (3D), two- (2D), one- (1D), and zero-dimensional (0D) structures on the molecular level all possible. While remarkable progress has been realized in perovskite research in recent years, the focus has been mainly on 3D and 2D structures, with 1D and 0D structures significantly underexplored. The synthesis and characterization of a series of low-dimensional organic tin bromide perovskites with 1D and 0D structures is reported. Using the same organic and inorganic components, but at different ratios and reaction conditions, both 1D (C N H )SnBr and 0D (C N H Br) SnBr can be prepared in high yields. Moreover, photoinduced structural transformation from 1D to 0D was investigated experimentally and theoretically in which photodissociation of 1D metal halide chains followed by structural reorganization leads to the formation of a more thermodynamically stable 0D structure.
Zero-dimensional (0D) halides perovskites, in which anionic metal-halide octahedra (MX6)4− are separated by organic or inorganic countercations, have recently shown promise as excellent luminescent materials.
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