Abstract
Single crystalline zero-dimensional (0D) organic-inorganic hybrid materials with perfect host-guest structures have been developed as a new generation of highly efficient light emitters. Here we report a series of lead-free organic metal halide hybrids with a 0D structure, (C4N2H14X)4SnX6 (X = Br, I) and (C9NH20)2SbX5 (X = Cl), in which the individual metal halide octahedra (SnX64-) and quadrangular pyramids (SbX52-) are completely isolated from each other and surrounded by the organic ligands C4N2H14X+ and C9NH20+, respectively. The isolation of the photoactive metal halide species by the wide band gap organic ligands leads to no interaction or electronic band formation between the metal halide species, allowing the bulk materials to exhibit the intrinsic properties of the individual metal halide species. These 0D organic metal halide hybrids can also be considered as perfect host-guest systems, with the metal halide species periodically doped in the wide band gap matrix. Highly luminescent, strongly Stokes shifted broadband emissions with photoluminescence quantum efficiencies (PLQEs) of close to unity were realized, as a result of excited state structural reorganization of the individual metal halide species. Our discovery of highly luminescent single crystalline 0D organic-inorganic hybrid materials as perfect host-guest systems opens up a new paradigm in functional materials design.
Highlights
Light emitting materials are one of the essential components of life today with applications in a wide range of areas, from energy to information, environmental and healthcare technologies
The isolation of the photoactive metal halide species by the wide band gap organic ligands leads to no interaction or electronic band formation between the metal halide species, allowing the bulk materials to exhibit the intrinsic properties of the individual metal halide species
These 0D organic metal halide hybrids can be considered as perfect host–guest systems, with the metal halide species periodically doped in the wide band gap matrix
Summary
A crystalline solid is a material whose constituents, such as atoms, molecules or ions, are arranged in an ordered structure, forming a periodic lattice that extends in all directions. The interactions between the lattice points could lead to the formation of electronic band structures.[8] As a result, the properties of inorganic crystals show a strong dependence on their size, especially in the nanoscale, the so called quantum size effect.[9] The molecular interactions in organic crystals cause their properties to be distinct from those of individual molecules.[10] Single crystalline materials that exhibit bulk properties consistent with their individual building blocks, or bulk assemblies of 0D materials without electronic band formation. Note that our 0D hybrid materials are bulk crystals with 0D structures on a molecular level, not morphological nanoscale 0D materials, such as quantum dots
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