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Sb-Doped Metal Halide Nanocrystals: A 0D versus 3D Comparison.

ABSTRACT: We synthesize colloidal nanocrystals (NCs) of Rb₃InCl₆, composed of isolated metal halide octahedra ("0D"), and of Cs₂NaInCl₆ and Cs₂KInCl₆ double perovskites, where all octahedra share corners and are interconnected ("3D"), with the aim to elucidate and compare their optical features once doped with Sb³⁺ ions. Our optical and computational analyses evidence that the photoluminescence quantum yield (PLQY) of all these systems is consistently lower than that of the corresponding bulk materials due to the presence of deep surface traps from under-coordinated halide ions. Also, Sb-doped "0D" Rb₃InCl₆ NCs exhibit a higher PLQY than Sb-doped "3D" Cs₂NaInCl₆ and Cs₂KInCl₆ NCs, most likely because excitons responsible for the PL emission migrate to the surface faster in 3D NCs than in 0D NCs. We also observe that all these systems feature a large Stokes shift (varying from system to system), a feature that should be of interest for applications in photon management and scintillation technologies. Scintillation properties are evaluated via radioluminescence experiments, and re-absorption-free waveguiding performance in large-area plastic scintillators is assessed using Monte Carlo ray-tracing simulations.

SUBMITTER: Zhu D

PROVIDER: S-EPMC8294020 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:To investigate the effect of the polycarboxylates and metal ions on the assembly and structures of complexes based on a thiophene-containing bis-pyridyl-bis-amide N,N'-bis(pyridine-3-yl)thiophene-2,5-dicarboxamide (3-bptpa) ligand, nine 0D ? 3D complexes of [Ni2(3-bptpa)4(1,2-BDC)2(H2O)2] (1), [Ni(3-bptpa)(IP)(H2O)2]·H2O (2), [Ni(3-bptpa)(5-MIP)(H2O)2]·H2O (3), [Ni(3-bptpa)(5-NIP)(H2O)] (4), [Ni(3-bptpa)(5-AIP)]·2H2O (5), [Ni2(OH)(3-bptpa)(1,3,5-BTC)]·DMA·5H2O (6), [Cu(3-bptpa)(5-MIP)]·3H2O (7), [Cu(3-bptpa)(5-AIP)(H2O)0.25]·H2O (8), and [Cu(3-bptpa)(1,3,5-HBTC)] (9) (1,2-H2BDC = 1,2-benzenedicarboxylic acid, H2IP = 1,3-benzenedicarboxylic acid, 5-H2MIP = 5-methylisophthalic acid, 5-H2NIP = 5-nitroisophthalic acid, 5-H2AIP = 5-aminoisophthalic acid, DMA = N,N'-dimethylacetamide, and 1,3,5-H3BTC = 1,3,5-benzenetricarboxylic acid) have been hydrothermally/solvothermally synthesized and structurally characterized by IR, thermogravimetric, powder X-ray diffraction, and single-crystal X-ray diffraction. Complex 1 is a zero-dimensional (0D) bimetallic complex. Complexes 2 and 3 feature two similar one-dimensional ladderlike structures. Complex 4 displays a two-dimensional (2D) 4-connected network based on single-metallic nodes. Complex 5 shows a 2D double-layer structure containing a pair of 63 [Ni(5-AIP)] honeycomblike sheets. Complex 6 is a 3,5-connected three-dimensional (3D) framework derived from bimetallic nodes and 63 [Ni2(OH)(1,3,5-BTC)] honeycomblike sheets. Complex 7 displays a 2D 4-connected grid based on bimetallic nodes. Complex 8 features a 2D double-layer structure based on two 4-connected [Cu(3-bptpa)(5-AIP)] sheets and bridging coordinated water molecules. Complex 9 is a 2D structure extended by incomplete deprotonation of 1,3,5-HBTC and 3-bptpa linkers. The effect of the metal ions and polycarboxylates on the structures of the title complexes was discussed, and the fluorescent properties of 1-9 were investigated. The carbon paste electrodes bulk-modified by complexes 3, 5, and 6-9 show different electrocatalytic activities for the oxidation of ascorbic acid as well as the reduction of hydrogen peroxide, nitrites, and bromates.

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Sb-Doped Metal Halide Nanocrystals: A 0D versus 3D Comparison.

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