Dataset Information

Ultrabright Au@Cu₁₄ nanoclusters: 71.3% phosphorescence quantum yield in non-degassed solution at room temperature.

ABSTRACT: The photoluminescence of metal nanoclusters is typically low, and phosphorescence emission is rare due to ultrafast free-electron dynamics and quenching by phonons. Here, we report an electronic engineering approach to achieving very high phosphorescence (quantum yield 71.3%) from a [Au@Cu₁₄(SPh ^t Bu)₁₂(PPh(C₂H₄CN)₂)₆]⁺ nanocluster (abbreviated Au@Cu ₁₄ ) in non-degassed solution at room temperature. The structure of Au@Cu ₁₄ has a single-Au-atom kernel, which is encapsulated by a rigid Cu(I) complex cage. This core-shell structure leads to highly efficient singlet-to-triplet intersystem crossing and suppression of nonradiative energy loss. Unlike the phosphorescent organic materials and organometallic complexes-which require de-aerated conditions due to severe quenching by air (i.e., O₂)-the phosphorescence from Au@Cu ₁₄ is much less sensitive to air, which is important for lighting and biomedical applications.

SUBMITTER: Song Y

PROVIDER: S-EPMC7787487 | biostudies-literature | 2021 Jan

REPOSITORIES: biostudies-literature

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Ultrabright Au@Cu14 nanoclusters: 71.3% phosphorescence quantum yield in non-degassed solution at room temperature.

Song Yongbo Y Li Yingwei Y Zhou Meng M Liu Xuan X Li Hao H Wang He H Shen Yuhua Y Zhu Manzhou M Jin Rongchao R

Science advances 20210106 2

The photoluminescence of metal nanoclusters is typically low, and phosphorescence emission is rare due to ultrafast free-electron dynamics and quenching by phonons. Here, we report an electronic engineering approach to achieving very high phosphorescence (quantum yield 71.3%) from a [Au@Cu14(SPh t Bu)12(PPh(C2H4CN)2)6]+ nanocluster (abbreviated Au@Cu 14 ) in non-degassed soluti ...[more]

PMID: 33523969

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Project description:Semiconducting polymer dots (Pdots) are increasingly used in biomedical applications due to their extreme single-particle brightness, which results from their large absorption cross section (σ). However, the quantum yield (Φ) of Pdots is typically below 40% due to aggregation-induced self-quenching. One approach to reducing self-quenching is to use FRET between the donor (D) and acceptor (A) groups within a Pdot; however, Φ values of FRET-based Pdots remain low. Here, we demonstrate an approach to achieve ultrabright FRET-based Pdots with simultaneously high σ and Φ. The importance of self-quenching was revealed in a non-FRET Pdot: adding 30 mol % of a nonabsorbing polyphenyl to a poly(9,9-dioctylfluorene) (PFO) Pdot increased Φ from 13.4 to 71.2%, yielding an ultrabright blue-emitting Pdot. We optimized the brightness of FRET-based Pdots by exploring different D/A combinations and ratios with PFO and poly[(9,9-dioctylfluorenyl-2,7-diyl)-co-(1,4-phenylene)] (PFP) as donor polymers and poly[(9,9-dioctyl-2,7-divinylenefluorenylene)-alt-co-(1,4-phenylene)] (PFPV) and poly[(9,9-dioctylfluorenyl-2,7-diyl)-alt-co-(1,4-benzo-{2,1',3}-thiadiazole)] (PFBT) as acceptor polymers, with a fixed concentration of poly(styrene-co-maleic anhydride) as surfactant polymer. Ultrabright blue-emitting Pdots possessing high Φ (73.1%) and σ (σR = σabs/σall, 97.5%) were achieved using PFP/PFPV Pdots at a low acceptor content (A/[D + A], 2.5 mol %). PFP/PFPV Pdots were 1.8 times as bright as PFO/PFPV Pdots due to greater coverage of acceptor absorbance by donor emission─a factor often overlooked in D/A pair selection. Ultrabright green-emitting PFO Pdots (Φ = 76.0%, σR = 92.5%) were obtained by selecting an acceptor (PFBT) with greater spectral overlap with PFO. Ultrabright red-emitting Pdots (Φ = 64.2%, σR = 91.0%) were achieved by blending PFO, PFBT, and PFTBT to create a cascade FRET Pdot at a D:A1:A2 molar ratio of 61:5:1. These blue, green, and red Pdots are among the brightest Pdots reported. This approach of using a small, optimized amount of FRET acceptor polymer with a large donor-acceptor spectral overlap can be generalized to produce ultrabright Pdots with emissions that span the visible spectrum.

Dataset Information

Ultrabright Au@Cu₁₄ nanoclusters: 71.3% phosphorescence quantum yield in non-degassed solution at room temperature.

Publications

Ultrabright Au@Cu<sub>14</sub> nanoclusters: 71.3% phosphorescence quantum yield in non-degassed solution at room temperature.

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