Crystallization-induced emission enhancement: A novel fluorescent Au-Ag bimetallic nanocluster with precise atomic structure.
Crystallization-induced emission enhancement: A novel fluorescent Au-Ag bimetallic nanocluster with precise atomic structure.
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结晶诱导发射增强：一种具有精确原子结构的新型荧光金银双金属纳米团簇
DOI：
10.1126/sciadv.1700956
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发表时间：
2017-08
期刊：
影响因子：
13.6
通讯作者：
Zhu M
中科院分区：
文献类型：
--
作者：
Chen T;Yang S;Chai J;Song Y;Fan J;Rao B;Sheng H;Yu H;Zhu M
首次在金属纳米团簇中实现了晶化诱导的发光增强。我们报道了第一个具有结晶诱导发射增强（CIEE）的贵金属纳米团簇Au 4Ag 13（DPPM）3（SR）9，其中DPPM表示双（二苯基膦基）甲烷，HSR表示2，5-二甲基苯乙胺。精确的原子结构由X射线晶体学确定。Au_4Ag_13的晶态在695 nm处显示出强的发光，与非晶态的弱发光形成鲜明对比，并且在溶液相中几乎没有发光。结构分析和密度泛函理论计算表明，紧密的C-H <$π相互作用显著地限制了分子内的转动和振动，从而显著地增强了晶态的辐射跃迁.由于非共价相互作用可以通过改变化学环境来容易地调节，CIEE现象可能代表了放大来自弱（甚至非）发射纳米团簇的荧光的一般策略。
Crystallization-induced emission enhancement was achieved in metal nanoclusters for the first time. We report the first noble metal nanocluster with a formula of Au4Ag13(DPPM)3(SR)9 exhibiting crystallization-induced emission enhancement (CIEE), where DPPM denotes bis(diphenylphosphino)methane and HSR denotes 2,5-dimethylbenzenethiol. The precise atomic structure is determined by x-ray crystallography. The crystalline state of Au4Ag13 shows strong luminescence at 695 nm, in striking contrast to the weak emission of the amorphous state and hardly any emission in solution phase. The structural analysis and the density functional theory calculations imply that the compact C–H⋯π interactions significantly restrict the intramolecular rotations and vibrations and thus considerably enhance the radiative transitions in the crystalline state. Because the noncovalent interactions can be easily modulated via varying the chemical environments, the CIEE phenomenon might represent a general strategy to amplify the fluorescence from weakly (or even non-) emissive nanoclusters.
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