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zhangkun232至尊木蟲 (著名寫手)
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貴金屬納米團(tuán)簇的分子發(fā)光機(jī)制 已有2人參與
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金屬納米團(tuán)簇的發(fā)光一直以來存在非常大的爭議，有兩個核心機(jī)制：貴金屬納米團(tuán)簇的量子尺寸限域效應(yīng)和表面配體主導(dǎo)的空間電子效應(yīng)，越來越多的證據(jù)證明表面配體對發(fā)光的調(diào)控起到?jīng)Q定性作用，但是發(fā)光的中心是表面的保護(hù)性配體還是其它吸附的化學(xué)組分。結(jié)合各種穩(wěn)態(tài)譜學(xué)以及飛秒超快技術(shù)，我們在國際上率先提出了，貴金屬納米團(tuán)簇的發(fā)光中心來源于界面吸附的結(jié)構(gòu)水分子，這正結(jié)構(gòu)水分子不同于傳統(tǒng)的氫鍵水分子，并且提出了拓?fù)浼ぐl(fā)的概念。論文發(fā)表在Nanoscale（Nanoscale, 2021,13, 15058-15066；DOI https://doi.org/10.1039/D1NR02389F）上，歡迎大家留言討論。文章鏈接如下：https://pubs.rsc.org/en/content/articlelanding/2021/nr/d1nr02389f Caged structural water molecules emit tunable brighter colors by topological excitation† bstract Intrinsically, free water molecules are a colourless liquid. If it is colourful, why and how does it emit the bright colours? We provided direct evidence that when water was trapped into the sub-nanospace of zeolites, the structural water molecules (SWs) exhibited strong tunable photoluminescence (PL) emissions from blue to red colours with unprecedented ultra-long lifetimes up to the second scale at liquid nitrogen temperature. Further controlled experiments and combined characterizations by time-resolved steady-state and ultra-fast femtosecond (fs) transient optical spectroscopy showed that the singly adsorbed hydrated hydroxide complex {OH−·H2O} as SWs in the confined nanocavity is the true emitter centre, whose PL efficiency strongly depends on the type and stability of the SWs, which is dominated by H-bond interactions, such as the solvent effect, pH value and operating temperature. The emission of SWs exhibits the characteristic of topological excitations (TAs) due to the many-body quantum electron correlations in confined nanocavities, which differs from the local excitation of organic chromophores. Our model not only elucidates the origin of the PL of metal nanoclusters (NCs), but also provides a completely new insight to understand the nature of heterogeneous catalysis and interface bonding (or state) at the molecule level, beyond the metal-centred d band theory. |
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zhangkun232
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9樓2022-04-19 10:01:12
zhangkun232
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willbuilder
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3樓2021-09-21 07:06:26
zhangkun232
至尊木蟲 (著名寫手)
- 應(yīng)助: 24 (小學(xué)生)
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最新的研究進(jìn)展，尤其是關(guān)于雙金屬納米團(tuán)簇的發(fā)光機(jī)制：鏈接如下： https://www.frontiersin.org/arti ... em.2021.756993/full |
4樓2021-09-27 18:51:31
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