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Role of anion polarizability in fluorescence sensitization of DNA-templated silver nanoclusters

机译:阴离子极化性在以DNA为模板的银纳米团簇的荧光增敏中的作用

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摘要

Fluorescent silver nanoclusters (Ag NCs) as novel fluorophores have received much attention because of their high brightness, good photostability and widely tunable emissions from the visible to the near-infrared range as a result of their size and existing environment. However, efforts are still needed to find the factors that tune the emission of Ag NCs. In this work, Ag NCs that were size-selectively grown on DNA were used to investigate the effect of the electronic properties of coordinating ligands. Halogen anions were used as the paradigm because of their periodicity in element properties. We found that addition of halogen anions did not alter the emission wavelength of Ag NCs, but the fluorescence intensity showed an initial increase at low concentrations of Cl~-, Br~- and I~- followed by a gradual decrease at high concentrations. No increase in fluorescence was observed for F~- at either low or high concentration. Such specific halogen-anion sensitization of the fluorescence of Ag NCs suggests that the binding strength/ manner and dipole polarizability of these anions synergistically tune the emission behavior of Ag NCs. Less fluorescence sensitization occurred for the anion having high enough polarizability to form a covalent bond with Ag NCs. The anion polarizability-sensitized fluorescence indicates the role of anion electronic properties in tuning the emission behavior of Ag NCs, which should be seriously considered in designing Ag NC-based sensors and devices.
机译:作为新型荧光团的荧光银纳米团簇(Ag NCs)由于其高亮度,良好的光稳定性以及由于其尺寸和现有环境而导致的从可见光到近红外范围的广泛可调发射而备受关注。但是,仍需要努力找到调节Ag NCs排放的因素。在这项工作中,使用大小选择性地在DNA上生长的Ag NCs来研究配位体电子性质的影响。卤素阴离子由于其元素性质的周期性而被用作范例。我们发现添加卤素阴离子不会改变Ag NCs的发射波长,但是荧光强度在低浓度的Cl〜-,Br〜-和I〜-时显示出初始增加,然后在高浓度时逐渐减少。在低浓度或高浓度下,F〜-均未观察到荧光增加。 Ag NCs荧光的这种特殊的卤素阴离子敏化表明,这些阴离子的结合强度/方式和偶极极化性可协同调节Ag NCs的发射行为。具有足够高的极化率以与Ag NCs形成共价键的阴离子发生的荧光增感较小。阴离子可极化性敏化的荧光表明阴离子电子性质在调节Ag NCs的发射行为中的作用,在设计基于Ag NC的传感器和设备时应认真考虑。

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