Monitoring hydroquinone-quinone redox cycling by single molecule fluorescence spectroscopy.
Monitoring hydroquinone-quinone redox cycling by single molecule fluorescence spectroscopy.
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DOI：
10.1039/c4cp02640c
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发表时间：
2014-08
期刊：
影响因子：
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通讯作者：
A. Rybina;B. Thaler;R. Krämer;D. Herten
中科院分区：
文献类型：
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作者：
A. Rybina;B. Thaler;R. Krämer;D. Herten
目前单分子化学领域的研究越来越多地集中在发展可靠的实验方法，用于使用单分子荧光光谱（SMFS）在分子水平上研究化学过程。在这里，我们报告的单分子观察的铜（II）/空气介导的氧化荧光标记的氢醌为基础的探针分子，然后用半胱氨酸还原。氧化还原循环分别通过添加氧化剂/还原剂后荧光发射的淬灭/恢复来发出信号。实验是通过将探针固定在载玻片上来实现的，以允许通过全内反射荧光显微镜进行单分子观察。除了检测单个探针分子上成功的氧化和还原事件外，单个分子强度轨迹揭示了反应后的动态过程和中间态的形成。对于所提出的实验设计，我们设想进一步的反应研究的催化氧化还原过程的单一的氢醌部分通过SMFS。
Current research in the field of single-molecule chemistry is increasingly focused on the development of reliable experimental approaches for investigating chemical processes on a molecular level using single-molecule fluorescence spectroscopy (SMFS). Herein, we report on single-molecule observations of the copper(II)/air mediated oxidation of fluorescently labeled hydroquinone-based probe molecules followed by their reduction with cysteine. The redox cycle is signaled by quenching/recovery of fluorescence emission after addition of the oxidant/reductant, respectively. The experiments were realized by immobilizing the probe on a glass cover slide to allow single-molecule observation by means of total-internal-reflection fluorescence microscopy. Besides detection of successful oxidation and reduction events on single probe molecules, individual molecular intensity trajectories revealed dynamic processes and formation of intermediate states upon reaction. For the experimental design presented, we envision further reaction studies of catalytic redox-processes of single hydroquinone-moieties by means of SMFS.