Real-space and real-time observation of a plasmon-induced chemical reaction of a single molecule

Real-space and real-time observation of a plasmon-induced chemical reaction of a single molecule
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DOI:
10.1126/science.aao0872
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发表时间:
2018-05-04
期刊:
影响因子:
56.9
通讯作者:
Kim, Yousoo
Kim, Yousoo
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Kazuma, Emiko;Jung, Jaehoon;Kim, Yousoo

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等离子体激元诱导的吸附在金属纳米结构上的分子的化学反应在光催化反应中引起了越来越多的关注。然而,该机制仍然存在争议,因为直接观察等离子体场中的化学反应是困难的,这是强烈的局部金属表面附近。我们利用扫描隧道显微镜(STM)实现了在单分子水平上对等离子体诱导的化学反应的实时空间观察。一个单一的二甲基二硫分子在银和铜表面的STM结处的光激发等离子体解离。STM研究结合理论计算表明,这种等离子体激元诱导的化学反应发生的直接分子内激发机制。
Plasmon-induced chemical reactions of molecules adsorbed on metal nanostructures are attracting increased attention for photocatalytic reactions. However, the mechanism remains controversial because of the difficulty of direct observation of the chemical reactions in the plasmonic field, which is strongly localized near the metal surface. We used a scanning tunneling microscope (STM) to achieve real-space and real-time observation of a plasmon-induced chemical reaction at the single-molecule level. A single dimethyl disulfide molecule on silver and copper surfaces was dissociated by the optically excited plasmon at the STM junction. The STM study combined with theoretical calculations shows that this plasmon-induced chemical reaction occurred by a direct intramolecular excitation mechanism.