Single-molecule laser nanospectroscopy with micro-electron volt energy resolution
Single-molecule laser nanospectroscopy with micro-electron volt energy resolution
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DOI：
10.1126/science.abg8790
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发表时间：
2021-07-02
期刊：
影响因子：
56.9
通讯作者：
Kim, Yousoo
中科院分区：
文献类型：
--
作者：
Imada, Hiroshi;Imai-Imada, Miyabi;Kim, Yousoo
需要在单分子和原子水平上表征和控制激发态的方法来利用激发触发的能量转换过程。在这里，我们提出了一个单分子光谱方法与微电子伏的能量和亚分子空间分辨率使用纳米腔等离子体激元的激光驱动，以诱导分子发光扫描隧道显微镜。这种可调谐的单色纳米探针允许对单个分子的单个电子和振动量子态的能级和线宽进行状态选择性表征。此外，我们还证明了利用隧道结中的斯塔克效应和等离子体激元-激子耦合可以对这些态的能级进行微调。我们的技术和研究结果开辟了一条路线，通过使用调谐的分子系统的能级设计的能量转换功能的创建。
Ways to characterize and control excited states at the single-molecule and atomic levels are needed to exploit excitation-triggered energy-conversion processes. Here, we present a single-molecule spectroscopic method with micro-electron volt energy and submolecular-spatial resolution using laser driving of nanocavity plasmons to induce molecular luminescence in scanning tunneling microscopy. This tunable and monochromatic nanoprobe allows state-selective characterization of the energy levels and linewidths of individual electronic and vibrational quantum states of a single molecule. Moreover, we demonstrate that the energy levels of the states can be finely tuned by using the Stark effect and plasmon-exciton coupling in the tunneling junction. Our technique and findings open a route to the creation of designed energy-converting functions by using tuned energy levels of molecular systems.