期刊
SCIENCE
卷 373, 期 6550, 页码 95-+出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.abg8790
关键词
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资金
- JST PRESTO [JPMJPR1862, JPMJPR20T1]
- Japan Society for the Promotion of Science (JSPS) KAKENHI [JP19H04681, JP 17H04796, JP 19K23591, JP 18H05257, JP17H06173, JP17H05430, JP20H02728, JP20K05412, JP20H04652, JP20K05592]
A single-molecule spectroscopic method with micro-electron volt energy and submolecular-spatial resolution has been developed to induce molecular luminescence in scanning tunneling microscopy. The state-selective characterization of energy levels and linewidths of individual electronic and vibrational quantum states of a single molecule has been demonstrated. Tuning energy levels of molecular systems through the Stark effect and plasmon-exciton coupling in the tunneling junction opens up possibilities for creating designed energy-converting functions.
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.
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