期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 12, 期 14, 页码 3535-3539出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.1c00763
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资金
- United States Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences Biosciences
- United States Department of Energy, Office of Science, Office of Biological and Environmental Research, through the bioimaging technology development program
- Laboratory Directed Research and Development (LDRD) program at Pacific Northwest National Laboratory
The research demonstrates that four-wave mixing at plasmonic tip-sample nano-junctions can visualize plasmonic fields with sub-2 nm spatial resolution under ambient laboratory conditions. By utilizing specific techniques, the four-wave mixing signal can be further enhanced, paving the way for visualizing chemical transformations and coherent electronic and vibrational dynamics with femtosecond temporal and few-nanometer spatial resolution under ambient conditions.
Four-wave mixing at plasmonic tip-sample nano-junctions may be used to visualize plasmonic fields with sub-2 nm spatial resolution under ambient laboratory conditions. We illustrate the latter using a gold-coated atomic force microscopy probe irradiated with a pair of near-infrared femtosecond laser pulses and used to image plasmonic gold nanoplates and silver nanocubes. Through diagnostic polarization-dependent tip-only measurements, we illustrate that the four-wave mixing signal is localized to the tip apex. The apex-bound signal is further enhanced when the tip is located at specific locations near plasmonic nanoparticles. Overall, this work paves the way for visualizing chemical transformations as well as coherent electronic and vibrational dynamics with joint femtosecond temporal and few-nanometer spatial resolution under ambient conditions.
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