期刊
ACS PHOTONICS
卷 8, 期 10, 页码 2868-2875出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsphotonics.1c01100
关键词
plasmonics; picocavity; adatom; SERS; localization spectroscopy
类别
资金
- European Research Council (ERC) under Horizon 2020 research and innovation programme PICOFORCE [883703]
- EPSRC (Cambridge NanoDTC) [EP/L015978/1, EP/L027151/1, EP/S022953/1, EP/P029426/1, EP/R020965/1]
- Trinity College, University of Cambridge
- Leverhulme Trust
- Isaac Newton Trust
- European Research Council (ERC) under Horizon 2020 research and innovation programme POSEIDON [861950]
- EPSRC [EP/R020965/1, EP/S022953/1, EP/P029426/1, EP/L027151/1] Funding Source: UKRI
The study reveals that light suppresses the local effective barrier height for adatom formation, and that the initial barrier height is decreased by reduced atomic coordination numbers near facet edges. Modeling the system also resolves the frequency-dependent picocavity field enhancements supported by these atomic scale features.
Transient atomic protrusions in plasmonic nanocavities confine optical fields to sub-1-nm(3) picocavities, allowing the optical interrogation of single molecules at room temperature. While picocavity formation is linked to both the local chemical environment and optical irradiation, the role of light in localizing the picocavity formation is unclear. Here, we combine information from thousands of picocavity events and simultaneously compare the transient Raman scattering arising from two incident pump wavelengths. Full analysis of the data set suggests that light suppresses the local effective barrier height for adatom formation and that the initial barrier height is decreased by reduced atomic coordination numbers near facet edges. Modeling the system also resolves the frequency-dependent picocavity field enhancements supported by these atomic scale features.
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