期刊
NANO LETTERS
卷 21, 期 11, 页码 4780-4786出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c01322
关键词
chiral plasmonics; photoemission electron microscopy; ultrafast optics; near-field imaging; nanofemto scale
类别
资金
- JSPS KAKENHI [JP18H05205, JP18K05053, JP20H05083]
- Dynamic Alliance for Open Innovation Bridging Human, Environment, and Materials (Five-Star Alliance) of MEXT
- Center for Emergent Functional Matter Science of National Chiao Tung University from the Featured Areas Research Center Program within Ministry of Education (MOE) in Taiwan
- Nanotechnology Platform (Hokkaido University)
By studying gold nanorods, the spatiotemporal origin of plasmonic chiroptical responses was revealed, promoting a full understanding of the ultrafast chiral origin in complex nanostructures. This research opens a way to design chiroptical nanophotonic devices for spatiotemporal control of chiral light-matter interactions.
The spatiotemporal origin of plasmonic chiroptical responses in nanostructures remains unexplored and unclear. Here, two orthogonally oriented Au nanorods as a prototype were investigated, with a giant chiroptical response caused by antisymmetric and symmetric mode excitations for obliquely incident left-handed circular polarization (LCP) and right-handed circular polarization (RCP) light. Time-resolved photoemission electron microscopy (PEEM) was employed to measure the near-field spatial distributions, spectra, and spatiotemporal dynamics of plasmonic modes associated with the chiroptical responses at the nanofemto scale, verifying the characteristic near-field distributions at the resonant wavelengths of the two modes and a very large spectral dichroism for LCP and RCP. More importantly, eigenmode excitations and their contributions to the ultrafast plasmonic chiroptical response in the space-time domain were directly revealed, promoting a full understanding of the ultrafast chiral origin in complex nanostructures. These findings open a way to design chiroptical nanophotonic devices for spatiotemporal control of chiral light-matter interactions.
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