期刊
NANO LETTERS
卷 15, 期 10, 页码 6601-6608出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.5b02363
关键词
ITR-PEEM; ultrafast plasmonics; optical antennas; multipolar surface plasmons; nanorice; surface plasmon retardation
类别
资金
- NanoLund
- Swedish Research Council (VR)
- Swedish Foundation for Strategic Research (SSF)
- Crafoord Foundation
- Knut and Alice Wallenberg Foundation
- European Research Council (ERC)
The local enhancement of few-cycle laser pulses by plasmonic nanostructures opens up for spatiotemporal control of optical interactions on a nanometer and few-femtosecond scale. However, spatially resolved characterization of few-cycle plasmon dynamics poses a major challenge due to the extreme length and time scales involved. In this Letter, we experimentally demonstrate local variations in the dynamics during the few strongest cycles of plasmon-enhanced fields within individual rice-shaped silver nanoparticles. This was done using 5.5 fs laser pulses in an interferometric time-resolved photoemission electron microscopy setup. The experiments are supported by finite-difference time-domain simulations of similar silver structures. The observed differences in the field dynamics across a single particle do not reflect differences in plasmon resonance frequency or dephasing time. They instead arise from a combination of retardation effects and the coherent superposition between multiple plasmon modes of the particle, inherent to a few-cycle pulse excitation. The ability to detect and predict local variations in the few-femtosecond time evolution of multimode coherent plasmon excitations in rationally synthesized nanoparticles can be used in the tailoring of nanostructures for ultrafast and nonlinear plasmonics.
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