Nanoscale Imaging of Local Few-Femtosecond Near-Field Dynamics within a Single Plasmonic Nanoantenna

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• 作者：Erik M氓rsell ; Arthur Losquin ; Robin Sv盲rd ; Miguel Miranda ; Chen Guo ; Anne Harth ; Eleonora Lorek ; Johan Mauritsson ; Cord L. Arnold ; Hongxing Xu ; Anne L鈥橦uillier ; Anders Mikkelsen
• 刊名：Nano Letters
• 出版年：2015
• 出版时间：October 14, 2015
• 年：2015
• 卷：15
• 期：10
• 页码：6601-6608
• 全文大小：418K
• ISSN：1530-6992

文摘

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.