Ultrafast Dynamics of Strong Near‐Field Coupled Localized and Delocalized Surface Plasmons

Abstract This paper reports transient dynamics of strong near‐field coupling behavior of plasmons in a multilayer metal nanostructure that enables ultrahigh‐efficient optical switching. Particle plasmon on the top array units couples with localized/delocalized plasmons on the bottom Au film to produce dipolar and high‐order hybrid modes with nearly suppressed reflection. The mode coupling can be tuned from near‐field to far‐field regime readily mediated by the spacer thickness. The dipolar mode inherits the high dispersive property of the delocalized plasmon, but the higher‐order one shows limited dispersion. Transient spectroscopy illustrates both hybrid modes have a picosecond timescale redshift under on‐ and off‐resonance excitation. However, the higher‐order mode exhibits a longer decay lifetime than the dipolar one because of resonance characteristics and cavity properties. An ultrafast optical switching effect with a response time of τ = 3.2 ps and an ultrahigh efficiency of 5100 mOD mJ −1 cm 2 is achieved under an extremely low pump fluence.