Localized surface plasmon (LSP) excitations provide an efficient strategy for advancing nanophotonic designs and applications where strong field enhancement and confinement are often required on the nanoscale. They represent an important plasmonic paradigm for achieving strong light−matter interactions in both linear and nonlinear regimes, enabling the development of high-performance chemical and biological sensing approaches and nonlinear optics with low light intensities. However, the LSP resonance line width, limited by both radiative and resistive losses of metallic nanostructures, is significantly larger than the line width of the waveguided modes supported by low-loss dielectric microcavities with a significantly lower field confinement. Hybrid microcavity−plasmonic systems are, therefore, often used to reduce the resonant line width which improves the detection spectral resolution while maintaining strong confinement. Employing the remarkable quality factors of whispering gallery mode (WGM) microresonators, the hybrid LSP-WGM systems demonstrate sensing capabilities down to the single-molecule level. In this Perspective, we review the recent advances in the hybridization of LSPs and WGMs, focusing on the fundamental understanding of the underlying coupling mechanisms and corresponding mode hybridization regimes. We further discuss opportunities for applying heterogeneous plasmonic−photonic integration to tailor the nanoscale light−matter interactions and realize novel waveguide−plasmon coupling based nontrivial responses and highlight their prospective applications in quantum optics, chiral spin-optics, nonlinear nanophotonics, and sensing.
The ultrasmall mode volume and ultralarge local field enhancement of compact plasmonic nanocavities have been widely explored to amplify a variety of optical phenomena at the nanoscale. Other than passively generating near-field enhancements, dynamic tuning of their intensity and associated nonlinear optical processes such as second-harmonic generation (SHG) play vital roles in the field of active nanophotonics. Here we apply a host–guest molecular complex to construct a photoswitchable molecule-sandwiched metallic particle-on-film nanocavity (MPoFN) and demonstrate both light-controlled linear and nonlinear optical tuning. Under alternating illumination of ultraviolet (UV) and visible light, the photoactive plasmonic molecular nanocavity shows reversible switching of both surface-enhanced Raman scattering (SERS) and plasmon resonance. Surprisingly, we observe more significant modulation of SHG from this photoactive MPoFN, which can be explained qualitatively by the quantum conductivity theory (QCT). Our study could pave the way for developing miniaturized integrated optical circuits for ultrafast all-optical information processing and communication.
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