The competition between plasmonic resonances and noble-metal interband transitions at near-ultraviolet (NUV) frequencies complicates nonlinear conversion processes at nanoscales. Here, we experimentally design a highly enhanced and reproducible plasmon-enhanced second-harmonic generation (PESHG) platform suitable for NUV frequencies by constructing three-dimensional silver mushroom arrays. The SHG emission from proposed platforms involved in geometrical asymmetry greatly outperforms that from unpatterned metallic films. Studies among mushroom arrays with various geometric parameters and weight ratios of component materials enable us to distinguish characteristics exhibited by plasmon-driven enhancement and interband-transition suppression, such that competitive effects on PESHG can be readily observed and quantitatively measured. Our work may provide insights for understanding the physical mechanism governing plasmon-enhanced nonlinear optical processes and may help attain efficient nonlinear wavelength conversions for quantum-optical and nonlinear metamaterial applications.

Plasmon-enhanced second-harmonic generation (PESHG) based on hybrid metal-dielectric nanostructures have extraordinary importance for developing efficient nanoscale nonlinear sources, which pave the way for new applications in photonic circuitry, quantum optics, and biosensors. However, the relatively high loss of excitation energies and the low spatial overlapping between the locally enhanced electromagnetic field and nonlinear materials still limit the promotion of nonlinear conversion performances in such hybrid systems. Here, we design and fabricate an array of silver nanoparticle-ZnO (AgNP-ZnO) nanocavities to serve as an efficient PESHG platform. The geometry of AgNP-ZnO nanocavity arrays provides a way to flexibly modulate hot spots in three-dimensional space, and to achieve a good mutual overlap of hot spots and ZnO material layers for realizing efficient SH photon generation originating from ZnO nanocavities. Compared to bare ZnO nanocavity arrays, the resulting hybrid AgNP-ZnO design of nanocavities reaches the maximum PESHG enhancement by a factor of approximately 31. Validated by simulations, we can further interpret the relative contribution of fundamental and harmonic modes to Ag-NP dependent PESHG performances, and reveal that the enhancement stems from the co-cooperation effect of plasmon-resonant enhancements both for fundamental and harmonic frequencies. Our findings offer a previously unreported method for designing efficient PESHG systems and pave a way for further understanding of a surface plasmon-coupled second-order emission mechanism for the enhancement of hybrid systems.

Plasmonic nanocavities offer prospects for the amplification of inherently weak nonlinear responses at subwavelength scales. However, constructing these nanocavities with tunable modal volumes and reduced optical losses remains an open challenge in the development of nonlinear nanophotonics. Herein, we design and fabricate three-dimensional (3D) metal-dielectric-metal (MDM) plasmonic nanocavities that are capable of amplifying second-harmonic lights by up to three orders of magnitude with respect to dielectric-metal counterparts. In combination with experimental estimations of quantitative contributions of constituent parts in proposed 3D MDM designs, we further theoretically disclose the mechanism governing this signal amplification. We discover that this phenomenon can be attributed to the plasmon hybridization of both dipolar plasmon resonances and gap cavity resonances, such that an energy exchange channel can be attained and helps expand modal volumes while maintaining strong field localizations. Our results may advance the understanding of efficient nonlinear harmonic generations in 3D plasmonic nanostructures.