Enhancement Mechanisms of the Second Harmonic Generation from Double Resonant Aluminum Nanostructures

Multiresonant plasmonic nanoantennas have recently gained a lot of attention due to their ability to enhance nonlinear optical processes at the nanoscale. The first nanostructure designed for this purpose was an aluminum antenna composed of three arms, designed to be resonant at both the fundamental and the second harmonic frequencies. It was demonstrated that second harmonic generation induced by its resonances at both the fundamental and second harmonic wavelengths is higher than the one from a simple dipolar nanoantenna supporting a resonance at the fundamental wavelength only. However, the underlying mechanisms leading to this strong nonlinear signal are still unclear. In this study, both advanced simulations and experiments are combined to investigate in details the role of the mode coupling in the enhancement of second harmonic generation. By varying the length of the nanoantenna arms, it is clearly demonstrated that second harmonic generation is enhanced when the coupling between the quadrupole and the dipole modes at the second harmonic wavelength is significant. Indeed, using a numerical analysis based on the spatial selection of the second harmonic sources, it is shown that the second harmonic quadrupolar mode, which is directly excited by the fundamental pump, can resonantly transfer its energy to the second harmonic dipolar mode supported by another part of the nanoantenna due to near-field coupling. The study of the second harmonic generation mechanisms of double resonant plasmonic systems is important for the design of efficient second harmonic meta-devices such as coherent extreme-ultraviolet sources, ultrasensitive index, and chiral plasmonic sensors.