Nonresonant Local Fields Enhance Second-Harmonic Generation from Metal Nanoislands with Dielectric Cover

We study second-harmonic generation from gold nanoislands covered with amorphous titanium oxide (TiO2) films. As the TiO2 thickness increases, the plasmon resonance of the nanoislands shifts away from the second-harmonic wavelength of 532 nm, diminishing the resonant enhancement of the process at this wavelength. Nevertheless, the second-harmonic signal is enhanced by up to a factor of 45 with increasing TiO2 thickness. This unexpected effect arises from the scaling of local fields at the fundamental wavelength of 1064 nm - which is at the far tail of the resonance - due to a change in the dielectric environment of the nanoislands.