Harmonic Generation in Metal-Insulator and Metal-Insulator-Metal Nanostructures

We report that the second and third harmonic signal reductions with insulator film surface coverage over a gold substrate gives a measure of the electron density in the spill out volume of the insulator, which is dubbed metal insulator gap states. For metal-insulator-metal (MIM) structures we observe enhancement saturation and quenching of the third harmonic efficiencies well above the efficiencies for metal-insulator (MI) samples. The measured optical harmonics of scattered light from MI and MIM systems are compared with detailed simulations of the nonlinear interactions including free electron spill out into the insulator, nonlocal and electron quantum tunneling effects. Gold coated substrates are covered with variable thin insulator film thicknesses using atomic layer deposition. Optical harmonics of light scattered from two insulator materials (ZnO and Al2O3) are measured in our experiments. Based on our simulations we conclude that the observed MIM signal enhancement effects are primarily due to nonlocal phenomena in an electron gas.