Dramatic Enhancement of Third-Harmonic Generation in Plasmonic Nanostructures via Nonlocal Effects

Classical nonlocality in conducting nanostructures has been shown to dramatically alter the linear optical response, by placing a fundamental limit on the maximum field enhancement that can be achieved. This limit directly extends to all nonlinear processes, which depend on field amplitudes. A study of third-harmonic generation in metal film-coupled nanowires reveals that for sub-nanometer vacuum gaps the nonlocality enhances the effective nonlinearity by four orders of magnitude as the field penetrates deeper inside the metal than that predicted assuming a purely local electronic response.