Third-harmonic generation in the presence of classical nonlocal effects in gap-plasmon nanostructures

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 numerical study of third-harmonic generation in metal film-coupled nanowires reveals that for subnanometer vacuum gaps, the nonlocality may boost the effective nonlinearity by 5 orders of magnitude as the field penetrates deeper inside the metal than that predicted assuming a purely local electronic response. We also study the impact of a nonlinear dielectric placed in the gap region. In this case the effect of nonlocality could be masked by the third-harmonic signal generated by the spacer. By etching the dielectric underneath the nanowire, however, it is possible to muffle such contributions. Calculations are performed for both silver and gold nanowire.