Inhomogeneities in the nonlinear tensorial responses of arrays of gold nanodots

We use second- and third-harmonic-generation microscopy to address the tensorial nonlinear responses of individual particles in an array of cylindrical gold nanodots. The responses in both orders exhibit widely-variable, polarization-dependent differences between individual nanodots and thereby indicate tensorial inhomogeneities in the sample. The result provides clear evidence that the second-order response, which is forbidden by symmetry for ideal particles, must arise from small-scale, symmetry-breaking features. A similar result for the third-order response, which is allowed for ideal particles, suggests that both nonlinear responses are dominated by strong variations in field localization around the small-scale features differing among individual nanodots.