Modeling of nonlinear microscopy of localized field enhancements in random metal nanostructures

Nonlinear microscopy of localized field enhancements in random metal nanostructures with a tightly focused laser beam scanning over a sample surface is modeled by making use of analytic representations of the Green dyadic in the near- and far-field regions, with the latter being approximated by the part describing the scattering via excitation of surface plasmon polaritons. The developed approach is applied to scanning second-harmonic (SH) microscopy of small gold spheres placed randomly on a gold surface. We calculate self-consistent fundamental harmonic (FH) and SH field distributions at the illuminated sample surface and, thereby, FH and SH images for different polarization configurations of the illuminating and detected fields. The simulated images bear close resemblance to the images obtained experimentally, exhibiting similar sensitivity to the wavelength and polarization, as well as sensitivity to the scattering configuration. We verify directly our conjecture that very bright spots in the SH images occur due to the spatial overlap of properly polarized FH and SH eigenmodes. Applications and further improvements of the developed model are discussed.