Abstract:Off-normal, polarization dependent second-harmonic generation (SHG) measurements were performed ex situ on plasmonic nanostructures grown by self-assembly on nanopatterned templates. These exploratory studies of Ag nanoparticle (NP) arrays show that the sensitivity of SHG to the local fields, which are modified by the NP size, shape and distribution, makes it a promising fixed wavelength characterization technique that avoids the complexity of spectroscopic SHG. The off-normal geometry provides access to the out-of-plane SH response, which is typically an order-of-magnitude larger than the in-surface-plane response measured using normal incidence, for example in SHG microscopy. By choosing the plane of incidence orthogonal to the NP array direction, it was shown that the p−polarized SH response, as a function of input polarization, is very sensitive to NP morphology, with a change of 20% in the aspect ratio of the NPs producing a variation of a factor of 30 in the easily measureable ratio of the p−polarized SH field strength for s− and p−polarized input. The results show that such a fixed geometry could be used for the in situ characterization of anisotropic nanostructure morphology during growth by self-assembly, which could be particularly useful in situations where rotating the sample may be neither desirable nor easily accomplished. Rep. 408, 131-314 (2005). 34. G. Bachelier and J. Butet and I. Russier-Antoine and C. Jonin and E.Benichou and P. F. Brevet, "Origin of optical second-harmonic generation in spherical gold nanoparticles: local surface and nonlocal bulk contributions," Phys.