Second harmonic generation microscopy is used for the investigation of the nonlinear optical response of single gold
nanowires and aggregates of quasi-spherical gold nanomaterials. Angular and spectral resolved approaches are
performed to study the origin of the second harmonic emission (SH) from isolated gold nanowire, nanosphere and
interacting nanospheres in aggregates. It is observed that the Second harmonic efficiency is enhanced when the
excitation wavelength is resonant with the surface plasmon mode (SP) of the metallic nanomaterials. The angular
resolved second harmonic analysis study demonstrated the presence of different origins (dipolar, quadrupolar and
octupolar modes) involved in the nonlinear optical emission from gold nanowires and nanospheres. Our investigation
demonstrates the important role of electric dipole arising from the breaking of the centrosymmetry at the surface of the
nanowire and imperfect spherical shape of the gold nanospheres, and in the size regime below 50 nm. The increase of the
aggregate and nanowire size induces the presence of interferences between higher orders (quadrupole) and dipole
sources. For size higher than 50 nm, the analysis of the angular resolved emission pattern demonstrates the presence of
retardation effects and the deviation from the dipolar emission picture. The results are in good agreement with the actual
reported results in terms of character of emission. Finally, the SH emission of gold nanowire was spectrally analyzed for
single gold nanowire and variable aggregates size. A clear SH emission is observed at 2ω for each excitation frequency
ω with the presence of 2 photons visible photoluminescence emission (2PL).
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