Second Harmonic Scattering from Silver Nanocubes

The second harmonic light scattered from silver nanocubes dispersed in an aqueous suspension is investigated. The first hyperpolarizability is determined and corrected for resonance enhancement. It is shown to be similar to that of silver nanospheres with a comparable volume. The polarization-resolved analysis of the scattered harmonic intensity exhibits a surface response strongly modulated by the different multipolar field contributions. As a result, the shape does not play a leading role anymore for nanoparticles with a centrosymmetric shape when retardation must be considered. Comparing the right angle and forward-scattered polarized intensity responses, the unequal balance of the eight nanocube corners' contribution to the total response is revealed despite the high degree of centrosymmetry of the cubic shape. It is then demonstrated with a simple model that the nanocubes' first hyperpolarizability exhibits an octupolar tensorial symmetry. The surface integral equation method calculations are finally provided to investigate further the role of the corners' and edges' rounding.