Enhancement of bulk-type multipolar second-harmonic generation arising from surface morphology of metals

Gold films of 20 and 150 nm nominal thickness were characterized by two-beam second-harmonic generation to address their second-order nonlinear optical responses of surface (dipolar) and bulk (higher multipolar) origin. The surface response is enhanced by ~20% in the case of the 20 nm film, as expected due to its higher surface roughness. Surprisingly, the bulk-type response is enhanced to a greater extent, exceeding 80%, and this can be explained by effective quadrupolar nonlinearity arising from the field interaction with the local nonlinearity of nanoscale surface features.