Ultrafast resonant optical scattering from single gold nanorods: Large nonlinearities and plasmon saturation

We measure nonlinear optical scattering from individual Au nanorods excited by ultrafast laser pulses on resonance with their longitudinal plasmon mode. Isolating single rods removes inhomogeneous broadening and allows the measurement of a large nonlinearity, much greater than that of nanorod ensembles. Surprisingly, the ultrafast nonlinearity can be attributed entirely to heating of conduction electrons and does not exhibit any response associated with coherent plasmon oscillation. This indicates an unanticipated damping of strongly driven plasmons.