Third order nonlinear optics in Ag nanocubes: local and nonlocal optical responses as a function of excitation wavelength and particle size.

Abstract

Colloidal silver nanocubes in solution were analyzed by the Z-scan technique in the resonant and non-resonant regimes. Three different systems with particle sizes of 56, 99 and 215 nm, and concentrations of 0.378, 0.831 and 0.715 mg/mL, respectively, were obtained by the polyol method. Nonlinear excitation of the samples was performed with laser pulses of 26 ps, at a repetition rate of 10 Hz, and using three different wavelenghts (355, 532 and 1064 nm), exciting only the electronic part of the optical nonlinearity, and avoiding induced thermal loading of the samples. Whenever observable, samples showed saturable absorption for all wavelengths, which was dependent, in general, on concentration and incident intensity. For samples featuring sizes of 55 and 99 nm, saturable absorption could be observed for wavelengths close to their dipolar surface plasmon resonances; while, for samples with sizes of 99 and 215 nm, saturable absorption and positive nonlinear optical refraction (only for size of 215 nm) could be observed at 1064 nm. Besides, for some samples, nonlinear optical response followed the incident intensity profile at wavelengths close to resonance. On the contrary, for wavelengths out of resonance, the nonlinear optical behavior showed to be nonlocal, ie, its profile was narrower than the incident one.