Spectral dependence of nonlinear absorption in ordered silver metallic nanoprism arrays.

Ordered metallic nanoprism arrays have been proposed as novel and versatile systems for the observation of nonlinear effects such as nonlinear absorption. The study of the effect of the local field reinforcement on the fast optical third order nonlinear response around the Surface Plasmon Resonance is of great interest for many plasmonic applications. In this work, silver nanoprism arrays have been synthesized by the nanosphere lithography method. A low repetition rate tunable picosecond laser source was used to study the irradiance and wavelength dependence of the nonlinear absorption properties around the dipolar and quadrupolar resonances of the nanoarray with the use of the z-scan technique. The irradiance dependence of the on-resonance nonlinearity was studied, and a spectral region where nonlinear absorption is negligible was identified. This is important for the possible application of these materials in optical information processing devices.

Ablation and optical third-order nonlinearities in Ag nanoparticles.

The optical damage associated with high intensity laser excitation of silver nanoparticles (NPs) was studied. In order to investigate the mechanisms of optical nonlinearity of a nanocomposite and their relation with its ablation threshold, a high-purity silica sample implanted with Ag ions was exposed to different nanosecond and picosecond laser irradiations. The magnitude and sign of picosecond refractive and absorptive nonlinearities were measured near and far from the surface plasmon resonance (SPR) of the Ag NPs with a self-diffraction technique. Saturable optical absorption and electronic polarization related to self-focusing were identified. Linear absorption is the main process involved in nanosecond laser ablation, but non-linearities are important for ultrashort picosecond pulses when the absorptive process become significantly dependent on the irradiance. We estimated that near the resonance, picosecond intraband transitions allow an expanded distribution of energy among the NPs, in comparison to the energy distribution resulting in a case of far from resonance, when the most important absorption takes place in silica. We measured important differences in the ablation threshold and we estimated that the high selectiveness of the SPR of Ag NPs as well as their corresponding optical nonlinearities can be strongly significant for laser-induced controlled explosions, with potential applications for biomedical photothermal processes.

Anisotropic linear and nonlinear optical properties from anisotropy-controlled metallic nanocomposites.

High-energy metallic ions were implanted in silica matrices, obtaining spherical-like metallic nanoparticles (NPs) after a proper thermal treatment. These NPs were then deformed by irradiation with Si ions, obtaining an anisotropic metallic nanocomposite. An average large birefringence of 0.06 was measured for these materials in the 300-800 nm region. Besides, their third order nonlinear optical response was measured using self-diffraction and P-scan techniques at 532 nm with 26 ps pulses. By adjusting the incident light's polarization and the angular position of the nanocomposite, the measurements could be directly related to, at least, two of the three linear independent components of its third order susceptibility tensor, finding a large, but anisotropic, response of around 10(-7) esu with respect to other isotropic metallic systems. For the nonlinear optical absorption, we were able to shift from saturable to reverse saturable absorption depending on probing the Au NP's major or minor axes, respectively. This fact could be related to local field calculations and NP's electronic properties. For the nonlinear optical refraction, we passed from self-focusing to self-defocusing, when changing from Ag to Au.

Size control of Au nanoparticles on TiO2 and Al2O3 by DP Urea: optical absorption and electron microscopy as control probes.

Gold nanoparticles supported on TiO2 and Al2O3 were prepared by using the deposition-precipitation with urea (DP Urea) method. The control of the particle size was achieved by varying both, the stirring time during the deposition-precipitation (DP) procedure and the conditions of thermal treatment. We focused mainly on the stirring time and the treatment temperature, although gas flow and type of atmosphere also influence importantly the particle's size and shape, as we shall show. The optical response of metallic nanoparticles is given by its surface plasmon resonance and its position and shape depends strongly on the size and the shape of the nanoparticle, as well as on its surrounding. Then, we followed the control of the nanoparticles size by using mainly optical absorption measurements, which gave us account of the size and the shape of the nanoparticles and the effect of the support on their optical response. These optical results were compared to, and supported with, TEM micrographs of our samples.

Large optical birefringence by anisotropic silver nanocomposites.

A large optical birefringence of oriented Ag nanoellipsoids embedded in silica was measured using an ellipsometric technique. The two main surface plasmon resonances associated with the axes of the ellipsoid were tuned, allowing us to quantify the light transmission through the samples when placed and rotated between crossed and parallel polarizers. This birefringence can be physically associated with the selective optical absorption of one component of the linear polarization of the incident light with respect to the anisotropic axis of the sample, depending on the wavelength used to perform the measurement.