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Linear and nonlinear optical susceptibilities and hyperpolarizability of borate LiNaB4O7 single crystals: Theory and experiment J. Appl. Phys. 112, 053526 (2012) Effect of Lorentz local field for optical second order nonlinear susceptibility in ZnO nanorod J. Appl. Phys. 111, 103112 (2012) Size dependent optical properties of the CdSe-CdS core-shell quantum dots in the strong confinement regime J. Appl. Phys. 111, 074312 (2012) Structural origin of the nonlinear optical properties of lead niobium germanate film glasses J. Appl. Phys. 110, 023522 (2011) Methyl groups at dielectric and metal surfaces studied by sum-frequency generation in co-and counterpropagating configurations J. Chem. Phys. 135, 044704 (2011) Additional information on J. Appl. Phys.An investigation of Au/SiO 2 composite multilayer films with a large third-order optical nonlinearity is reported in this article. Multilayer films containing Au nanoparticles with narrow size and shape distributions can be obtained by controlling the thickness of the Au layer, as well as the annealing temperature and time duration. It is found that the peak of surface plasmon resonance ͑SPR͒ of films with mean nanoparticle size of 30 nm is located at 2.35 eV with a width of 350 meV. The SPR peak of films containing larger or smaller particles red-shifts and broadens due to the particle size and shape effects. The third-order optical nonlinear susceptibility (3) of these films has a maximum value of about 5.1ϫ10 Ϫ6 esu at 532 nm when the mean nanoparticle size is around 30 nm. We attribute the observed size dependence of (3) to the competition between the enhancement of the local field factor and the skin-depth effect.

Femtosecond pump-probe experiments with a time resolution of 100 fs have been performed for copper particles with a radius of 4 nm. Differential absorption spectra for a pump centered at 2.05 eV indicates the broadening of the absorption band due to the surface plasmon. The nonlinear response time derived from the recovery time of the nonlinear absorption is dependent on the pumping laser fluences, and is as short as 0.7 ps for 210 μJ/cm2. The relaxation dynamics of nonequilibrium electrons can be described by the usual electron-phonon coupling model.

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