Third-order nonlinearities of glasses doped with a large number of copper or silver particles are studied by degenerate four-wave mixing with an emphasis on particle-size dependence. The nonlinear susceptibility χ(3) exhibits a peak at the wavelength of the absorption peak, with a maximum value of the order of 10−7 esu. The value of χ(3)/α is roughly independent of the absorption coefficient α and increases as the particle radius increases. This result is well explained by the size dependence of the imaginary part of the dielectric constant of metal particles and the local-field factor. The time response of the nonlinearity exhibits two-component behavior: the fast decay time is shorter than the pulse width of the laser (~12 ps), whereas the slow one is 120–200 ps, being weakly dependent on the radius.
K. Uchida, S. Kaneko, S. Omi, C. Hata, H. Tanji, Y. Asahara, A. J. Ikushima, T. Tokizaki, and A. Nakamura, "Optical nonlinearities of a high concentration of small metal particles dispersed in glass: copper and silver particles," J. Opt. Soc. Am. B 11, 1236-1243 (1994)