Nonlinear optical properties and surface-plasmon enhanced optical limiting in Ag-Cu nanoclusters co-doped in SiO2 sol-gel films

The nonlinear optical properties and the role of the surface-plasmon resonance (SPR) on optical limiting (OL) properties of Ag-Cu nanoclusters co-doped in SiO2 matrix prepared using the sol-gel technique with a Cu/Ag molar ratio of 1, 2 and 3, respectively, are presented. The studies were made using the second harmonic of high-power nanosecond and picosecond Nd:YAG lasers. These films show a self-defocusing nonlinearity with both nanosecond and picosecond pulses and a good nonlinear absorption behavior with the nanosecond pulse excitation. The nonlinear refractive index decreased with decreasing particle size, whereas the nonlinear absorption increased with an increase in Cu concentration. The observed nonlinear absorption is explained by taking into account the cumulative effect of both the intraband and interband mechanisms. The excitation near the SPR of Cu resulted in an enhanced OL behavior with increasing Cu concentration. No such concentration dependence is observed when the excitation is near the SPR of Ag, however, the limiting threshold is reduced approximately 10-17 times. Excitation at wavelengths far below the SPR of Ag and Cu has not shown any OL behavior. The major contribution toward OL is observed to be from the interband absorption and from a possible energy transfer within the higher unoccupied states of Cu and Ag. Although nonlinear scattering is observed at higher intensities, its contribution is found to be much less than that of the nonlinear absorption assisted by an energy transfer. (C) 2004 American Institute of Physics.