Giant enhanced optical nonlinearity of colloidal nanocrystals with a graded-index host

The effective linear and third-order nonlinear optical properties of metallic colloidal crystal immersed in a graded-index host fluid are investigated theoretically. The local electric fields are extracted self-consistently based on the layer-to-layer interactions, which are readily given by the Lekner summation method. The resultant optical absorption and nonlinearity enhancement show a series of sharp peaks, which merge in a broadened resonant band. The sharp peaks become a continuous band for increasing packing density and number of layers. We believe that the sharp peaks arise from the in-plane dipolar interactions and the surface plasmon resonance, whereas the continuous band is due to the presence of the gradient in the host refractive index. These results have not been observed in homogeneous and randomly-dispersed colloids, and thus would be of great interest in optical nanomaterial engineering.