Abstract
We develop a theoretical model for the nondegenerate nonlinear optical susceptibility of dielectric composite materials containing metal nanoparticles. The model is based on the theory of transient nonlinear response of metal nanoparticles in combination with the effective medium approximation and the discrete dipole approximation. Its validity is confirmed by comparison with a preceding experimental result. Through numerical simulations, we demonstrate that for off-plasmon-resonant pumping the imaginary part of nondegenerate third-order nonlinear susceptibility becomes negative over a wide spectral range of signal. We additionally show the saturation effect of nondegenerate susceptibility depending on pump intensity and wavelength.
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