Abstract

By applying the Maxwell Garnett model to gold nanoparticles in water we deduce a value of Im χi(3)=1.1 ×10-7 esu for the imaginary part of the cubic susceptibility for gold corresponding to a Fermi smearing mechanism. We also demonstrate a sign reversal in the nonlinear absorption for gold particles in 1, 1, 3, 3, 3, 3-hexamethylindotricarbocyanine iodide. Although the imaginary part of χ(3) is positive for each component by itself, remarkably the imaginary part of χ(3) is negative for the colloid as a whole. We show that the nonlinearity of the host must be considered and that the sign reversal in χ(3) is a result of the fact that at the surface plasmon resonance the local field factor has an imaginary component that arises from a phase shift between the applied field and the local field inside the particle.

© 1997 Optical Society of America

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