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Abstract: Two-photon absorption and photoinduced anistropy of a methyl orange/Au nanoparticles composite system were investigated. Open aperture Z-scan measurements demonstrated that the absorption cross section of methyl orange in an Au colloid solution can increase 42-fold compared to purified that of a methyl orange aqueous solution. Meanwhile, a 2.6-fold enhancement of the photoinduced birefringence of methyl orange in the presence of Au was also observed. The mechanism accounting for the enhancement of two-photon absorption coefficient and photoinduced birefringence was discussed in terms of the localized field effect via surface plasmon resonance of Au nanoparticles, which was further confirmed using the fluorescence spectrum technique. [Copyright &y& Elsevier]