Abstract

Near-resonant optical pumping is applied for encoding the anisotropy of third-order susceptibility ${\chi }^{(3)}$ in a Disperse Red 1 poly (methyl methacrylate) polymer thin film. The encoding process involves one- or two-photon excitation that results in trans–cis isomerization of azo molecules. Third-harmonic generation from the sample is used to probe the ${\chi }^{(3)}$ anisotropy. We demonstrate large reversible variations of the third-harmonic generation (several times in intensity) in a sample pumped by the second harmonic of a Nd:YAG laser or a cw He–Cd laser. A microscopic model, which includes mechanisms for angular hole burning and molecular reorientation, is presented. The model is in good qualitative agreement with the experimental results.

© 2001 Optical Society of America

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