Abstract
Near-resonant optical pumping is used to encode an anisotropy of third-order susceptibility χ (3) in azo-dye doped polymethylmethacrylate thin films. The χ (3)-anisotropy is probed with two nonlinear techniques: third harmonic generation (THG) and nonlinear transmission (NLT). Using the NLT technique, the photoisomerization-induced change of the imaginary part of χ (3) is probed. A dynamic microscopic model of the third-order nonlinearity behavior based on angular hole burning and angular redistribution mechanisms of the photoisomerization effect is presented to describe the observed optical nonlinear responses. Results from the model are generally consistent with optically pumped THG and NLT experiments.
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