Near-resonant optical pumping was used to modulate third-order susceptibility χ(3) in disperse red 1 doped poly(methylmethacrylate) thin films. An optically pumped degenerate four-wave mixing (DFWM) experiment was conducted to examine the photoreactive phase conjugation (PC) signals. Experimental results indicated a large anisotropy in PC signals arising from ∣χ3333(3)∣2, and almost isotropic PC signals from ∣χ1331(3)∣2 under s-polarized and p-polarized pump fields. Additionally, a dynamic microscopic model, based on the theory developed by Sekkat et al.[Synth. Met. 54, 373 (1993); J. Phys. Chem. B 106, 12407 (2002); Opt. Commun. 229, 291 (2004)] was presented to describe the observed optical nonlinear responses. Results from the model were generally consistent with those of the optically pumped DFWM experiment.
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