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All-optical control of the noncentrosymmetry of azodye-doped polymer films was demonstrated by nonresonant dual-frequency coherent excitation. Three kinds of noncentrosymmetries of the polymer films were optically tailored using appropriate combinations of the writing beam polarizations, linearly polarized, and circularly polarized light. The tensor analysis of the photoinduced noncentrosymmetry was performed by monitoring second harmonic generation (SHG) of the samples. The quadratic dependence of SHG on film thickness was observed, indicating that a χ(2) grating satisfying the phase-matching condition for SHG was optically induced in the polymer films and that this nonresonant all-optical poling can be used to tailor the symmetry of bulk samples.

Control of the noncentrosymmetry of thick polymer films by nonresonant all-optical poling