We demonstrate the possibility of controlling the symmetry properties of photoinduced macroscopic susceptibility in polymer films. Ellipsometric adjustment of the write beams allows one to monitor the macroscopic symmetry from a dipolar to an octupolar configuration. Experimental results are in agreement with an irreducible spherical tensor-based model jointly applied to the molecular hyperpolarizability and field tensors. We found a purely octupolar polarization-independent photoinduced second-harmonic-generation response in a Dispersed Red 1–methyl methacrylate thin film. Such a configuration, as generated by an octupolar tensor write field tensor made up of counterclockwise circularly polarized and beams, is not within the reach of the classical electric-field poling technique.
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