Abstract

The transient polar orientation of a solution of the octupolar molecule ethyl violet is achieved by optical means in an experimental geometry of phase conjugation. The corresponding resonant six-wave mixing process is described in terms of anisotropic nonlinear absorption. Orientation results from the consistent octupolar symmetry of both the molecular species and the orienting field tensor. The 26 ps decay time of the induced non-centrosymmetry is limited by electronic excitation relaxation. A 510×10 −30 esu second-harmonic hyperpolarizability at 1064 nm fundamental wavelength with 13 D transition dipole moment between excited states is inferred. Octupolar nature of the hyperpolarizability tensor symmetry is verified by polarization analysis of the induced second-harmonic susceptibility components.

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