Coherent control of the optical nonlinear and luminescence anisotropies in molecular thin films by multiphoton excitations

Photoinduced orientational distributions are implemented with one- and two-photon absorption interference in polymer films containing chromophores that exhibit luminescent and nonlinear properties. The odd- and even-order parameters of the final distribution are probed by simultaneous measurement of second-harmonic generation (SHG) and two-photon fluorescence (TPF). We show the possibility of engineering local SHG and TPF anisotropies by controlling the polarization states and intensities of the writing optical fields. Complex multipolar orders are modeled with an irreducible spherical tensor-based formalism jointly applied to the molecular polarizabilities and field tensors.