Identification of the alignment of azobenzene molecules induced by all-optical poling in polymer film

The alignment of azobenzene molecules in DR19-PUI film induced by all-optical poling is identified. When the writing beams of frequencies ω and 2ω are both linearly polarized with their polarization directions parallel to each other, azobenzene molecules tend to reorient to perpendicular direction (i.e. direction perpendicular to the polarization of writing beams). At the end of the writing process more molecules orient in perpendicular direction than those in parallel direction (i.e. direction parallel to the polarization of writing beams). The alignment of molecules in parallel or perpendicular direction is, respectively, characteristic of noncentrosymmetry or centrosymmetry. It is the alignment of molecules in parallel direction that results in the second-order nonlinearity in the poled film.