Postpulse molecular alignment measured by a weak field polarization technique

We report a direct nonintrusive observation of alignment and planar delocalization of ${\mathrm{C}\mathrm{O}}_{2}$ after an intense linearly polarized femtosecond laser pulse excitation. The effects are measured by a polarization technique involving a perturbative probe that itself does not induce appreciable alignment. We show that this technique allows one to measure a signal proportional to $⟨{cos}^{2}\ensuremath{\theta}⟩\ensuremath{-}1/3$, with $\ensuremath{\theta}$ the angle between the molecular axis and the laser polarization. Simulations that support this analysis allow one to characterize the experimentally observed alignment and planar delocalization quantitatively.