Postpulse molecular alignment measured by a weak field polarization technique -: art. no. 153601

We report a direct nonintrusive observation of alignment and planar delocalization of CO2 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)theta] - 1/3, with 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.