Nonadiabatic alignment of symmetric top molecules induced by a linearly polarized, moderately intense picosecond laser pulse is studied theoretically and experimentally. Our studies are based on the combination of a nonperturbative solution of the Schrödinger equation with femtosecond time-resolved photofragment imaging. Using methyliodide and tert-butyliodide as examples, we calculate and measure the alignment dynamics, focusing on the temporal structure and intensity of the revival patterns, including their dependence on the pulse duration, and their behavior at long times, where centrifugal distortion effects become important. Very good agreement is found between the experimental and numerical results. This allows us to use our theory and numerical results to provide additional insight into the origin of the experimental findings.

• Received 21 July 2005

DOI:https://doi.org/10.1103/PhysRevA.72.043402