We report an experimental study of the control of molecular alignment of ${\mathrm{N}}_2$ by use of spectrally modulated pulses at an intensity regime below the intrinsic saturation of the alignment. By manipulating the relative timing of the alignment revival pattern arising from the even subset of the thermal ensemble as compared to the odd subset, we demonstrate that the angular distribution of the aligned molecule can be converted into planar delocalization at specific times. We also show that the angular focusing of the molecular axis can be switched off by applying a specific bipulse.

• Received 5 May 2004

DOI:https://doi.org/10.1103/PhysRevA.72.025401