1 Department of Chemistry, Technical University of Denmark2 Physical and Biophysical Chemistry, Department of Chemistry, Technical University of Denmark
We consider the rotational excitation of molecules induced by asymmetric (“half-cycle”) as well as symmetric single-cycle THz pulses, leading to field-free time-dependent orientation. We show that the basic excitation mechanisms are very similar for the two types of pulses; i.e., the frequency distributions of the pulses at the rotational resonance frequencies play an important role. Furthermore, we investigate the interference between multiple rotational excitation pathways following prealignment with a nonresonant 800-nm femtosecond pulse. It is shown that such interference can lead to an enhancement of the orientation of the linear HCN molecule by a factor close to 2.
Physical Review a (atomic, Molecular and Optical Physics), 2013, Vol 87, Issue 1