Vibrationally selective optimal control of alignment and orientation using infrared laser pulses: application to carbon monoxide.
Optimal control methods are used to study molecular alignment and orientation using infrared laser pulses. High order molecule-field interactions are taken into account through the use of the electric-nuclear Born-Oppenheimer approximation [G. G. Balint-Kurti et al., J. Chem. Phys. 122, 084110 (2005)]. High degrees of alignment and orientation are achieved by optimized infrared laser pulses of duration on the order of one rotational period of the molecule. It is shown that, through the incorporation of a vibrational projection operator into the optimization procedure, it is possible not only to maximize the alignment and orientation but also to bring the whole system into a single prescribed vibrational manifold. Numerical calculations are performed for carbon monoxide using ab initio potential energies computed in the presence of external electric fields.
School of Chemistry, University of Bristol, Bristol BS8 1TS, United Kingdom. shiyang.zou@bristol.ac.uk
Shiyang
S
Zou
Gabriel G
GG
Balint-Kurti
Frederick R
FR
Manby