Permanent planar alignment of gas-phase linear molecules is achieved by a pair of delayed perpendicularly polarized short laser pulses. The experiment is performed in a supersonic jet, ensuring a relatively high number density of molecules with moderately low rotational temperature. The effect is optically probed on a femtosecond time scale by the use of a third short pulse, enabling a time-resolved birefringence detection performed successively in two perpendicular planes of the laboratory frame. The technique allows for an unambiguous estimation of the molecular planar delocalization produced within the polarization plane of the pulse pair after the turn-off of the field. The measurements are supported by numerical simulations which lead to the quantification of the observed effect and provide more physical insights into the phenomenon.
We analyze the control of field-free molecular orientation at high temperature by use of a two-color laser bipulse strategy proposed in Zhang et al. [Phys. Rev. A 83, 043410 (2011)]. A general study shows that there exist two types of linear molecules for which a different mechanism has to be used. For molecules with a large hyperpolarizability, a monochromatic laser pre-pulse is applied before the two-color laser pulse at a time close to the rotational period T r , while for molecules with a small hyperpolarizability, the optimal delay is found close to T r /4 or 3T r /4. We extend this analysis to the case of a 2 molecule such as NO where a similar control strategy can be derived. These control processes are robust against temperature effects.
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