Theory of "laser distillation" of enantiomers: Purification of a racemic mixture of randomly oriented dimethylallene in a collisional environment

Enantiomeric control of 1,3 dimethylallene in a collisional environment is examined. Specifically, our previous '' laser distillation '' scenario wherein three perpendicular linearly polarized light fields are applied to excite a set of vib-rotational eigenstates of a randomly oriented sample is considered. The addition of internal conversion, dissociation, decoherence, and collisional relaxation mimics experimental conditions and molecular decay processes. Of greatest relevance is internal conversion which, in the case of dimethylallene, is followed by molecular dissociation. For various rates of internal conversion, enantiomeric control is maintained in this scenario by a delicate balance between collisional relaxation of excited dimethylallene that enhances control and collisional dephasing, which diminishes control. (c) 2006 American Institute of Physics.