Three dimensional orientation of small polyatomic molecules excited by two-color femtosecond pulses

Abstract We study the excitation of asymmetric-top (including chiral) molecules by two-color femtosecond laser pulses. In cases non-chiral excited an orthogonally polarized pulse, we demonstrate, classically and quantum mechanically, three-dimensional orientation. For chiral molecules, show that orientation induced a cross-polarized pulse is enantioselective along propagation direction, namely, two enantiomers are oriented in opposite directions. The classical simulations excellent agreement on short time scale, whereas longer exhibits beats. These observations qualitatively explained analyzing interaction potential between molecular (hyper-)polarizability. prospects for using enantiomers’ separation discussed.