Principles of enantio-selective excitation in three-wave mixing spectroscopy of chiral molecules

Three-wave mixing spectroscopy of chiral molecules, which exist in left-handed and right-handed conformations, allows for enantioselective population transfer despite random orientation of the molecules. This is based on constructive interference of the three-photon pathways for one enantiomer and the destructive one for the other. We prove here that three mutually orthogonal polarization directions are required to this end. Two different...