Non linear effects in the interaction of time-dependent fields and chiral systems. A computational investigation

The nonlinear changes induced in the refractive index and in the optical rotatory dispersion when radiation interacts with a chiral system are studied computationally. The molecular parameters describing these effects are determined for methyloxirane, employing Hartree-Fock and density functional frequency dependent analytical response theory, the latter with the use of Becke three-parameter Lee-Yang-Parr functional. Their contribution to several circular and axial birefringences, which could be observed in pump-and-probe experiments for various combinations of polarization status and propagation direction of the two beams, is ascertained.