Quantum calculation of the second-order hyperpolarizability of chiral molecules in the "one-electron" model
Résumé
Quantum calculation of the hyperpolarizabilty tensor is carried out for chiral molecules displaying a "one-electron" chirality. Calculation is made possible by introducing a chiral perturbation term in the potential energy surface. We show that a one-electron chiral molecule is intrinsically nonlinear and diplays a nonzero electric chiral hyperpolarizability. Existence of magnetic contributions is discussed, and it is shown that higherorder perturbation terms are necessary to introduce such magnetic effects in the second-order hyperpolarizability. Cop. 2010 American Chemical Society.