Computational implementation of the hyper-Rayleigh scattering optical activity: theory, symmetry considerations and quantum chemistry applications

We performed the first computational implementation of the hyper-Rayleigh scattering optical activity (HRS-OA) spectroscopy, a nonlinear chiroptical method theoretically predicted by D. Andrews and T. Thirunamanchandran in 1979 [1]. Recent experiments on silver nanohelices and on molecular oligoamide foldamers confirmed this chiroptical phenomenon [2, 3]. Moreover, the measured circular differential scattering ratios make the HRS-OA a promising method for application in chiral discrimination problems due to its high sensitivity compared to other linear chiroptical methods like electronic circular dichroism.