title: Assessment of DFT Exchange-Correlation Functionals for Evaluating the Multipolar Contributions to the Quadratic Nonlinear Optical Responses of Small Reference Molecules.
abstract: The hyper-Rayleigh scattering responses as well as the multipolar contributions to the first hyperpolarizabilities are calculated by means of density functional theory for a series of reference molecules (acetonitrile, dichloromethane, trichloroacetonitrile, chloroform, carbon tetrachloride), covering the whole range of dipolar/octupolar character. The performance of various exchange-correlation functionals is addressed by comparison to CCSD(T) calculations. The best functionals turn out to be LC-BLYP, M05-2X, and M06-2X.
authors.affiliation: Institut des Sciences Moléculaires (ISM), Université de Bordeaux , UMR 5255 CNRS, Cours de la Libération, 351, F-33405 Talence, France.
authors.forename: Frédéric
authors.initials: F
authors.lastname: Castet
authors.affiliation: Laboratoire de Chimie Théorique, UCPTS, Facultés Universitaires Notre-Dame de la Paix (FUNDP) , rue de Bruxelles 61, B-5000 Namur, Belgium.
authors.forename: Benoît
authors.initials: B
authors.lastname: Champagne