title: Accurate modeling of infrared multiple photon dissociation spectra: the dynamical role of anharmonicities.
abstract: The dynamical response of a molecular system to a macropulse typically produced by a free-electron laser is theoretically modeled over experimentally long times, within a realistic kinetic Monte Carlo framework that incorporates absorption, stimulated emission, spontaneous emission, and dissociation events. The simulation relies on an anharmonic potential energy surface obtained from quantum chemistry calculations. Application to cationic naphthalene yields a better agreement with measurements than the anharmonic linear absorption spectrum, thus emphasizing the importance of specific dynamical effects on the spectral properties.
authors.affiliation: Institut des Sciences Moléculaires d'Orsay, UMR CNRS 8214, Université Paris Sud 11, Bât. 210, F91405 Orsay Cedex, France. pascal.parneix@u-psud.fr
authors.forename: Pascal
authors.initials: P
authors.lastname: Parneix
authors.forename: Marie
authors.initials: M
authors.lastname: Basire
authors.forename: Florent
authors.initials: F
authors.lastname: Calvo