title: Multiconfiguration time-dependent Hartree and classical dynamics studies of the photodissociation of HF and HCl molecules adsorbed on ice: extension to three dimensions.
abstract: The 3D photodissociation dynamics of HCl and HF molecules adsorbed on ice is studied by quantum and classical simulations. The quantum calculations are carried out with the multiconfiguration time-dependent Hartree (MCTDH) approach. Dynamical observables like angular distributions in the momentum space of the H fragments, absorption cross sections are computed. The results are compared with our previous 2D studies. As expected, less encapsulation of the H atom between the ice surface and the halogen atom is obtained in the 3D study, resulting in less pronounced interference structures in the photoabsorption cross sections and in a decrease of the classical rainbow peaks observed in the 2D scheme. Although the amplitudes of the oscillations corresponding to quantum interferences in the asymptotic angular distribution of the H fragment are different between the 2D and 3D results, the qualitative pattern of the oscillations is similar in the 2D and 3D approaches. In addition, a good agreement is observed for the angular distribution between the classical and the quantum calculations.
authors.affiliation: Leiden Institute of Chemistry, Gorlaeus Laboratories, Leiden University, P.O. Box 9502, 2300 RA Leiden, The Netherlands.
authors.forename: S
authors.initials: S
authors.lastname: Woittequand
authors.forename: C
authors.initials: C
authors.lastname: Toubin
authors.forename: M
authors.initials: M
authors.lastname: Monnerville
authors.forename: S
authors.initials: S
authors.lastname: Briquez
authors.forename: B
authors.initials: B
authors.lastname: Pouilly
authors.forename: H-D
authors.initials: HD
authors.lastname: Meyer