title: Coupled electronic and structural relaxation pathways in the postexcitation dynamics of Rydberg states of BaArN clusters.
abstract: We investigate, theoretically, the joint relaxation of orbital and structure in postexcitation dynamics of Rydberg states of cluster BaArN (N=250). Mixed quantum-classical dynamics is used to account for the nonadiabatic transitions among more than 160 electronic states, represented via a diatomics-in-molecules Hamiltonian. The simulation illustrates the complex multistep relaxation processes and provides detailed insight in the mechanisms contributing to the final-time experimental photoelectron spectrum.
authors.affiliation: Laboratoire Francis Perrin, CNRS-URA 2453, CEA IRAMIS, Laboratoire Interactions, Dynamique et Lasers, F-91191 Gif-sur-Yvette Cedex, France.
authors.forename: A
authors.initials: A
authors.lastname: Masson
authors.affiliation: Laboratoire de Chimie et de Physique Quantiques/IRSAMC, CNRS and Université de Toulouse (UPS), Université Paul Sabatier, 118 route de Narbonne, F-31062 Toulouse Cedex, France.
authors.forename: M-C
authors.initials: MC
authors.lastname: Heitz
authors.affiliation: Laboratoire Francis Perrin, CNRS-URA 2453, CEA IRAMIS, Laboratoire Interactions, Dynamique et Lasers, F-91191 Gif-sur-Yvette Cedex, France.
authors.forename: J-M
authors.initials: JM
authors.lastname: Mestdagh
authors.affiliation: Laboratoire Francis Perrin, CNRS-URA 2453, CEA IRAMIS, Laboratoire Interactions, Dynamique et Lasers, F-91191 Gif-sur-Yvette Cedex, France.
authors.forename: M-A
authors.initials: MA
authors.lastname: Gaveau
authors.affiliation: Laboratoire Francis Perrin, CNRS-URA 2453, CEA IRAMIS, Laboratoire Interactions, Dynamique et Lasers, F-91191 Gif-sur-Yvette Cedex, France.
authors.forename: L
authors.initials: L
authors.lastname: Poisson
authors.affiliation: Laboratoire de Chimie et de Physique Quantiques/IRSAMC, CNRS and Université de Toulouse (UPS), Université Paul Sabatier, 118 route de Narbonne, F-31062 Toulouse Cedex, France.
authors.forename: F
authors.initials: F
authors.lastname: Spiegelman
mesh_terms: D001128:Argon / Q000737:chemistry*; D017609:Barium Compounds / Q000737:chemistry*; D008962:Models, Theoretical; D055668:Photochemical Processes; D011789:Quantum Theory; D013816:Thermodynamics
chemical_list: D017609:Barium Compounds; D001128:Argon