title: Quasi-classical statistico-dynamical description of polyatomic photo-dissociations: state-resolved distributions.
abstract: An alternative methodology to investigate indirect polyatomic processes with quasi-classical trajectories is proposed, which effectively avoids any binning or weighting procedure while provides rovibrational resolution. Initial classical states are started in terms of angle-action variables to closely match the quantum experimental conditions and later transformed into Cartesian coordinates, following an algorithm very recently published [J. Chem. Phys. 2009, 130, 114103]. Trajectories are then propagated using the 'association' picture, i.e. an inverse dynamics simulation in the spirit of the exit-channel corrected phase space theory of Hamilton and Brumer [J. Chem. Phys. 1985, 82, 595], which is shown to be particularly convenient. Finally, an approximate quasi-classical formula is provided which under general conditions can be used to add possible rotational structures into the vibrationally-resolved quasi-classical distributions. To introduce the method and illustrate its capabilities, correlated translational energy distributions from recent experiments in the photo-dissociation of ketene at 308 nm [J. Chem. Phys. 2006, 124, 014303] are investigated. Quite generally, the overall theoretical algorithm reduces the total number of trajectories to integrate and allows for fully theoretical predictions of experiments on polyatomics.
authors.affiliation: Departamento de Física General, Instituto Superior de Tecnologías y Ciencias Aplicadas, Habana 6163, Cuba. mleo@instec.cu
authors.forename: Maykel Leonardo
authors.initials: ML
authors.lastname: González-Martínez
authors.forename: Laurent
authors.initials: L
authors.lastname: Bonnet
authors.forename: Pascal
authors.initials: P
authors.lastname: Larrégaray
authors.forename: Jean-Claude
authors.initials: JC
authors.lastname: Rayez