Dissociative ionization of neon clusters Ne[sub n], n=3 to 14: A realistic multisurface dynamical study - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Journal of Chemical Physics Année : 2005

Dissociative ionization of neon clusters Ne[sub n], n=3 to 14: A realistic multisurface dynamical study

David Bonhommeau
Alexandra Viel

Résumé

The molecular dynamics with quantum transitions (MDQT) method is applied to study the fragmentation dynamics of neon clusters following vertical ionization of neutral clusters with 3 to 14 atoms. The motion of the neon atoms is treated classically, while transitions between the adiabatic electronic states of the ionic clusters are treated quantum mechanically. The potential energy surfaces are described by the diatomics-in-molecules model in a minimal basis set consisting of the effective 2p2p orbitals on each neon atom for the missing electron. The fragmentation mechanism is found to be rather explosive, with a large number of events where several atoms simultaneously dissociate. This is in contrast with evaporative atom by atom fragmentation. The dynamics are highly nonadiabatic, especially at shorter times and for the larger clusters. Initial excitation of the neutral clusters does not affect the fragmentation pattern. The influence of spin-orbit coupling is also examined and found to be small, except for the smaller size systems for which the proportion of the Ne+ fragment is increased up to 43%. From the methodological point of view, most of the usual momentum adjustment methods at hopping events are shown to induce nonconservation of the total nuclear angular momentum because of the nonzero electronic to rotation coupling in these systems. A new method for separating out this coupling and enforcing the conservation of the total nuclear momentum is proposed. It is applied here to the MDQT method of Tully but it is very general and can be applied to other surface hopping methods.

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hal-01118371 , version 1 (10-07-2017)

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David Bonhommeau, Alexandra Viel, Nadine Halberstadt. Dissociative ionization of neon clusters Ne[sub n], n=3 to 14: A realistic multisurface dynamical study. Journal of Chemical Physics, 2005, 123 (5), pp.054316. ⟨10.1063/1.1953530⟩. ⟨hal-01118371⟩
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