Photon Driven Charge Transfer Half-Collision: The Photodissociation of CO2.O2+ Cluster Ions with Resolution of the O2 Product Vibrational States

摘要

The photodissociation process is interesting, from a fundamental point of view, because it brings together the distinct but related phenomena of spectroscopy (photon absorption) and dynamics (subsequent dissociation). From a molecular dynamics point of view the dissociation process can be viewed as a half-collision, where the optical absorption process is used to prepare the complex for dissociation. The advantages of this method are first, control of the angular momentum and thus the impact parameter and, second, the collision geometry is defined by the structure of the complex that absorbs the photon. This process is intellectually related to both laser-induced charge exchange and attempts to directly observe properties of transition states of reactions. Both of these areas of research are currently of great interest. In this manuscript we are concerned with charge transfer half-collisions. The process is schematically represented in Fig.1. A loosely bound (A.BC+) complex absorbs a photon and undergoes intramolecular charge transfer to form (A+.BC). Carbon dioxide, Oxygen.