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Molecular chlorine was photolyzed using circularly polarized radiation at 310 and 330 nm, and orientation moments of the chlorine-atom Cl(2Pj) photofragment distributions were measured by resonance enhanced multiphoton ionization using circularly polarized light with Doppler resolution. The product atoms were found to be strongly oriented in the laboratory as a result of both incoherent and coherent dissociation mechanisms, and the orientation moments contributed by each of these mechanisms have been separately measured. The experimental results can be explained by nonadiabatic transitions from the C 1Π1u state to higher states of Ω=1u symmetry, induced by radial derivative coupling. Ab initio calculations indicate strong Rosen–Zener–Demkov noncrossing-type radial derivative couplings between states of 1u symmetry. The observed angular distribution (β parameter) indicates that 88% of Cl*(2P1/2) fragments produced at 310 nm originate from a perpendicular transition to the C state. The orientation measureme...

Oriented chlorine atoms as a probe of the nonadiabatic photodissociation dynamics of molecular chlorine