Abstract
Sequential two photon studies of Xe:Cl2 complexes in liquid Ar are reported. The first photon prepares the excited state complex Xe:Cl2(3Πu), which radiatively relaxes with a lifetime of 10±1 μs (22±2 μs for the uncomplexed Cl2(3Πu)). A second photon accesses either the molecular ion pair state, Xe:Cl+Cl−, or the contact charge transfer transition, Xe+Cl−2. The latter dissociates to Xe+Cl−+Cl even though the product is formed at threshold. The former undergoes charge rearrangement and decays radiatively via Xe+Cl−2 (2Σu)→XeCl2(1Σg). Analysis of the excitation and emission spectra of the key intermediate in laser induced harpoon reactions, Xe+Cl−2, leads to the conclusions that the complex is linear in both ionic and neutral states, and allows a direct contrast between dissociation dynamics on ionic versus neutral surfaces.
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