Abstract
Multiphoton excitation and dissociation of DN3 by short CO2 laser pulses is shown to be a collisionless process. The characteristic features of this multiphoton process are systematically studied. The average number of photons absorbed per DN3 molecule and the absolute dissociation yield show a strong dependence on the peak laser intensity. Resonantly enhanced coherent multiphoton excitation, rather than stepwise incoherent excitation, is suggested. The primary dissociation products of DN3 are ND[1Δ] and N2. Formation of vibrationally excited ND[1Δ] intermediates is suggested. The reactions of ND[1Δ] with DN3 lead to chemiluminescent signals originating from the formation of electronically excited ND2[2A1] and ND[3Π]. Formation of the ND[3Π] intermediate is attributed to a reaction of ND[1Δ] and vibrationally excited DN*3 molecules: ND[1Δ]+DN*3→ND[3Π]+ND[3Σ−]+N2.
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