Abstract
In this paper we report femtosecond studies of the influence of rare-gas collisions on the dissociation reaction of NaI molecules by investigating the coherent wave packet motion in NaI at a temperature of 670 °C and rare-gas pressures ranging from 0 to 1000 bar. The photodissociation dynamics of NaI is influenced by the interaction between the excited covalent and the ionic ground state potential energy surfaces, which cross at a certain internuclear separation. Due to the adiabaticity of the so formed potential, studies of the elementary nuclear motion and reaction dynamics along the covalent (Na + I) and the ionic (Na+ + I-) channels are possible. The probing is made for the transition-state complex [Na···I]⧧*. Even at low rare-gas pressures a considerable influence of collisions on the wave packet motion within the adiabatic potential well is found. Only few collisions between NaI molecules and surrounding rare-gas atoms result in fast vibrational relaxation and loss of coherence. Furthermore, a stabi...
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