Real-time probing of reactions in clusters

Abstract

In this Communication we report our first study of real-time reaction dynamics in finite size clusters. The reaction is of the type AH + Sn, where the proton transfer (bimolecular) dynamics is examined as the acid AH is solvated with different number of molecules, n = 1,2,... etc. This is in continuation of out effort to study reaction dynamics in real-time [1], but now extending the scope of the previous collisionless (solvent free) condition to a range where condensed phase effects can play a role. Of particular interest to us is the condition at which solvation induces vibrational relaxation and modifies IVR. Real-time studies of reactions in clusters offer great opportunities for obtaining the rates directly [2] and for examining these solvation processes under controlled conditions in molecular beams. Such stepwise solvation by beam methods has been advanced for a variety of systems spanning small molecules [3], large molecules [4], hydrogen-bonded systems [5], and electrons [6].