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| - Investigation of Ion−Molecule Reactions via Femtosecond Excitation and Ionization of[Tetrakis(dimethylamino)ethylene]n≥1
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| - The dynamics of ionic monomer and multimers of the ethylenic molecule TDMAE (tetrakis(dimethylamino)ethylene) have been studied under femtosecond stepwise excitation using an energy surface of the neutralmolecule (or cluster) as a relay. This specific excitation takes advantage of the wave packet evolution in theneutral intermediate state to (i) allow access to different regions of the ionic potential surface and (ii) identifysome aspects of the dynamics in the ionic state of either TDMAE+ or TDMAEn+. This original experimentalapproach we shall name double pump excitation. We have identified the existence of a double well in TDMAEn+corresponding to a different localization of the positive charge, the most stable corresponding to a completedelocalization over the nitrogen atoms. A reaction in the dimer and higher multimer ions is observed thatinvolves the formation of compounds of general mass 200m116n+. This reaction is only observed in clustersand not in thermal ion molecule collisions between TDMAE+ and TDMAE. A tentative mechanism of formationfor this product is proposed that involves the creation of a distonic ion via H-atom migrations. The doublepump method could be extended to many other systems to explore competing pathways in ionic reactions,differently accessed via transient states of a neutral intermediate.
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