Orateur
Description
Experimental evidence for long-range electron transfer in alkali
clusters interacting with fullerene-doped helium nanodroplets was
reported by the Scheier group. Such reactions are hindered by the very
different propensities of the two reaction partners towards
solubility, alkalis being heliophobic while fullerenes are
heliophilic.
In this contribution, we present a preliminary investigation of a
similar chemical situation, namely the formation of the ionic bond in
NaCl from the two initially distant neutral partners, by means of
semiclassical computational modeling. Our approach relies on
ring-polymer molecular dynamics simulations, that take into account
vibrational delocalization but ignore the superfluid character. A
reactive potential energy surface is designed from empirical
valence-bond theory, both neutral and ionic states being dressed by
the helium solvent with appropriate polarization forces for the ionic
state.
Two conditions were considered for triggering the reaction, either
through an adiabatic collision between one isolated parner and the
solvated, other partner, or the progressive shrinking of the droplet
by solvent evaporation. In both cases, nuclear delocalization is found
to influence not only the solvent itself, but also the NaCl solute
upon its formation.
| Affiliation de l'auteur principal | Laboratoire Interdisciplinaire de Physique |
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