Volume 127, Issue 5, 07 August 2007
Index of content:
127(2007); http://dx.doi.org/10.1063/1.2769633View Description Hide Description
We report experimental evidence for molecular deformation due to a vibrationally active transition state of multiply charged acetylene molecules under the impact of low energy projectiles. “Butterflylike” structures are observed in the experimental coincidence spectra between hydrogen and carbon ionic fragments. Such structures can be generated by numerical simulations and are found to originate from the bending motion of the dissociating molecule. Angular distributions for dissociation products from triply charged ion are reported.
Hybrid approach for free energy calculations with high-level methods: Application to the reaction of and in water127(2007); http://dx.doi.org/10.1063/1.2768343View Description Hide Description
We present an approach to calculate the free energy profile along a condensed-phase reaction path based on high-level electronic structure methods for the reactive region. The bulk of statistical averaging is shifted toward less expensive descriptions by using a hierarchy of representations that includes molecular mechanics, density functional theory, and coupled clustertheories. As an application of this approach we study the reaction of with in aqueous solution.