Our group's research unifies themes in catalysis, biology, and molecular clusters.
The central tenet of our work is that the inherent coupling between electronic
and nuclear motion drives the chemistry of these systems. In fact, while all
bond-breaking and -making chemistry involves the rearrangement of electrons and nuclei, we focus
on systems in which electrons themselves serve as a driving force for chemistry.
The unifying theme among these seemingly disparate systems is shown in the following
diagram. In each case, attachment of an electron (or flipping of a redox state) stabilizes
otherwise-inaccessible
products and induces proton transfer. The source of the electron is the primary distinction
among these sytems. The crucial factors still missing, however, are the details
of the electron's influence in the molecular orbital framework—i.e., what drives the
chemistry—and the dynamical manner in which the electron and proton motion are coupled.
The simulation of such systems is difficult because both the electronic and nuclear states/motion can be highly quantum mechanical. For proton transfer and proton-coupled electron transfer, in particular, quantum mechanical treatments of both halves of the problem are required for even a qualitatively correct understanding of the system. Therefore, our group develops theoretical and computational methods that apply quantum mechanics to both the electrons and nuclei. In particular, we develop methods at the interface of ab initio electronic structure theory and nuclear methods, where a dearth of methods currently exists.