We experimentally explore the dynamics of photo-induced or collision-induced unimolecular decomposition of molecules and radicals in the gas-phase. We probe the dynamics of bond fission processes in competition with isomerization reactions using time- and frequency-resolved spectroscopic techniques. We learn about the fate of highly energized molecules and radicals and gain detailed insight into the mechanisms and pathways the parent species chooses to sample on complex multidimensional potential energy surfaces prior to dissociation.

See our recent articles in Chem. Commun. and Phys. Chem. Chem. Phys.

We experimentally investigate the vibronic structure of small hydrocarbon radicals using frequency-resolved laser spectroscopy. Together with predictions from high-level ab initio calculations we learn about the interactions between valence and Rydberg electronically excited states in open-shell species and the mechanism of their photoionization dynamics. The experimental observations also provides detailed information of the electronic and vibrational spectra of open-shell systems needed for benchmark studies of new ab initio methods.

Read our recent articles in J. Phys. Chem. A and in J. Mol. Spectrosc.

Computational Chemisty and Theory

We extensively explore the complex potential energy surfaces in the electronic ground state of (open-shell) species using both density functional and high-level multireference ab initio methods to predict their products and the likely dissociation pathways. Large scale ab initio direct dynamics simulations provides insight in the competition between adiabatic and non-adiabatic pathways in dissociation of small hydrocarbon radicals mediated by conical intersections. Semiclassical trajectory surface hopping simulations also provide unique insight at the atomistic level into the mechanism of non-radiative decay following photo-excitation and the dynamics near seams of conical intersections.

Check out our recent papers in Phys. Chem. Chem. Phys. and J. Chem. Phys.