Monitoring laser driven hydrogen atom motion by transient infrared spectroscopy Original Research Article

Laser control of a hydrogen transfer reaction in a small model system embedded in a condensed phase environment is investigated. The two-dimensional model comprises those features of the multi-dimensional potential energy surface of thioacetylacetone which are most relevant for the isomerization reaction from the enol to the enethiol configuration. The influence of the remaining intramolecular coordinates as well as of a possible environment is described by a spectral density within the reduced density matrix approach. Different forms of the driving infrared laser pulse are explored placing emphasis on their capability for competing successfully with relaxation processes. The reaction dynamics is characterized by calculating the nonlinear optical response nonperturbatively in the driving field.