1 Department of Chemistry, Technical University of Denmark2 Physical and Biophysical Chemistry, Department of Chemistry, Technical University of Denmark
We consider a phaselocked two-pulse sequence applied to photofragmentation in the weak-field limit. The two pulses are not overlapping in time, i.e., the energy of the pulse-train is constant for all time delays. It is shown that the relative yield of excited Br* in the nonadiabatic process: I + Br*←IBr → I + Br, changes as a function of time delay when the two excited wave packets interfere. The underlying mechanisms are analyzed and the change in the branching ratio as a function of time delay is only a reflection of a changing frequency distribution of the pulse train; the branching ratio does not depend on the detailed pulse shape.
Journal of Chemical Physics, 2014, Vol 141, Issue 20