Coherent Control About a Conical Intersection

Conical intersections (CIs) are degeneracies between molecular potential energy surfaces that occur in essentially all molecules with more than three atoms. Many studies have established that CIs allow for non-Born-Oppenheimer (non-adiabatic) molecular dynamics. In addition, CIs have many useful attributes for coherent control that have not been fully studied. Here we demonstrate two modes of control around a CI that make use of these properties. The first method uses a continuous light field, resonant absorption, and stimulated emission to control the population on two intersecting electronic states. The second method uses a pulsed light field and the geometric phase accumulated by a wavepacket traversing a CI to control the shape of the wavepacket.