Coherent control using kinetic energy and the geometric phase of a conical intersection

Autor: Liekhus-Schmaltz, Chelsea, McCracken, Gregory A., Kaldun, Andreas, Cryan, James P., Bucksbaum, Philip H.
Rok vydání: 2016
Předmět:
Druh dokumentu: Working Paper
DOI: 10.1063/1.4964392
Popis: Conical intersections (CI) between molecular potential energy surfaces with non-vanishing non-adiabatic couplings generally occur in any molecule consisting of at least three atoms. They play a fundamental role in describing the molecular dynamics beyond the Born-Oppenheimer approximation and have been used to understand a large variety of effects, from photofragmentation and isomerization to more exotic applications such as exciton fission in semiconductors. However, few studies have used the features of a CI as a tool for coherent control. Here we demonstrate two modes of control around a conical intersection. The first uses a continuous light field to control the population on the two intersecting electronic states in the vicinity of a CI. The second uses a pulsed light field to control wavepackets that are subjected to the geometric phase shift in transit around a CI. This second technique is likely to be useful for studying the role of nuclear dynamics in electronic coherence phenomena.
Databáze: arXiv