화학공학소재연구정보센터
Journal of Physical Chemistry A, Vol.107, No.40, 8259-8270, 2003
Controlling non-Franck-Condon transitions: Counterintuitive schemes of population transfer in the adiabatic and strong adiabatic regimes
Vibrationally selective population transfer in electronic transitions involving small Franck-Condon factors is studied by means of two-photon excitation with pulse sequences applied in counterintutive order. Depending on the intensity of the pulses, two schemes allow ultrafast adiabatic passage. Both schemes, called STIRAP and APLIP, are analyzed as a function of the geometry of the electronic states and of the time duration and intensity of the pulses that drive the transitions. Although both schemes imply adiabatic following, the APLIP scheme requires pulses of considerably larger intensity than STIRAP, hence operating in a strong adiabatic regime. Simple adiabatic criteria for high-quality transfer are proposed, and analytic proofs are provided that show under which conditions STIRAP and APLIP converge. The results of this paper are illustrated with numerical simulations for two different electronic transitions in the Na-2 molecule.