Anomalous Rabi Oscillations in Multilevel Quantum Systems.

We show that the excitation probability of a state within a manifold of levels undergoes Rabi oscillations with the frequency determined by the energy difference between the states and not by the pulse area, for sufficiently strong pulses. The population and coherence remains in the two-level subsystem formed by the initial and target state even at Rabi frequencies exceeding the energy difference. The observed dynamics can be useful in nonlinear spectroscopy and quantum state preparation.

Control of ultrafast molecular photodissociation by laser-field-induced potentials.

Experiments aimed at understanding ultrafast molecular processes are now routine, and the notion that external laser fields can constitute an additional reagent is also well established. The possibility of externally controlling a reaction with radiation increases immensely when its intensity is sufficiently high to distort the potential energy surfaces at which chemists conceptualize reactions take place. Here we explore the transition from the weak- to the strong-field regimes of laser control for the dissociation of a polyatomic molecule, methyl iodide. The control over the yield of the photodissociation reaction proceeds through the creation of a light-induced conical intersection. The control of the velocity of the product fragments requires external fields with both high intensities and short durations. This is because the mechanism by which control is exerted involves modulating the potentials around the light-induced conical intersection, that is, creating light-induced potentials.