Time-resolved Stark effect in rapidly varying fields

Abstract.

The cycle-averaged ac Stark effect associated with the ^[ A _]2Σ⁺v^′=2?^[ X _]2Π1/2v^′=0 two-photon absorption of NO at intensities between 7.7 and 15.2 TW cm^-2 has been characterized in real time through a synergic combination of bichromatic laser experiments and quantum-dynamics calculations. Measurements of the fluorescence emitted by the Rydberg ^[ A _]2Σ⁺v^′=2 level as a function of time between Stark and probe components of a bichromatic field exhibit a characteristic evolution in temporal peak structure with Stark-field intensity, which is interpreted in terms of a time-dependent Floquet analysis of the laser–matter interaction. The experimental observations are consistent with a dynamic Stark shift of Δε_s(ω₁,ω₂)≤0.23 eV of the optical transition at these intensities.