Rates and Recurrences in Quasicontinuum Photoexcitation

The photoexcitation of a quasicontinuum of atomic or molecular levels by a laser pulse with a fast rise-time is considered. We first generalize non-perturbative treatments of quasicontinuum excitation. A second general theoretical method is developed in which resonant states are considered non-perturbatively whereas background non-resonant states are included through a perturbative approximation. As a simple example we show how our method describes the photoexcitation of a quasicontinuum of equally spaced levels, exhibiting Rabi oscillations periodically perturbed by background states. We then examine the case of a Rydberg series of highly excited states coherently excited from a low-lying initial state. The time evolution of the coherent superposition of Rydberg levels is shown to be a perturbed Rabi oscillation, but without the periodic disruption of the equally spaced quasicontinuum. Finally, we include the effect of further excitation to a second continuum.