Coherent population dynamics of a three-level atom in spacetime

Abstract

This work explores temporal and spatial aspects of coherent population transfer in a three-level atom through a synergic combination of experimental measurements and theoretical calculations. Experimental measurements exploit the broad bandwidth of a femtosecond laser pulse to initiate simultaneous excitation of the $5p{}^{2}{P}_{1/2}\ensuremath{\leftarrow}5s{}^{2}{S}_{1/2}$ and $5p{}^{2}{P}_{3/2}\ensuremath{\leftarrow}5s{}^{2}{S}_{1/2}$ components of the doublet line of atomic rubidium. By adjusting positive or negative frequency sweeps the pump pulse favors either one of the two transitions and eventually even decouples the two excited states. The population of the excited spin-orbit levels is monitored in real time by stimulated emission probing under conditions of different intensity, chirp, and pulse width of the driving field, giving detailed information on the coupling between the three levels and their interactions with the driving and probe fields at different points in spacetime. Both pump and probe pulses are carefully characterized after the interaction region by frequency-resolved optical gating. In order to interpret and understand the experimental results it is essential to consider the close relationship between pulse propagation and time evolution of the atomic system via the coupled Maxwell-Bloch equations. This analysis highlights the importance of spatial propagation of the light fields, as well as their temporal dependence, in understanding the dynamical population evolution, and quantitatively reproduces all aspects of the experimental measurements.