Cooperative behavior among three-level systems: Transient effects of coherent optical pumping

Abstract

The dynamical evolution of an excited-state population in a macroscopic volume of three-level molecules is considered where the population is driven optically between the initial ground state and the excited states by an externally applied ($c$-number) coherent pump. The intermediate and ground states are taken as nonradiatively coupled whereas the excited-to-intermediate-state transition is coupled to the radiation field which is treated quantum mechanically. It is found that stimulated Raman processes can significantly influence the dynamical evolution of population inversion and macroscopic polarization by producing coherence effects among the populations. We examine the evolution of collective relaxation between the excited and intermediate levels in the time regime of the pump pulse duration. It is shown, using the mean-field approximation, that for uniform pumping and conditions such that the pump Rabi rate ${\ensuremath{\omega}}_{R}$, the characteristic collective radiation time ${\ensuremath{\tau}}_{R}$, and the pump pulse duration ${\ensuremath{\tau}}_{P}$ satisfy the inequalities, ${\ensuremath{\omega}}_{R}>\frac{1}{{\ensuremath{\tau}}_{R}}>\ensuremath{\gamma}$ and ${\ensuremath{\tau}}_{P}\ensuremath{\gtrsim}{\ensuremath{\tau}}_{R}$ ($\ensuremath{\gamma}$ is a characteristic internal dephasing rate for the molecules), the system is left in a state with classical transverse polarization when the pump pulse terminates. The system can evolve collectively from such a state only as superradiant (classical) evolution. For superfluorescent evolution which requires a state of preparation of complete inversion (zero transverse polarization), it is shown that the pump pulse must be effectively of area $\ensuremath{\pi}$ and that ${\ensuremath{\tau}}_{P}<{\ensuremath{\tau}}_{R}$. Our results show that when the former conditions are satisfied the delay time ${\ensuremath{\tau}}_{D}$ for collective free pulse evolution is a function of both ${\ensuremath{\tau}}_{P}$ and ${\ensuremath{\tau}}_{R}$. It is shown further that the pump pulse shape as well as temporal duration significantly affect the final state of preparation. The results of this work are interpreted in connection with recent reported results of experiments in superfluorescence and superradiance.