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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Parametric pulse breakup due to population pulsations in three-level systems

Steven F. DiMarco, Cyrus D. Cantrell

Published Sep 1, 1991• 0 citations
Publisher

Abstract

This paper presents the results of a numerical calculation of laser pulse propagation in a vapor of three-level atoms. The calculation is semi-classical in that the macroscopic electric fields are determined classically using Maxwell's equations, while the microscopic polarization is determined quantum mechanically using Schrodinger's equation. The pump laser field is tuned nearly resonant with the first atomic transition of the three-level folded-ladder system. It has previously been shown that in a three-level vapor in which the dipole coupling of the second transition is sufficiently smaller than the dipole coupling of the first transition, the dynamics of the laser-matter interaction are dominated by self-action effects of the pump pulse. This calculation shows dramatically different propagation effects when the second transition dipole moment is greater than the first transition. The larger dipole moment allows the final state to compete with the ground state for population that is pumped into the intermediate state by the pump pulse. This enhances the Stokes gain and increases the Raman efficiency while hindering the processes that produce self-induced transparency and other self-action effects. The periodic fluctuations of the intermediate state population leads to the parametric breakup of the electric fields.

DOI
10.1117/12.46773

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Sep 1, 1991•0 citations
This paper presents the results of a numerical calculation of laser pulse propagation in a vapor of three-level atoms. The calculation is semi-classical in that the macroscopic electric fields are determined classically using Maxwell's equations, while the microscopic polarization is determined quantum mechanically using Schrodinger's equation. The pump laser field is tuned nearly resonant with the first atomic transition of the three-level folded-ladder system. It has previously been shown that in a three-level vapor in which the dipole coupling of the second transition is sufficiently smaller than the dipole coupling of the first transition, the dynamics of the laser-matter interaction are dominated by self-action effects of the pump pulse. This calculation shows dramatically different propagation effects when the second transition dipole moment is greater than the first transition. The larger dipole moment allows the final state to compete with the ground state for population that is pumped into the intermediate state by the pump pulse. This enhances the Stokes gain and increases the Raman efficiency while hindering the processes that produce self-induced transparency and other self-action effects. The periodic fluctuations of the intermediate state population leads to the parametric breakup of the electric fields.
It is now known that conical emission in a two-level atomic system is a fundamental propagation effect brought about by the breakup of the exciting laser pulse into solitary waves.1 This report presents a semiclassical numerical calculation that extends this previous work by solving the optical Bloch and Maxwell equations for a three-level atomic vapor excited by laser fields of two different frequencies. The applied fields satisfy a two-photon resonance condition between the ground and final states and are slightly detuned from the intermediate state to enhance the nonlinear polarization.2 As the fields propagate, oscillations in the nonlinear polarization of the pump beam dominate the interaction and lead to the pump's breakup into solitary waves. The Stokes polarization, depending on the pump radiation, also experiences these oscillations. Because of the intensity-dependence of the refractive index, the solitary waves experience a curvature in the time-radius plane. This curvature manifests itself in the spectrum as a radial component of the wave vector at the Rabi frequency. The Stokes field, experiencing parametric breakup, displays a similar curvature. Spectral analysis reveals a radial component of the Stokes wave vector as well. This frequency-shifted off-axis radiation is identified as conical emission in the Stokes field.
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 (ccc-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.
We report on computer-generated solutions to the coupled matter-field equations which provide the first evidence for distortionless optical pulse propagation in an absorbing medium of three-level atoms. The associated phenomenon represents the three-level equivalent of self-induced transparency in two-level atoms. Results have application to the propagation of short, coherent optical pulses in a medium in which the atoms have two distinct transition frequencies in near resonance with the pulse carrier frequency. We relate in particular to the case of pulse propagation in a magnetically perturbed sodium vapor where the pulse carrier frequency is tuned near the frequencies of the well-known sodium DDD lines. Here we obtain particular solutions corresponding to three and five peak pulses with "areas" of approximately $6\ensuremath{\pi}$ and $10\ensuremath{\pi}$, respectively. The solutions are strongly supported by a number of analytical results. In particular, simple algebraic relations are found which give the populations of the levels in terms of the field variables.
This paper investigates stimulated emission and absorption near resonance for a driven system of interacting two-level atoms. Microscopic kinetic equations for the density matrix elements of N-atom states including atomic motion are built, taking into account atom-field and atom-atom interactions. Analytical solutions are given for the resulting macroscopic equations in different limits, for a system composed of a strong coherent “pump” field and a weak counter-propagating “probe” field. It was shown that the existence of a dipole-dipole (long-range) interaction between atoms separated by distance less than the pump wave-length can cause the formation of periodic polarization and population structures (gratings in time and space) in the pumped medium without a probe field. The magnitude of pump induced population grating can have a strong dependence on the relation between the pump field detuning and the polarization decay rate. The “interaction” between pump and probe induced polarization/population gratings through a dipole-dipole interaction mechanism causes the absorption line shape asymmetry. Under certain conditions, this asymmetry is revealed in increasing probe gain for the “red”-shifted (relative to pump) probe and suppressing the gain for the “blue”-shifted probe field when pump is “red”-shifted relative to the ensemble averaged resonant frequency. The theoretical results are consistent with experimental data for the probe gain or absorption as the function of frequency and the dependance of the gain on atomic density for sodium vapor when the pump laser is tuned near the D 2 line. Here the dependance of gain on particle density was explained in the terms of the long-range interaction between the atoms.
The effect of the collisions on the control of coherent population transfer in a closed inverse YYY-type four-level system driven by three laser fields is investigated with the stimulated Raman adiabatic passage technique. An arbitrary coherent superposition between the initial state and target state can be created either by varying the Rabi frequency of the control laser field or by tuning the one-photon detunings of the pump and Stokes laser fields. When the three laser fields with nearly equal peak Rabi frequencies are each tuned to resonance with the respective transitions, the low transfer efficiency due to the nonadiabatic coupling between two degenerate adiabatic states could be enhanced dramatically with the increase of the collision-induced coherence decay rates to the value nearly comparable to the Rabi frequency of the control field. The enhanced transfer efficiency results from the collision-controlled electromagnetically induced transparency in the $\ensuremath{\Lambda}$-type three-level subsystem and electromagnetically induced absorption in the ladder-type three-level subsystem of the four-level system.
Using a semiclassical, effective-state approach to laser pulse propagation in a dilute gas of polyatomic molecules, a numerical model of multiphoton excitation which includes quasi- continuum transitions is used to calculate the effects of coherent propagation on multi-photon absorption. The initial laser field is assumed to be a quasimonochromatic Gaussian envelope which is nearly resonant with a portion of the lower vibrational states of the molecule. The molecular model consists of a single ground state and several bands of discrete states which are successively connected via electric dipole transitions. This model correctly mimics some of the major characteristics of multiphoton absorption, such as power threshold, fluence dependent absorption, and complete population inversion at high fluences. The model also allows for the calculation of the polarization induced in the medium by the electric field, and the subsequent influence that the polarization has on the field. As the pulse propagates, the Rabi oscillations induced in the lower level states become encoded onto the pulse, creating a series of peaks and troughs similar to the behavior of pulse propagation in two-level systems. Another coherent propagation effect which can change the excitation process is coherent sideband generation. The temporal distortions and the generation of new frequencies results in changes in the population distribution among the states, as well as changes in the total population transferred to the quasi-continuum. The pulse reshaping occurs while the total fluence of the pulse is decreasing due to energy loss to the quasi-continuum. The effective increase in total population transfer due to propagation effects is offset by the decrease in fluence. The resulting transfer of energy from the pulse to the molecule depends strongly on the initial characteristic of the pulse. These processes play an important role in any system where the efficient transfer of laser energy to the medium is required, such as laser-induced chemistry and laser isotope separation.