Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Physical Review A

Transient effects of dephasing and relaxation in cooperative evolution among three-level systems: II

C. M. Bowden, Chi C. Sung

Published Nov 1, 1979• 26 citations
Publisher

Abstract

The effect of uniform dephasing and relaxation on the dynamical evolution of the population in a macroscopic volume of three-level molecules is considered where the population is driven optically between the initial ground state and the extreme excited state 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. The authors examine the evolution of collective relaxation between the excited and intermediate levels in the time regime of the pump pulse duration ${\ensuremath{\tau}}_{p}$. It is found that in the homogeneously broadened regime, in the mean-field limit, for uniform pumping, and under conditions such that the pump Rabi rate ${\ensuremath{\omega}}_{R}$, the characteristic collective relaxation time ${\ensuremath{\tau}}_{R}$ and ${T}_{1}$ and ${T}_{2}$ satisfy the inequalities ${\ensuremath{\omega}}_{R}{\ensuremath{\tau}}_{R}$, ${\ensuremath{\omega}}_{R}{T}_{1}$, ${\ensuremath{\omega}}_{R}{T}_{2}\ensuremath{\gg}1$, collective transverse polarization will evolve if $\frac{{\ensuremath{\gamma}}_{R}}{4\ensuremath{\gamma}}>1$, ${\ensuremath{\omega}}_{R}{\ensuremath{\tau}}_{p}\ensuremath{\approx}\ensuremath{\pi}$ ($\ensuremath{\gamma}$ is the uniform dephasing rate, i.e., $\ensuremath{\gamma}={T}_{2}^{\ensuremath{-}1}$). If, on the other hand, the above conditions are met, but $\frac{{\ensuremath{\gamma}}_{R}}{4\ensuremath{\gamma}}<1$, no collective transverse polarization will evolve during the pump-pulse duration ${\ensuremath{\tau}}_{p}$. In the first case super-radiant pulse evolution (classical collective evolution) may evolve after pump-pulse termination. In the latter case it is possible for collective spontaneous relaxation (superfluorescence) to take place if other conditions are satisfied. Further, a convenient algorithm is established whereby results for the super-radiance or superfluorescence model in the mean-field, small-tipping-angle limit are shown to be formally identical to corresponding results for the lethargic, asymptotic regime of swept-gain super-radiance. In the latter case, the equations of motion are with respect to the retarded time frame and the field equations are replaced by Maxwell's equations. It is shown that the mean-field approximation for the case of super-radiance or superfluorescence is formally equivalent to the asymptotic-limit approximation for swept-gain super-radiance. It is found that a solitary pulse will evolve if the gain-to-loss ratio $\frac{{\ensuremath{\gamma}}_{R}}{4\ensuremath{\gamma}}>1$; if $\frac{{\ensuremath{\gamma}}_{R}}{4\ensuremath{\gamma}}<1$, no solitary pulse will evolve.

DOI
10.1103/physreva.20.2033

Related papers

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

C. M. Bowden, Chi C. Sung

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.

Physical Review A•Oct 1, 1978•58 citations

Laser-induced rate processes in gases: Intermolecular and intramolecular relaxation in a polyatomic molecule

James P. Stone, Myron F. Goodman

We present a formalism to analyze the effects of collisions and intramolecular energy transfer and dephasing processes (${T}_{1}$ and ${T}_{2}$ relaxation) on level-population dynamics and unimolecular decay of laser-driven gas molecules. Utilizing a Boltzmann or optical Bloch equation for the density matrix to describe laser excitation of a relaxing multilevel absorber, we develop a generalized master equation (GME) to describe the dynamics of level population evolution for multilevel absorbers having arbitrary numbers of quantum levels $N$. Because the resulting level-population equations explicitly retain phase memory, the effect of complete or partial phase-coherent driving or incoherent driving by the laser field are all included within the GME solutions. The formalism provides straightforward means to calculate time-dependent solutions for arbitrary $N$, where a single expression is valid on transient, post transient, approach to steady state, and steady-state time scales. We illustrate the behavior of these solutions for the special case of three- and eight-level systems, but the method is not restricted with regard to number of levels. In both this and the following paper, we use specific examples and general arguments to show that an ordinary master equation (OME) is invalid even under apparently favorable conditions including saturating field strengths. We demonstrate that, for an $N$-level absorber with given coupling elements, there are $\frac{N}{2}$ [or $\frac{(N+1)}{2}$] independent saturation solutions and that special conditions on the relaxation times are required to produce the ordinary equal-population solution. Explicit forms for the steady-state radiative-transition matrix $W(\ensuremath{\lambda}=0)$ are derived for arbitrary $N$, and general arguments are given to show that the correct description of the dynamics given by the GME results from matrix singularities in $W(\ensuremath{\lambda}=0)$ which can never occur in an OME or similar rate equations.

Physical Review A•Dec 1, 1978•25 citations

Nonlinear polarizations and excitations and their time dependence in discrete multilevel systems

H. B. Puell, C. R. Vidal

For the interaction of coherent radiation with a nondegenerate, homogeneously broadened multilevel system the nonlinear susceptibilities and excitations and their time dependence are evaluated using a perturbation approach to the density matrix up to fourth order. This is done for the "off-resonance" case, ${(\ensuremath{\Delta}{\ensuremath{\omega}}^{2}+{\ensuremath{\Gamma}}^{2})}^{\frac{1}{2}}\ensuremath{\gg}\frac{1}{\ensuremath{\tau}}$, as well as for the "on-resonance" case, ${(\ensuremath{\Delta}{\ensuremath{\omega}}^{2}+{\ensuremath{\Gamma}}^{2})}^{\frac{1}{2}}\ensuremath{\ll}\frac{1}{\ensuremath{\tau}}$, with $\ensuremath{\tau}$ being the pulse duration, by taking into account the temporal change of the electric field amplitude and the phase and energy relaxation times, ${T}_{2}$ and ${T}_{1}$. It is shown that the transient one-photon excitation known as adiabatic following, is not only important for a pulse duration $\ensuremath{\tau}<{T}_{2}$, but may also be important for ${T}_{2}\ensuremath{\lesssim}\ensuremath{\tau}<{T}_{1}$. In addition, expressions for the transient two-photon excitation in a multilevel system are derived. Finally, the two-level limit is evaluated to all orders of the perturbation including damping effects, which gives results valid also for large incident light intensities. For the "off-resonance" case an expression is obtained which describes not only the transient adiabatic following process, but also the usual one-photon absorption including saturation effects giving rise to power broadening.

Physical Review A•Dec 1, 1976•32 citations

Optical coherence properties of collective molecular systems: A comparison of the statistical and quantum approaches

Izo I. Abram, Robin M. Hochstrasser

The formalism of collective (Dicke-like) states and operators is used to describe the relaxation of the initially prepared state of a material in the presence of a laser field. The material states are shown to be expressible as minimum uncertainty wave packets formed from those special collective states that couple with the radiation field. It is shown that these coherent states of matter exhibit all the features that are usually attributed to ensemble averages of two-level molecules in a conventional statistical picture. However, there are new features in the quantum mechanical model when there are correlations among the molecules in the ensemble. The loss of minimum uncertainty characteristics of the wave packet correspnds to the transverse (T2) relaxation of the statistical model. Different types of T2 processes can be defined corresponding to the decay of different orders of coherence of the wave packet. Only for the case that the system decays in all orders of coherence do the quantum and statistical results coincide. There is expected to be a transverse relaxation that preserves one or more orders of coherence. Experiments are suggested that can test these ideas. A particular case of the formalism of collective states applies to molecular crystals and it provides a quantum mechanical picture of the dephasing of molecular excitons in terms of orders of coherence analogous to the usual manner of describing states of the radiation field.

The Journal of Chemical Physics•Jul 1, 1981•12 citations

Dynamics of coherent cooperative effects in extended systems under incoherent pumping

A. Sh. Aslaeva, R. F. Malikov

The dynamics of the pulse shape and spectra of superfluorescence, stimulated superradiance, and coherent amplification of ultrashort light pulses is studied for a system of four-level atoms under incoherent cw pumping taking into account homogeneous and inhomogeneous broadening of the luminescence lines. It is found that incoherent pumping at a high level of excitation may significantly change the shape of the emission pulse in cooperative coherent processes. Also, it is found that, depending on the ratio of parameters of the pump, nonradiative transitions, and relaxation, different regimes of superfluorescence and stimulated superradiance may be realized.

Optics and Spectroscopy•Nov 1, 2004•0 citations

Cooperative Transients In Inter-Atomic Correlation In The Presence Of An Externally Applied Coherent Field: Relation To Intrinsic Mirrorless Optical Bistability

Charles M. Bowden, Chi C. Sung

Our model, presented earlier, which predicts the circumstances under which intrinsic mirrorless optical bistability (OB) can occur due to atomic pair correlation in a small volume, is outlined and the results presented. These results, which Predict a first-order phase transition in steady state for an externally-driven collection of a large number of atoms far removed from thermodynamic equilibriun, forms the motivation for a detailed microscopic examination of the dynamical behavior of atonic pair correlation in the presence of externally-applied coherent radiation. 4 model is presented and results are discussed for the transient dynamic evolution of two, two-level atoms separated from each other by a distance r in the presence of an externally-applied coherent radiation field. The results predict collective radiation reaction, frequency shifts, relaxation in terms of the atomic seoaration r (assumed much larger than single atom dimensions), the externally-applied field intensity and spacial uniformity of the field with respect to the inter-atomic volume.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Aug 2, 1982•3 citations
The effect of uniform dephasing and relaxation on the dynamical evolution of the population in a macroscopic volume of three-level molecules is considered where the population is driven optically between the initial ground state and the extreme excited state 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. The authors examine the evolution of collective relaxation between the excited and intermediate levels in the time regime of the pump pulse duration \ensuremathτp{\ensuremath{\tau}}_{p}\ensuremathτp​. It is found that in the homogeneously broadened regime, in the mean-field limit, for uniform pumping, and under conditions such that the pump Rabi rate \ensuremathωR{\ensuremath{\omega}}_{R}\ensuremathωR​, the characteristic collective relaxation time \ensuremathτR{\ensuremath{\tau}}_{R}\ensuremathτR​ and T1{T}_{1}T1​ and T2{T}_{2}T2​ satisfy the inequalities \ensuremathωR\ensuremathτR{\ensuremath{\omega}}_{R}{\ensuremath{\tau}}_{R}\ensuremathωR​\ensuremathτR​, \ensuremathωRT1{\ensuremath{\omega}}_{R}{T}_{1}\ensuremathωR​T1​, \ensuremathωRT2\ensuremath≫1{\ensuremath{\omega}}_{R}{T}_{2}\ensuremath{\gg}1\ensuremathωR​T2​\ensuremath≫1, collective transverse polarization will evolve if \ensuremathγR4\ensuremathγ>1\frac{{\ensuremath{\gamma}}_{R}}{4\ensuremath{\gamma}}>14\ensuremathγ\ensuremathγR​​>1, \ensuremathωR\ensuremathτp\ensuremath≈\ensuremathπ{\ensuremath{\omega}}_{R}{\ensuremath{\tau}}_{p}\ensuremath{\approx}\ensuremath{\pi}\ensuremathωR​\ensuremathτp​\ensuremath≈\ensuremathπ (\ensuremathγ\ensuremath{\gamma}\ensuremathγ is the uniform dephasing rate, i.e., \ensuremathγ=T2\ensuremath−1\ensuremath{\gamma}={T}_{2}^{\ensuremath{-}1}\ensuremathγ=T2\ensuremath−1​). If, on the other hand, the above conditions are met, but \ensuremathγR4\ensuremathγ<1\frac{{\ensuremath{\gamma}}_{R}}{4\ensuremath{\gamma}}<14\ensuremathγ\ensuremathγR​​<1, no collective transverse polarization will evolve during the pump-pulse duration \ensuremathτp{\ensuremath{\tau}}_{p}\ensuremathτp​. In the first case super-radiant pulse evolution (classical collective evolution) may evolve after pump-pulse termination. In the latter case it is possible for collective spontaneous relaxation (superfluorescence) to take place if other conditions are satisfied. Further, a convenient algorithm is established whereby results for the super-radiance or superfluorescence model in the mean-field, small-tipping-angle limit are shown to be formally identical to corresponding results for the lethargic, asymptotic regime of swept-gain super-radiance. In the latter case, the equations of motion are with respect to the retarded time frame and the field equations are replaced by Maxwell's equations. It is shown that the mean-field approximation for the case of super-radiance or superfluorescence is formally equivalent to the asymptotic-limit approximation for swept-gain super-radiance. It is found that a solitary pulse will evolve if the gain-to-loss ratio \ensuremathγR4\ensuremathγ>1\frac{{\ensuremath{\gamma}}_{R}}{4\ensuremath{\gamma}}>14\ensuremathγ\ensuremathγR​​>1; if \ensuremathγR4\ensuremathγ<1\frac{{\ensuremath{\gamma}}_{R}}{4\ensuremath{\gamma}}<14\ensuremathγ\ensuremathγR​​<1, no solitary pulse will evolve.
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 present a formalism to analyze the effects of collisions and intramolecular energy transfer and dephasing processes (T1{T}_{1}T1​ and T2{T}_{2}T2​ relaxation) on level-population dynamics and unimolecular decay of laser-driven gas molecules. Utilizing a Boltzmann or optical Bloch equation for the density matrix to describe laser excitation of a relaxing multilevel absorber, we develop a generalized master equation (GME) to describe the dynamics of level population evolution for multilevel absorbers having arbitrary numbers of quantum levels NNN. Because the resulting level-population equations explicitly retain phase memory, the effect of complete or partial phase-coherent driving or incoherent driving by the laser field are all included within the GME solutions. The formalism provides straightforward means to calculate time-dependent solutions for arbitrary NNN, where a single expression is valid on transient, post transient, approach to steady state, and steady-state time scales. We illustrate the behavior of these solutions for the special case of three- and eight-level systems, but the method is not restricted with regard to number of levels. In both this and the following paper, we use specific examples and general arguments to show that an ordinary master equation (OME) is invalid even under apparently favorable conditions including saturating field strengths. We demonstrate that, for an NNN-level absorber with given coupling elements, there are N2\frac{N}{2}2N​ [or (N+1)2\frac{(N+1)}{2}2(N+1)​] independent saturation solutions and that special conditions on the relaxation times are required to produce the ordinary equal-population solution. Explicit forms for the steady-state radiative-transition matrix $W(\ensuremath{\lambda}=0)$ are derived for arbitrary NNN, and general arguments are given to show that the correct description of the dynamics given by the GME results from matrix singularities in $W(\ensuremath{\lambda}=0)$ which can never occur in an OME or similar rate equations.
For the interaction of coherent radiation with a nondegenerate, homogeneously broadened multilevel system the nonlinear susceptibilities and excitations and their time dependence are evaluated using a perturbation approach to the density matrix up to fourth order. This is done for the "off-resonance" case, ${(\ensuremath{\Delta}{\ensuremath{\omega}}^{2}+{\ensuremath{\Gamma}}^{2})}^{\frac{1}{2}}\ensuremath{\gg}\frac{1}{\ensuremath{\tau}}$, as well as for the "on-resonance" case, ${(\ensuremath{\Delta}{\ensuremath{\omega}}^{2}+{\ensuremath{\Gamma}}^{2})}^{\frac{1}{2}}\ensuremath{\ll}\frac{1}{\ensuremath{\tau}}$, with $\ensuremath{\tau}$ being the pulse duration, by taking into account the temporal change of the electric field amplitude and the phase and energy relaxation times, T2{T}_{2}T2​ and T1{T}_{1}T1​. It is shown that the transient one-photon excitation known as adiabatic following, is not only important for a pulse duration $\ensuremath{\tau}<{T}_{2}$, but may also be important for ${T}_{2}\ensuremath{\lesssim}\ensuremath{\tau}<{T}_{1}$. In addition, expressions for the transient two-photon excitation in a multilevel system are derived. Finally, the two-level limit is evaluated to all orders of the perturbation including damping effects, which gives results valid also for large incident light intensities. For the "off-resonance" case an expression is obtained which describes not only the transient adiabatic following process, but also the usual one-photon absorption including saturation effects giving rise to power broadening.
The formalism of collective (Dicke-like) states and operators is used to describe the relaxation of the initially prepared state of a material in the presence of a laser field. The material states are shown to be expressible as minimum uncertainty wave packets formed from those special collective states that couple with the radiation field. It is shown that these coherent states of matter exhibit all the features that are usually attributed to ensemble averages of two-level molecules in a conventional statistical picture. However, there are new features in the quantum mechanical model when there are correlations among the molecules in the ensemble. The loss of minimum uncertainty characteristics of the wave packet correspnds to the transverse (T2) relaxation of the statistical model. Different types of T2 processes can be defined corresponding to the decay of different orders of coherence of the wave packet. Only for the case that the system decays in all orders of coherence do the quantum and statistical results coincide. There is expected to be a transverse relaxation that preserves one or more orders of coherence. Experiments are suggested that can test these ideas. A particular case of the formalism of collective states applies to molecular crystals and it provides a quantum mechanical picture of the dephasing of molecular excitons in terms of orders of coherence analogous to the usual manner of describing states of the radiation field.
The dynamics of the pulse shape and spectra of superfluorescence, stimulated superradiance, and coherent amplification of ultrashort light pulses is studied for a system of four-level atoms under incoherent cw pumping taking into account homogeneous and inhomogeneous broadening of the luminescence lines. It is found that incoherent pumping at a high level of excitation may significantly change the shape of the emission pulse in cooperative coherent processes. Also, it is found that, depending on the ratio of parameters of the pump, nonradiative transitions, and relaxation, different regimes of superfluorescence and stimulated superradiance may be realized.
Our model, presented earlier, which predicts the circumstances under which intrinsic mirrorless optical bistability (OB) can occur due to atomic pair correlation in a small volume, is outlined and the results presented. These results, which Predict a first-order phase transition in steady state for an externally-driven collection of a large number of atoms far removed from thermodynamic equilibriun, forms the motivation for a detailed microscopic examination of the dynamical behavior of atonic pair correlation in the presence of externally-applied coherent radiation. 4 model is presented and results are discussed for the transient dynamic evolution of two, two-level atoms separated from each other by a distance r in the presence of an externally-applied coherent radiation field. The results predict collective radiation reaction, frequency shifts, relaxation in terms of the atomic seoaration r (assumed much larger than single atom dimensions), the externally-applied field intensity and spacial uniformity of the field with respect to the inter-atomic volume.