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Physical Review A

Cooperative radiation processes in two-level systems: Superfluorescence

R. Bonifacio, Luigi A. Lugiato

Published May 1, 1975• 623 citations
Publisher

Abstract

We give a general nonperturbative treatment of cooperative emission in systems of $N$ two-level atoms, starting from first principles and including inhomogeneous broadening. In particular, we study superfluorescence, which is defined as the cooperative spontaneous emission, i.e., radiation rate proportional to ${N}^{2}$, from an atomic system initially excited with zero macroscopic dipole moment and a uniform population difference between the excited and the fundamental states. The atomic system is described by means of collective dipole operators. A fundamental justification is given for the existence of damped "quasimodes" of the mirrorless active volume. The damping of such modes is simply due to the propagation of the Maxwell field, which escapes from the active volume. A general atom-field master equation is derived for the system atoms plus field inside the active volume, described, respectively, in terms of collective dipole operators and quasimode operators. An important feature of this equation is that inhomogeneous broadening simply appears via a time-dependent atom-field coupling constant. In this paper we give a semiclassical treatment of such a master equation. For a pencil-shaped geometry of the active volume, generalized Maxwell-Bloch equations are derived for the envelopes of the radiation inside the active volume and polarization. Such equations take into account the two directions of propagation of the radiation and the inhomogeneous broadening. Suitably phrasing our initial condition in semiclassical terms, we find that propagation effects can be neglected at all times and the generalized Maxwell-Bloch equations reduce to a simple pendulum equation. On the basis of the discussion of the pendulum equation, we conclude that superfluorescence occurs when (i) the length $L$ of the active volume is much larger than a suitable threshold length ${L}_{T}$ (this condition ensures that the dephasing atomic processes occur on a time scale much larger than the times characteristic of the cooperative emission); (ii) the length $L$ is smaller or of the same order of a suitable cooperation length ${L}_{c}$ (this condition ensures that cooperative spontaneous emission dominates stimulated processes, which give radiation proportional to $N$). For $L\ensuremath{\ll}{L}_{c}$, one has a hyperbolic-secant superfluorescent pulse; for $L\ensuremath{\approx}{L}_{c}$, as one has in the recent experiments of Skribanowitz et al., one finds oscillations in the cooperative decay and in the radiation emission. Such oscillations are due to the contribution of stimulated processes. For $L\ensuremath{\gg}{L}_{c}$, this contribution increases. As a consequence one gets more oscillations in the radiated intensity, which becomes proportional to $N$, so that superfluorescence effects disappear.

DOI
10.1103/physreva.11.1507

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We discuss from first principles the cooperative decay of a system of two-level atoms, initially prepared in an uncorrelated excited state with population inversion $N$, and we give the conditions under which the superfluorescence effect occurs. Describing the atomic system in terms of collective variables, we derive a master equation for the reduced atomic density operator, which gives rise both to a damping and to a time-dependent frequency shift in the dynamics of collective modes. The coupled equations of motion are solved with a self-consistent approach. It is found that the system goes through a nonexponential decay if the maximum length of the active volume is smaller than a "cooperation range" and larger than a "threshold length," in agreement with the one-mode theory. The radiation burst has a time width proportional to ${N}^{\ensuremath{-}1}$, and its intensity is proportional to ${N}^{2}$. Specializing to a pencil-shaped volume, we find that only two atomic modes need to be considered; in this case, the average emitted radiation is all condensed in the two diffraction patterns of the opposite axial modes.

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Cooperative radiation processes in two-level systems: Superfluorescence. II

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Master-Equation Approach to Spontaneous Emission. III. Many-Body Aspects of Emission from Two-Level Atoms and the Effect of Inhomogeneous Broadening

G. S. Agarwal

A general theory of spontaneous emission was developed in Papers I and II of this series. In the present paper, the mastre equation describing spontaneous emission from $N$ identical two-level atoms is investigated further. It is shown that the equation of motion for the $p(<N)$-atom density matrix is coupled to the ($p+1$)-atom density matrix. We first consider the initial excitation of the system to state $|{\ensuremath{\theta}}_{0},{\ensuremath{\phi}}_{0}〉$ (${\ensuremath{\theta}}_{0}<\ensuremath{\pi}$) and solve the hierarchy of equations so obtained in the "uncorrelated approximation." It is found that the presence of other atoms is equivalent to an external field which is determined from a self-consistent analysis. It is also found that in this approximation the state of the atom at time $t$ can be described by a single parameter $\ensuremath{\theta}(t)$ ($\ensuremath{\theta}<\ensuremath{\pi}$), with ${sin}^{2}\frac{1}{2}\ensuremath{\theta}$ giving the probability that the atom is to be found in the excited state. Next, some improvements over the uncorrelated approximation are given. This is done by decoupling the equation of motion for higher-order mean values. It is found that the fluctuation $〈({S}_{i}^{Z}\ensuremath{-}〈{S}_{i}^{Z}〉)({S}_{j}^{Z}\ensuremath{-}〈{S}_{j}^{Z}〉)〉$ for any pair of atoms is of the order of $\frac{1}{N}$. The case when ${\ensuremath{\theta}}_{0}=\ensuremath{\pi}$ is considered separately and we obtain an expression for the radiation rate by making a "Hartree-Fock" type of approximation on the two-particle mean values. In this case, the behavior of the radiation rate is found to differ markedly from the "sech" behavior. It is then shown that the entire dynamics of two-level atoms emitting spontaneously can be described by a set of $2N$ coupled first-order equations which clearly exhibit the type of nonlinearity (which is the analog of the van der Pol type of nonlinearity) for this problem and provide a better understanding of spontaneous emission. Finally in Sec. V, the theory is extended to include the effects of inhomogeneous broadening, and the functional dependence of the radiation rate on the atomic-line-shape factor is obtained.

Physical Review A•Nov 1, 1971•62 citations
We give a general nonperturbative treatment of cooperative emission in systems of NNN two-level atoms, starting from first principles and including inhomogeneous broadening. In particular, we study superfluorescence, which is defined as the cooperative spontaneous emission, i.e., radiation rate proportional to N2{N}^{2}N2, from an atomic system initially excited with zero macroscopic dipole moment and a uniform population difference between the excited and the fundamental states. The atomic system is described by means of collective dipole operators. A fundamental justification is given for the existence of damped "quasimodes" of the mirrorless active volume. The damping of such modes is simply due to the propagation of the Maxwell field, which escapes from the active volume. A general atom-field master equation is derived for the system atoms plus field inside the active volume, described, respectively, in terms of collective dipole operators and quasimode operators. An important feature of this equation is that inhomogeneous broadening simply appears via a time-dependent atom-field coupling constant. In this paper we give a semiclassical treatment of such a master equation. For a pencil-shaped geometry of the active volume, generalized Maxwell-Bloch equations are derived for the envelopes of the radiation inside the active volume and polarization. Such equations take into account the two directions of propagation of the radiation and the inhomogeneous broadening. Suitably phrasing our initial condition in semiclassical terms, we find that propagation effects can be neglected at all times and the generalized Maxwell-Bloch equations reduce to a simple pendulum equation. On the basis of the discussion of the pendulum equation, we conclude that superfluorescence occurs when (i) the length LLL of the active volume is much larger than a suitable threshold length LT{L}_{T}LT​ (this condition ensures that the dephasing atomic processes occur on a time scale much larger than the times characteristic of the cooperative emission); (ii) the length LLL is smaller or of the same order of a suitable cooperation length Lc{L}_{c}Lc​ (this condition ensures that cooperative spontaneous emission dominates stimulated processes, which give radiation proportional to NNN). For L\ensuremath≪LcL\ensuremath{\ll}{L}_{c}L\ensuremath≪Lc​, one has a hyperbolic-secant superfluorescent pulse; for L\ensuremath≈LcL\ensuremath{\approx}{L}_{c}L\ensuremath≈Lc​, as one has in the recent experiments of Skribanowitz et al., one finds oscillations in the cooperative decay and in the radiation emission. Such oscillations are due to the contribution of stimulated processes. For L\ensuremath≫LcL\ensuremath{\gg}{L}_{c}L\ensuremath≫Lc​, this contribution increases. As a consequence one gets more oscillations in the radiated intensity, which becomes proportional to NNN, so that superfluorescence effects disappear.
We discuss from first principles the cooperative decay of a system of two-level atoms, initially prepared in an uncorrelated excited state with population inversion NNN, and we give the conditions under which the superfluorescence effect occurs. Describing the atomic system in terms of collective variables, we derive a master equation for the reduced atomic density operator, which gives rise both to a damping and to a time-dependent frequency shift in the dynamics of collective modes. The coupled equations of motion are solved with a self-consistent approach. It is found that the system goes through a nonexponential decay if the maximum length of the active volume is smaller than a "cooperation range" and larger than a "threshold length," in agreement with the one-mode theory. The radiation burst has a time width proportional to ${N}^{\ensuremath{-}1}$, and its intensity is proportional to N2{N}^{2}N2. Specializing to a pencil-shaped volume, we find that only two atomic modes need to be considered; in this case, the average emitted radiation is all condensed in the two diffraction patterns of the opposite axial modes.
In this paper we discuss the quantum features of cooperative radiation processes in a two-level system taking into account non-Markovian effects. If the initial condition is spatially uniform, the many-mode atom-field master equation which has been derived and semiclassically discussed in a previous paper, reduces to the well-known single-mode model laser master equation. Hence, using a suitable projection operator, we derive a generalized non-Markovian master equation which turns out to be correct already in the first Born approximation. This master equation incorporates the effects both of stimulated emission and absorption and of spontaneous emission. When stimulated processes can be neglected, it reduces to a previously known Markovian superradiance master equation, whereas in general it describes non-Markovian oscillations of the radiated intensity. Finally we derive a linear system of equations for the probability of occupation of the Dicke states which generalizes a previously discussed system, taking into account the contribution of stimulated processes.
In order to study the cooperative emission of radiation from an extended system of NNN two-level atoms, we use the master-equation approach within the Born and Markov approximations. All the properties of the emission of radiation can be deduced from the diagonalization of the coupling matrix $\ensuremath{\Gamma}$, where an element ${\ensuremath{\Gamma}}_{\mathrm{jk}}$ gives the coupling between the atoms labeled jjj and kkk via the electromagnetic field. We choose a pencil-shaped volume and study analytically the coupling matrix in the limit for small and large Fresnel numbers. For Fresnel numbers of order unity numerical methods are used. Thus we prove that, for the pencil-shaped geometry, any elaborated model must take into account the interaction of the atoms with the infinity of electromagnetic field modes lying inside two small solid angles about the axis of the largest linear dimension, which we label the zzz axis. In other words, the intensity of radiation emitted by any atom of the system depends on its position with respect to the others and this "propagation effect" cannot be neglected when interpreting superradiance experiments. For small Fresnel numbers the zzz dependence predominates, in the opposite case the (x,yx, yx,y) dependence does, while for Fresnel numbers of order unity the dependence of all three components must be taken into account. Preliminary calculations are given for which only the zzz dependence is considered; for Fresnel numbers of magnitude of order unity or smaller, the effect of propagation along the zzz axis displays large delays for the appearance of superradiance with respect to the time at which the superradiant pulse is maximum when the "propagation effects" are neglected (one-mode model).
In this paper we attempt to unify the theoretical treatment of a variety of cooperative interaction phenomena occurring in resonantly interacting radiation-matter systems. The system consists of a multimode optical field interacting with NNN resonant atoms in a region of large spatial extent. The field and atoms may or may not be coupled to reservoirs. We derive a set of coupled master equations for the reduced matter and radiation density operators of the composite system in the first Born approximation, using a method due to Bogoliubov. These equations describe within a single framework phenomena involving superradiant emission and coherent propagation. In the first place, our theory generalizes existing formulations of the superradiance problem by treating the radiation field as part of the dynamical system rather than as a reservoir. Hence, our equations describe stimulated interaction effects, which are entirely absent in the usual superradiance master equations. Moreover, our equations contain terms describing the self-consistent interaction of an average field with a set of polarizable atoms, as in the coupled Bloch and Maxwell equations of the theory of coherent pulse propagation, and enable us to describe fluctuations, arising from incoherent emission, about the average behavior described by the Bloch-Maxwell theory. We solve formally the dynamical equation for the radiation density operator and obtain a displaced multivariate Gaussian distribution centered on the solution of the Maxwell wave equation, which has as parameters the first and second moments of the matter density operator. Then we derive and discuss the field and atomic-moment equations, both in the wave-number and position representations. The moment equations enable us to show the relationship between descriptions of superradiant damping based on the Bloch equations and those based on the existence of correlated atomic states, including both as special cases. We introduce reduced matter moments, which allow us to separate incoherent- and coherent-emission effects and enable us to discuss the question of the closure of the moment equations. Then we consider cases where the behavior of the atomic system is dominated by a strong coherent pump wave or where the atoms are in a symmetric correlated state and show how the slowly-varying-envelope approximation simplifies the radiation-moment equations in these two cases. In the former case, we obtain an approximate theory which consists, in lowest order, of the Bloch-Maxwell equations with radiative-damping terms, plus an equation describing the time development of the correlation function for field fluctuations. Returning to our general formalism, we relate the usual parameters of the theory of radiative decay and of resonant interactions to the more general quantities appearing in our spatial analysis. Finally, we discuss the importance of the stimulated-emission terms appearing in our theory and describe several extensions, including the introduction of inhomogeneous broadening.
We discuss the cooperative decay of initial atomic excitation for a pencil-shaped active volume filled with two-level atoms. As long as the length of the sample is much smaller than a certain maximal cooperation length, the atom-field interaction producing the superradiant pulse can be treated in terms of the simplest possible laser model (single mode). The basic laser master equation turns out to be exactly solvable if specified for the superradiance limit which is characterized by two conditions: (i) The photons escape from the low-QQQ cavity so fast that they cannot feed themselves back into atomic excitation to any appreciable amount (this no-feedback condition is equivalent to the above-mentioned requirement for the length of the sample). (ii) The incoherent atomic decay due to natural relaxation is so slow that the individual atomic dipoles do not dephase before engaging themselves cooperatively in the interaction with the electromagnetic field. The present paper presents the derivation and general discussion of the equations describing the statistical properties of atoms and field in a superradiant pulse. Analytical and numerical solutions will be presented in a subsequent paper.
A general theory of spontaneous emission was developed in Papers I and II of this series. In the present paper, the mastre equation describing spontaneous emission from NNN identical two-level atoms is investigated further. It is shown that the equation of motion for the p(<N)p(<N)p(<N)-atom density matrix is coupled to the (p+1p+1p+1)-atom density matrix. We first consider the initial excitation of the system to state $|{\ensuremath{\theta}}_{0},{\ensuremath{\phi}}_{0}〉$ (${\ensuremath{\theta}}_{0}<\ensuremath{\pi}$) and solve the hierarchy of equations so obtained in the "uncorrelated approximation." It is found that the presence of other atoms is equivalent to an external field which is determined from a self-consistent analysis. It is also found that in this approximation the state of the atom at time ttt can be described by a single parameter $\ensuremath{\theta}(t)$ ($\ensuremath{\theta}<\ensuremath{\pi}$), with ${sin}^{2}\frac{1}{2}\ensuremath{\theta}$ giving the probability that the atom is to be found in the excited state. Next, some improvements over the uncorrelated approximation are given. This is done by decoupling the equation of motion for higher-order mean values. It is found that the fluctuation $〈({S}_{i}^{Z}\ensuremath{-}〈{S}_{i}^{Z}〉)({S}_{j}^{Z}\ensuremath{-}〈{S}_{j}^{Z}〉)〉$ for any pair of atoms is of the order of 1N\frac{1}{N}N1​. The case when ${\ensuremath{\theta}}_{0}=\ensuremath{\pi}$ is considered separately and we obtain an expression for the radiation rate by making a "Hartree-Fock" type of approximation on the two-particle mean values. In this case, the behavior of the radiation rate is found to differ markedly from the "sech" behavior. It is then shown that the entire dynamics of two-level atoms emitting spontaneously can be described by a set of 2N2N2N coupled first-order equations which clearly exhibit the type of nonlinearity (which is the analog of the van der Pol type of nonlinearity) for this problem and provide a better understanding of spontaneous emission. Finally in Sec. V, the theory is extended to include the effects of inhomogeneous broadening, and the functional dependence of the radiation rate on the atomic-line-shape factor is obtained.