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Physical Review A

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

Published Nov 1, 1971• 62 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.4.1791

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Using the formalism developed earlier, we treat spontaneous emission from a pair of identical two-level atoms ${A}_{1}$, ${A}_{2}$, whose separation ${r}_{21}$ can be comparable to the wavelength $\ensuremath{\lambda}$. We obtain expressions for time-dependent intensities and damping rates with the initial conditions (a) both atoms inverted, (b) prior excitation by a short $\frac{1}{2}\ensuremath{\pi}$ pulse, and (c) only ${A}_{1}$ inverted. The results in (a) are compared with those obtained for a model consisting of two initially excited harmonic oscillators ${O}_{1}$, ${O}_{2}$. The atoms exhibit superradiant behavior, whereas ${O}_{1}$, ${O}_{2}$ tend to trap radiation. In (a), the intensity pattern $\mathcal{R}(\ensuremath{\theta},t)$ develops lobes in different directions at different times, so that the spatial distribution of photons at time $t\ensuremath{\rightarrow}\ensuremath{\infty}$ is the same as in the independent-atom case ${r}_{21}\ensuremath{\gg}\ensuremath{\lambda}$. For the oscillators, the lobes of $\mathcal{R}(\ensuremath{\theta},t)$ do not change direction, but only become more pronounced as time increases. In (b) and (c), the lobes oscillate back and forth at frequency $2{\ensuremath{\Omega}}_{12}$ corresponding to the shifts $\ifmmode\pm\else\textpm\fi{}{\ensuremath{\Omega}}_{12}$ of the triplet and singlet states due to the ${A}_{1}\ensuremath{-}{A}_{2}$ interaction. The intensity can therefore have a sinusoidal component. Field correlation functions calculated for (a) and (c) show that ${A}_{2}$ and ${A}_{2}$ radiate simultaneously around the frequencies $\ensuremath{\epsilon}\ifmmode\pm\else\textpm\fi{}{\ensuremath{\Omega}}_{12}$, where $\ensuremath{\epsilon}$ is the single-atom resonant frequency. The spectrum is calculated for case (c), and shows the effects of coherent linewidth enhancement in addition to the frequency shifts.

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In a previous investigation, a general theory for spontaneous emission from a system of $N$ identical atoms or molecules was developed. This theory was based on the master equation recently derived in another paper. In that paper, the master equation relating to spontaneous emission from a system of harmonic oscillators was also derived. In the present investigation, the normally ordered correlation functions for the oscillator system are calculated and these are then used to calculate the radiation-field correlation functions in the far zone. These correlation functions are compared for two different modes of excitation, viz., (i) when each of the oscillators is excited initially to a Fock state, and (ii) when each of the oscillators is excited to some coherent state. It is found that the even-order ($2n$) correlation functions for the second mode of excitation (superradiant excitation) are of order ${N}^{2n}$ higher than those for the first mode of excitation. It is also shown that the photoelectron counting distribution for the superradiant excitation is Poissonian. Finally, the non-Markoffian effects in the spontaneous emission are studied in detail and their connection with exact results is described.

Physical Review A•May 1, 1971•33 citations
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 ∣\ensuremathθ0,\ensuremathϕ0〉|{\ensuremath{\theta}}_{0},{\ensuremath{\phi}}_{0}〉∣\ensuremathθ0​,\ensuremathϕ0​〉 (\ensuremathθ0<\ensuremathπ{\ensuremath{\theta}}_{0}<\ensuremath{\pi}\ensuremathθ0​<\ensuremathπ) 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 \ensuremathθ(t)\ensuremath{\theta}(t)\ensuremathθ(t) (\ensuremathθ<\ensuremathπ\ensuremath{\theta}<\ensuremath{\pi}\ensuremathθ<\ensuremathπ), with sin212\ensuremathθ{sin}^{2}\frac{1}{2}\ensuremath{\theta}sin221​\ensuremathθ 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 〈(SiZ\ensuremath−〈SiZ〉)(SjZ\ensuremath−〈SjZ〉)〉〈({S}_{i}^{Z}\ensuremath{-}〈{S}_{i}^{Z}〉)({S}_{j}^{Z}\ensuremath{-}〈{S}_{j}^{Z}〉)〉〈(SiZ​\ensuremath−〈SiZ​〉)(SjZ​\ensuremath−〈SjZ​〉)〉 for any pair of atoms is of the order of 1N\frac{1}{N}N1​. The case when \ensuremathθ0=\ensuremathπ{\ensuremath{\theta}}_{0}=\ensuremath{\pi}\ensuremathθ0​=\ensuremathπ 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.
Spontaneous emission from a system of NNN identical two-level atoms is considered using a master equation recently derived by the author. The master equation describing the time evolution of the phase-space distribution function associated with the reduced density operator of the atomic system is obtained. This master equation, which is of the type of a Fokker-Planck equation, is used to derive the equation of motion for the mean values of various atomic operators characterizing the physical properties of the system. This leads to a hierarchy of equations, which is decoupled by making a suitable approximation. The intensity of the spontaneously emitted radiation is then calculated. Next, the spontaneous emission from geometrically small systems is considered. For this case, the master equation is solved exactly, and an exact expression for the radiation rate is obtained. The exact solution of the master equation is also used to calculate the normally ordered correlation functions for the electric field. Section V deals with the spontaneous emission from a system of harmonic oscillators, the size of the system being small compared to a wavelength. The master equation for this problem is also solved exactly, and it is shown that this system also leads to superradiant emission in some cases, e.g., if all the oscillstors are excited initially to some coherent state ∣z0〉|{z}_{0}〉∣z0​〉.
In this chapter, the authors develop a consistent theory of spontaneous emission in an optical micro cavity from a broadened atom. They derive the atomic broadening from first principles by assuming the presence of reservoirs coupled to the atoms. The simplest model of the atom is the so-called two-level atom, which has only two energy levels, the excited and the ground level. However, realistic atoms are surrounded by media that affect the atoms, giving them homogeneous or inhomogeneous broadening. The important parameter of coupling ratio of spontaneous emission to a desired quasi mode cannot be exactly treated by the present mathematical model of the cavity, although it is easily seen qualitatively that the ratio will decrease with increasing atomic broadening. The authors assume that each atom emits independently and ignored the possible interaction among atoms during spontaneous emission. Solving the master equation for the density matrix elements, the readers have derived formulas for spontaneous emission rate and emission spectrum.
The spontaneous emission of a set of NNN identical two-level atoms interacting with a quantized electromagnetic field is studied. The atoms are assumed to be close together compared to the mean wavelength of the emitted radiation, and their initial state is either a Dicke state or a superposition of the ground and excited state for each atom. Approximate expressions are obtained for transition probabilities, expectation values, and correlations as functions of time. The spontaneous emission for a very large separation of the atoms is also studied. In this case the directional properties of the emitted radiation, as well as the time within which the atoms decay to their ground state, depend on the position of each atom.
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 $L\ensuremath{\ll}{L}_{c}$, 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 NNN, so that superfluorescence effects disappear.
Using the formalism developed earlier, we treat spontaneous emission from a pair of identical two-level atoms A1{A}_{1}A1​, A2{A}_{2}A2​, whose separation r21{r}_{21}r21​ can be comparable to the wavelength $\ensuremath{\lambda}$. We obtain expressions for time-dependent intensities and damping rates with the initial conditions (a) both atoms inverted, (b) prior excitation by a short $\frac{1}{2}\ensuremath{\pi}$ pulse, and (c) only A1{A}_{1}A1​ inverted. The results in (a) are compared with those obtained for a model consisting of two initially excited harmonic oscillators O1{O}_{1}O1​, O2{O}_{2}O2​. The atoms exhibit superradiant behavior, whereas O1{O}_{1}O1​, O2{O}_{2}O2​ tend to trap radiation. In (a), the intensity pattern $\mathcal{R}(\ensuremath{\theta},t)$ develops lobes in different directions at different times, so that the spatial distribution of photons at time $t\ensuremath{\rightarrow}\ensuremath{\infty}$ is the same as in the independent-atom case ${r}_{21}\ensuremath{\gg}\ensuremath{\lambda}$. For the oscillators, the lobes of $\mathcal{R}(\ensuremath{\theta},t)$ do not change direction, but only become more pronounced as time increases. In (b) and (c), the lobes oscillate back and forth at frequency $2{\ensuremath{\Omega}}_{12}$ corresponding to the shifts $\ifmmode\pm\else\textpm\fi{}{\ensuremath{\Omega}}_{12}$ of the triplet and singlet states due to the ${A}_{1}\ensuremath{-}{A}_{2}$ interaction. The intensity can therefore have a sinusoidal component. Field correlation functions calculated for (a) and (c) show that A2{A}_{2}A2​ and A2{A}_{2}A2​ radiate simultaneously around the frequencies $\ensuremath{\epsilon}\ifmmode\pm\else\textpm\fi{}{\ensuremath{\Omega}}_{12}$, where $\ensuremath{\epsilon}$ is the single-atom resonant frequency. The spectrum is calculated for case (c), and shows the effects of coherent linewidth enhancement in addition to the frequency shifts.
In a previous investigation, a general theory for spontaneous emission from a system of NNN identical atoms or molecules was developed. This theory was based on the master equation recently derived in another paper. In that paper, the master equation relating to spontaneous emission from a system of harmonic oscillators was also derived. In the present investigation, the normally ordered correlation functions for the oscillator system are calculated and these are then used to calculate the radiation-field correlation functions in the far zone. These correlation functions are compared for two different modes of excitation, viz., (i) when each of the oscillators is excited initially to a Fock state, and (ii) when each of the oscillators is excited to some coherent state. It is found that the even-order (2n2n2n) correlation functions for the second mode of excitation (superradiant excitation) are of order N2n{N}^{2n}N2n higher than those for the first mode of excitation. It is also shown that the photoelectron counting distribution for the superradiant excitation is Poissonian. Finally, the non-Markoffian effects in the spontaneous emission are studied in detail and their connection with exact results is described.