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Journal of the Optical Society of America B

Harmonic generation accompanying collective spontaneous emission

Victor A Malyshev, Pablo Moreno

Published Dec 1, 1997• 0 citations
Publisher

Abstract

We discuss the possibility of producing harmonics while the process of collective spontaneous emission (superradiance) takes place in a solid. Self correlations of dipole radiators induced by the emitted field lead to a reduction of the emission time and consequently to an increase of the intensity. Estimations of the superradiant energy flux show that, for crystalline densities of radiators, this flux may be comparable with the atomic unit. This assures the highly nonlinear behavior necessary to observe a pulse of high harmonics during superradiant pulse. We apply the Floquet–Bloch expansion to analyze the features of harmonic production in the framework of the two-level model.

DOI
10.1364/josab.14.003273

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Radiation from an N -Atom System. II. Spontaneous Emission from a Pair of Atoms

Robert H. Lehmberg

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.

Physical Review A•Sep 1, 1970•280 citations
We discuss the possibility of producing harmonics while the process of collective spontaneous emission (superradiance) takes place in a solid. Self correlations of dipole radiators induced by the emitted field lead to a reduction of the emission time and consequently to an increase of the intensity. Estimations of the superradiant energy flux show that, for crystalline densities of radiators, this flux may be comparable with the atomic unit. This assures the highly nonlinear behavior necessary to observe a pulse of high harmonics during superradiant pulse. We apply the Floquet–Bloch expansion to analyze the features of harmonic production in the framework of the two-level model.
The present state of theoretical and experimental research on collective spontaneous emission (superradiance) in a system of radiators (atoms, molecules, or nuclei) is reviewed. The distinction between superradiance and the amplification of spontaneous emission is discussed. There is also a discussion of conditions under which the effect can be observed and of various theoretical methods for describing superradiance: the quantum single-mode and multimode models and the semiclassical approach. Theoretical papers on superradiance in systems with dimensions smaller than the wavelength of the radiation and also in extended systems are reviewed. It is shown that superradiance may occur in weakly amplifying media. A situation in which the superradiance is oscillatory is described. The possible use of superradiance to generate coherent emission in the x-ray and ? ranges is discussed. The superradiance accompanying Raman scattering of light in atomic and molecular media is studied. The theoretical results are compared with experimental observations of superradiance in the optical range. In an appendix, the nature of the phase transition in a system of radiators interacting through an electromagnetic field is discussed.
A theoretical model for the propagation of coherent light pulses in resonant media where a large number of atoms cooperate in spontaneous emission (superradiance) is discussed. The medium is supposedly free of inhomogeneous broadening, and no lossy relaxation mechanisms are taken into account. The conditions for the emission of all spontaneous radiation in the direction of pulse propagation are described. A semi-classical model is used and, at each point in the medium, the propagation field and the spontaneous damping field are considered separately. The equation governing the evolution of a superradiant system in the presence of an applied pulse is derived. A mechanism of energy transfer from the traveling pulse to the medium is described which includes superradiant spontaneous emission effects. As a result of the neglect of all lossy relaxation processes, all energy stored in the medium is eventually returned to the pulse by coherent spontaneous emission. Therefore, in this theory, all pulses travel through the medium without energy loss. Numerical results for square input pulses are discussed which show two possible types of propagation behavior: (a) Low input intensities produce a negative tail to the input (positive) pulse and sharpening of the tail with the advance in the medium; (b) higher input intensities produce, after sufficient penetration, a steady-state pulse envelope somewhat similar to the $2\ensuremath{\pi}$ pulses of self-induced transparency. The steady-state solutions of the equations of motion are found numerically and the pulse shapes are computed for different degrees of superradiance. In the limit of strong superradiance, very asymmetric pulse envelopes of large area are found. For negligible superradiance, approximately $2\ensuremath{\pi}$ hyperbolic-secant pulses are obtained. The effects of inhomogeneous broadening are briefly considered, and the consequences of important superradiant damping in photon-echo experiments are qualitatively discussed.
Spontaneous decay is a phenomenon that has been described for the first time by Dirac, Wigner and Weisskopf, at the early ages of the development of quantum electrodynamics. The theory is applicable to a multi-body system only when atoms don’t interact during their decay. Dicke introduces in his seminal paper the case where this assumption doesn’t hold. The results he obtains not only tell that the system emits pulses, but the pulse duration now depends on 1/N, where N is the number of participating atoms to the process. The pulses temporal profile is described by a squared hyperbolic secant function. The resulting emission intensity scales as N^2. The atomic system radiates more intensively than the ordinary fluorescent emission, this is the reason why the process is called superradiance, or by a generalization to extended systems, superfluorescence. The superradiant emission has preferential escape directions, depending on the atomic sample shape. Superradiance is a collective process and it takes place when the group of excited atoms is left unper- turbed during the formation of of the macroscopic dipole. A fundamental difference compared to the spontaneous and stimulated emission processes is that all atoms act together as a single entity and it isn’t possible to identify single atoms involved. This remarkable behaviour is manifest when the atomic coherence of the system, while influenced by environmental interactions that cause dephasing in atoms, persists for a sufficient interval of time. Typical dephasing mechanisms, such as collisions in gases or lattice phonon interactions in crystals, make its experimental observation difficult. A possible solution to this problem is the use of optical crystals doped with rare-earths that are characterized by long and narrow levels lifetimes.
We introduce a straightforward quantum-electrodynamic approach to the problem of superradiant spontaneous emission from a system of two-level atoms, and also discuss two classical superradiant systems. The same physical concepts underlie our treatment of both the quantum and classical cases. Explicit expressions are found which describe the time evolution and directional character of the radiated power. Our approach applies to an arbitrary number of atoms which are confined to a region with linear dimensions which may be large compared with the mean wavelength of the emitted radiation. The radiative decay half-life of a large many-atom system is found to be much shorter than the natural lifetime of a single atom, but not as short as the half-life of a small atomic system with the same number of atoms. The far-field radiation pattern appropriate to the case of a circular cylinder of emitters which have been excited by a plane-wave pulse is considered in detail. Polar plots are presented of the radiation patterns produced when the atoms are excited by a plane-wave pulse. Exciting pulses traveling in directions both parallel and at an angle of 10\ifmmode^\circ\else\textdegree\fi{} to the axis of the cylinder are considered. A discussion and generalization of Dicke's "coherence-brightening" criterion is given.
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.