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Journal of Physics C Solid State Physics

Cooperative radiation from highly excited magnetic insulators

Keisuke Nakamura, Satoru Sugano

Published Dec 7, 1975• 5 citations
Publisher

Abstract

Following the methods of Dicke, the authors study the cooperative emission of light which is produced from a periodic linear lattice consisting of N exchange-coupled two-level atoms. The atom-field coupling is assumed to be much smaller than the atom-atom coupling, as in the case of both parity- and spin-forbidden optical transitions in magnetic insulators. Numerical computations show that enhanced radiation may be produced by some highly excited quasi-equilibrium states. Using analytical calculations, the rate of the strongest radiation is shown to be proportional to N 1.5 when the interaction of atomic excitations is absent though the transfer of atomic excitations is operative. The pair correlation between transition dipole moments in the state bearing such a rate is examined, as well as the effect of a non-vanishing propagation vector of light. Finally, the crucial role of rapid non-radiative relaxations is pointed out, in observing these enhanced radiations.

DOI
10.1088/0022-3719/8/23/020

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Following the methods of Dicke, the authors study the cooperative emission of light which is produced from a periodic linear lattice consisting of N exchange-coupled two-level atoms. The atom-field coupling is assumed to be much smaller than the atom-atom coupling, as in the case of both parity- and spin-forbidden optical transitions in magnetic insulators. Numerical computations show that enhanced radiation may be produced by some highly excited quasi-equilibrium states. Using analytical calculations, the rate of the strongest radiation is shown to be proportional to N 1.5 when the interaction of atomic excitations is absent though the transfer of atomic excitations is operative. The pair correlation between transition dipole moments in the state bearing such a rate is examined, as well as the effect of a non-vanishing propagation vector of light. Finally, the crucial role of rapid non-radiative relaxations is pointed out, in observing these enhanced radiations.
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.
We present an exact, analytic solution for the probability of radiative, cooperative transitions of stationary, weakly coupled atoms in strong light fields. Very simple expressions are obtained for pair-emission and -absorption probabilities by use of the ``dressed-atom'' formalism applied to atoms in solids or nearly at rest in optical traps. Analogies between radiative collisions in gases and the pair transitions encountered in solids, which may be viewed as ``frozen'' radiative collisions, are explored. Conditions are predicted for the occurrence of electric dipole decoupling in the presence of a suitable rotating electric field, similar to the well-known phenomenon of ``magic-angle'' decoupling of magnetic spins due to a rotating magnetic field. Observations of this new effect should permit precision determinations of interaction Hamiltonians in optical pair systems.
Fully-excited two-level atoms separated by less than the transition wavelength cooperatively emit light in a short burst, a phenomenon called superradiance by R. Dicke in 1954. The burst is characterized by a maximum intensity scaling with the square of the number of atoms NNN and a temporal width reduced by NNN compared to the single atom spontaneous decay time. Both effects are usually attributed to a synchronization of the electric dipole moments of the atoms occurring during the process of light emission. Contrary to this explanation, it was recently shown by use of a quantum path description that the peak intensity results from the quantum correlations among the atoms when occupying symmetric Dicke states. Here we investigate from this perspective the temporal evolution of the ensemble, starting in the small sample limit, i.e., when the atoms have mutual separations much smaller than the transition wavelength λλλ and pass down the ladder of symmetric Dicke states. In addition, we explore the temporal evolution for the case of non-interacting atoms with mutual separations much larger than λλλ. We show that in this case a similar superradiant burst of the emitted radiation is observed if the quantum correlations of the atoms are generated by conditional photon measurements retaining the atomic ensemble within or close to the symmetric subspace.
We study cooperative effects on the radiation interaction of a pair of two-level atoms with a spatial separation r\ensuremath{\ll}${\ensuremath{\lambda}}_{0}$ much closer than the optical wavelength of the dipole transition. In this regime we allow for charge exchange between the atoms (hybridization), which leads to qualitatively different behavior in contrast to an isolated pair of atoms because of the presence of the monopole Coulomb interaction. The interaction of the atoms with the radiation field and an external classical driving field is treated within a master equation approach. The numerical as well as the analytical results indicate the existence of quantum beats in the radiative decay of the system. In the case of an external driving field the system shows a dark resonance for a fixed detuning independent of the strength of the external field.
Radiative coupling between identical atoms sharing an excitation is studied in media where dispersion creates photonic band gaps, i.e., forbidden bands of light propagation for all directions and polarizations. Photonic band gaps can exist in media whose dielectric index exhibits strong three-dimensionally periodic modulations (``photonic crystals'') or in bands of polaritonic media. It is shown that the resonant dipole-dipole interaction as well as cooperative fluorescence of two-atom systems can be strongly enhanced or suppressed, to the extent of being essentially eliminated, by one of the following mechanisms: (a) dependence on location of the atoms within a unit cell of a photonic crystal, i.e., sensitivity to the spatial variation of the field normal modes; (b) dependence on the density of normal modes in allowed bands and on the density of virtual (evanescent) modes in band gaps. The ability to suppress the dipole-dipole interactions at interatomic separations characterizing quasimolecules would have far-reaching implications on their dissociative or collisional dynamics, spectroscopy, and rates of energy transfer.
The interaction between electromagnetic radiation and two three-level atoms is investigated. The atom-atom separation is assumed to be smaller than the corresponding mean resonance wavelength. The total radiance rate of the atomic system is calculated as a function of time. Explicit results are given for several different initial states of the atomic system. Some of them exhibit superradiance, and some act as photon-trapping states. Instead of exponential decay, the oscillations appear in the time evolution of the radiation rate due to the correlation between atoms. The decay constants and coupling decay constants show strong effects on the emission rates. Completely differing from two identical double-level atoms, the cooperative effects always exist in the three-level atomic system except for the case in which the coupling decay constants ${\ensuremath{\gamma}}_{12}$ and ${\ensuremath{\gamma}}_{21}$ are zero.