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Canadian Journal of Physics

Theory of resonance fluorescence from a gas of identical two level atoms

Haider R. Zaidi

Published Feb 1, 1983• 2 citations
Publisher

Abstract

A Green's function formulation of the problem of resonance fluorescence from a system of identical two level atoms is presented. The general formulation is suitable for the investigation of a variety of nonlinear phenomena, e.g., propagation of electromagnetic waves inside the medium, fluorescence from a finite medium, optical bistability, atomic correlations, and additional side bands. Translational motion, collisions, Coulomb dipole–dipole interaction, excitation transfer, and local field corrections are also included in the basic equations. The effect of atom–atom correlations in the relaxation mechanism (radiative or collisional) is also taken into account. Finally, the results are also presented in the "generalized dressed atom" (GDA) representation. Applications of the general theory will be given in a future paper.

DOI
10.1139/p83-030

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A Green's function formulation of the problem of resonance fluorescence from a system of identical two level atoms is presented. The general formulation is suitable for the investigation of a variety of nonlinear phenomena, e.g., propagation of electromagnetic waves inside the medium, fluorescence from a finite medium, optical bistability, atomic correlations, and additional side bands. Translational motion, collisions, Coulomb dipole–dipole interaction, excitation transfer, and local field corrections are also included in the basic equations. The effect of atom–atom correlations in the relaxation mechanism (radiative or collisional) is also taken into account. Finally, the results are also presented in the "generalized dressed atom" (GDA) representation. Applications of the general theory will be given in a future paper.
A Green's function formulation, valid for thermal as well as nonthermal equilibrium, is developed for the resonance fluorescence from strongly driven two level atoms. Translational motion and the Doppler broadening are also taken into account (collisions are considered in a second paper). The Feynman diagram technique is used to calculate the contribution of the physically important processes. The formulation is not based on the Markovian approximation or the quantum regression theorem. It takes full account of the dynamic Stark splitting and the saturation, and leads to a generalization of the "dressed atom" approach. Our "generalized dressed atom" (GDA) approach is valid for arbitrary values of the detuning and the pump field strength. The lowest order diagrams in the GDA picture give results equivalent to the existing theories. Some higher order diagrams are also considered. Although the resulting corrections are small, the physical processes involved are of some interest. These corrections include nonMarkovian effects.
A theoretical analysis is developed for the spectrum of the light scattered by two two-level atoms driven near resonance by an external coherent electromagnetic field. The atoms are assumed to relax to equilibrium with the driving field as a result of radiation damping. The explicit dependence of the coherent dipole-dipole interactions on the distance between the two atoms is taken into account. For the case of two two-level atoms with a fixed distance smaller than a wavelength, an analytical result for the resonance fluorescence line shape is obtained, and the result is compared to previous work.>
The excitation spectrum arising from photon density-density correlations has been considered in a system of two interacting identical atoms. The two-level atoms are pumped near resonance by a strong electromagnetic field while they interact through their dipole-dipole interaction and radiate to each other as well. In such a system the photon density-density correlations arise from the interference spectrum due to the beating of the frequency of the pump field and the atomic transition frequency, as well as from the spectrum induced by the dipole-dipole and radiative interactions between the atoms. The spectral function of this system has been calculated in the limit of high photon densities. It consists of four terms describing four bands which are similar to those appearing in the two-atom resonance fluorescence spectrum for the symmetric modes when the central peak is missing. The collective behavior as well as the dynamics of the system are discussed in detail. By using the spectral function, an expression for the photon density-density correlation function at different times has been derived where thermal effects have been also included.
The problem of resonant interaction between an electromagnetic radiation field and a vibronic system, such as a molecule or a localized electronphonon system, is considered. The vibronic coupling is assumed to result from displaced and distorted potential energy surfaces for the vibrational motion in the electronic quantum states involved in the resonant interaction with the radiation field. Furthermore, the vibrational energy relaxation is taken into account without assumptions about Markovian-type relaxation. In order to study correlation properties of higher than second order in the electric field strength of the light emitted a method of calculation of the expectation value of an arbitrary product combination of effective time evolution operators of the vibronic system is developed. The calculations are performed by utilizing Feynman's disentangling and operator ordering techniques and yield closed solutions in the low-temperature limit. The theory is used for studying the intensity and the normally ordered intensity correlation function of the resonance fluorescence light from a two-atom molecule excited by a relatively weak laser field, which undergoes phase fluctuations. It is shown that the vibronic coupling can give rise to an anticorrelation effect which is substantially stronger than in the case of resonance fluorescence from an atom. For the case of small vibrational damping a general formula which directly connects the asymptotic long-time behaviour of the normalized intensity correlation function with the vibrational relaxation in the molecule is deduced. It should be convenient for the determination of very small vibrational decay rates.
The response of a collision-broadened gas sample to driving coherent radiation is studied theoretically, taking into account effects of coherent excitations of two or more atoms (or molecules). In analogy to the Bloch-type master equation for one-atom coherences, describing the motion of a single atom "dressed" by the relevant (incident and detected) field modes, a master equation is derived for two-atom coherences, including an effective interaction of the Bethe-Salpeter---type, accounting for the mutual interaction of the coherently driven pair. The master equation includes also all symmetrization effects owing to resonance exchange between identical atoms, and is limited to nonreactive gas atoms (or molecules) undergoing binary collisions, including otherwise all (internal and translational) relaxation effects. The self-energy kernels are expressed in a nonperturbative fashion, in terms of binary-collision scattering amplitudes, and include renormalization effects due to coincidence of radiative couplings with the collisions (optical and radiative collisions). The concept of two-atom coherences is generalized to higher coherence ranks by constructing a hierarchy of master equations, including vertex operators that upgrade or downgrade the coherence rank, as a prelude to a diagrammatic method for calculating continuous-wave spectra. This hierarchy is compared with prevalent Agarwal-type master equations, based on the Dicke pseudospin method, and used in the study of two-level atoms.
The problem of resonance fluorescence from a two-level atom that is driven near resonance by a laser beam of finite bandwidth is tackled via the Heisenberg equations of motion, by a simple generalization of our previous treatment. It is found that the two-time intensity correlation function is again factorizable into a product of the mean light intensities at the two times, each of which is slightly modified under broad-band excitation from its value under monochromatic excitation. The spectrum of the fluorescence is affected rather more drastically, and, in general, becomes asymmetric under broad-band excitation.