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Physical Review A

Master-equation approach to collisionally induced absorption and emission

G. Alber, J. Cooper

Published May 1, 1986• 14 citations
Publisher

Abstract

We study the collisionally induced excitation and photon emission of a neutral radiator atom surrounded by a gas of neutral foreign perturbers within the binary-collision approximation. We derive an equation of motion for the reduced density matrix of the radiator and obtain the spectrum of the spontaneously emitted photons including components due to collisionally induced radiation and to Rayleigh scattering, which is valid in both impact and quasistatic regimes. In our formulation single and subsequent collisional contributions are taken into account, and various coherent and incoherent corrections are examined.

DOI
10.1103/physreva.33.3084

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We study the collisionally induced excitation and photon emission of a neutral radiator atom surrounded by a gas of neutral foreign perturbers within the binary-collision approximation. We derive an equation of motion for the reduced density matrix of the radiator and obtain the spectrum of the spontaneously emitted photons including components due to collisionally induced radiation and to Rayleigh scattering, which is valid in both impact and quasistatic regimes. In our formulation single and subsequent collisional contributions are taken into account, and various coherent and incoherent corrections are examined.
The effect of correlations between an absorber atom and perturbers in the binary-collision approximation are applied to degenerate atomic systems. A generalized absorption profile which specifies the final state of the atom after an absorption event is related to the total intensities of Rayleigh scattering and fluorescence from the atom. It is suggested that additional dynamical information to that obtainable from ordinary absorption experiments is required in order to describe redistributed atomic radiation. The scattering of monochromatic radiation by a degenerate atom is computed in a binary-collision approximation; an equation of motion is derived for the correlation function which is valid outside the quantum-regression regime. Solutions are given for the weak-field conditions in terms of generalized absorption and emission profiles that depend on the indices of the atomic multipoles.
We present a calculation of the scattering of monochromatic radiation by a degenerate atom in the binary-collision approximation. We limit ourselves to field strengths such that $\ensuremath{\Omega}{\ensuremath{\tau}}_{c}\ensuremath{\ll}1$, where $\ensuremath{\Omega}$ is the Rabi frequency for the atomic transition, and ${\ensuremath{\tau}}_{c}$ is the duration of a strong collision. Our calculation is not limited to the impact regime, $\ensuremath{\Delta}\ensuremath{\omega}\ensuremath{\ll}{\ensuremath{\tau}}_{c}^{\ensuremath{-}1}$, or to the region where thermal correlations may be neglected, i.e., $\ensuremath{\Delta}\ensuremath{\omega}\ensuremath{\ll}\frac{\mathrm{kT}}{\ensuremath{\hbar}}$. (Here $\ensuremath{\Delta}\ensuremath{\omega}$ is the difference between either the incoming or outgoing photon's frequency and the atom's natural frequency.) To do this we derive an equation of motion for the correlation function, valid outside the quantum-regression regime, whose solution for practical cases is straightforward. We present solutions for the weak-field (linear-response) regime in terms of generalized absorption and emission profiles that depend on the indices of the atomic multipoles created.
Perturbation theory for the interaction of light with a binary collisional system is applied to the calculation of line profiles, spontaneous emission rates and absorption or stimulated emission coefficients. For the usual radiation fields are perturber densities, this approximation is valid at all detunings Delta omega except the very narrow resonance region. Appropriate expansions of the total binary system wavefunctions give the emission and absorption profiles or rates, for atom-electron systems as well as for atom-atom systems, from the impact regime at small Delta omega up to the Born-Oppenheimer regime at very large Delta omega in collision-induced radiative transitions, the transitions being asymptotically allowed or forbidden. Emphasis is given to the proper averages and sums over initial and final states of the binary system which give rise to non-adiabatic effects. One shows that it is of crucial importance to include all dynamical effects during one collisional event before undertaking any calculation at small Delta omega where simultaneous collisions may occur.
We apply the analysis of paper I to degenerate atomic systems and calculate the effect of correlations between an atom (the absorber) and perturbers in the binary-collision approximation. The result of our calculation is a generalized absorption profile that specifies the final state of the atom an absorption event. This profile is then related to the total intensities of Rayleigh scattering and fluorescence (redistributed radiation) from the atom. The profile is expressed in terms of collision operators that depend on the index of the multipole of the atom that is created. Some of the operators represent correlations between radiative and collisional events and cannot, except in certain limits, be expressed in terms of the usual line-broadening operators. This, of course, implies that one needs extra dynamical information, on top of that obtainable from ordinary absorption experiments, to be able to describe redistribution. Conversely, redistribution offers a probe of collisional dynamics, not given by absorption experiments, via the polarization of fluorescent light. We give practical expressions for the calculation of these operators and discuss their implications.
As a first step in deriving accurate, calculable expressions for collisional redistribution of radiation, valid outside the impact regime, we present a method for calculating an accurate binary-collision density operator for an atom in the presence of a driving field and perturbers. We use projection-operator techniques to establish first the precise validity of the Markoff approximation for radiative relaxation. Using the same techniques, we show how the collisional-relaxation problem may be analyzed in a practical manner outside the Markoff approximation. The effect of correlations between radiative and collisional events is included in a consistent way, and the physical implications of these correlation effects are demonstrated for a simple example, the two-level atom with nondegenerate levels.
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​〉.