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Physical Review A

Atomic decay in saturated resonant light scattering

B. R. Mollow

Published Feb 1, 1976• 29 citations
Publisher

Abstract

The emission spectrum is found for transitions between a pair of atomic levels which are coupled by a coherent applied field, in the case in which decay to other levels of lower energy takes place during the emission process. The problem is solved by first finding the spectral distribution of radiation emitted by an atom which is initially prepared in some combination of the two coupled states, and which then decays to states of lower energy. (The solution found to this initial-value problem is valid even when many photons are emitted before the decay takes place.) It is then shown how the solution so obtained may be used to describe the case in which the atom is continually excited to the pair of levels in question by a weak, incoherent pumping mechanism. Limiting cases are discussed and compared with those which apply when no decay out of the two-dimensional subspace of coupled states takes place. The method of solution, which is based on an evaluation of the appropriate atomic correlation function by means of the quantum fluctuation-regression theorem, is compared to the method of simply adding imaginary terms, proportional to the decay constants, to the state energies. The latter method is of far more restricted validity, in that it depends on a particular strong inequality which must be assumed to hold between the decay constants.

DOI
10.1103/physreva.13.758

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The excitation and decay probabilities for resonance scattering of radiation from an atom with two coupled excited states in an external static field are calculated as a function of time and frequency. Various oscillatory terms are found in the probabilities. These oscillations depend on the frequency of radiation, the external coupling and the energy difference between the excited states. Two special cases are investigated in detail. In the first case where one of the excited states does not decay a 'hole' appears in the emission line at a frequency equal to the frequency difference between the ground state and the unperturbed non-decaying excited state. In the second case where the two excited states decay with the same rate, one of the two lines in the emission spectrum is suppressed and the other is enhanced.

Journal of Physics B Atomic and Molecular Physics•Jun 1, 1974•3 citations
The emission spectrum is found for transitions between a pair of atomic levels which are coupled by a coherent applied field, in the case in which decay to other levels of lower energy takes place during the emission process. The problem is solved by first finding the spectral distribution of radiation emitted by an atom which is initially prepared in some combination of the two coupled states, and which then decays to states of lower energy. (The solution found to this initial-value problem is valid even when many photons are emitted before the decay takes place.) It is then shown how the solution so obtained may be used to describe the case in which the atom is continually excited to the pair of levels in question by a weak, incoherent pumping mechanism. Limiting cases are discussed and compared with those which apply when no decay out of the two-dimensional subspace of coupled states takes place. The method of solution, which is based on an evaluation of the appropriate atomic correlation function by means of the quantum fluctuation-regression theorem, is compared to the method of simply adding imaginary terms, proportional to the decay constants, to the state energies. The latter method is of far more restricted validity, in that it depends on a particular strong inequality which must be assumed to hold between the decay constants.
A fully quantum-mechanical treatment of resonant light scattering is presented. The incident field is assumed to be described by a coherent state, and is allowed to be intense enough to cause saturation. Complete solutions are obtained for the correlated atom-field pure state vector, including multiphoton contributions of arbitrary order. The frequency spectrum of the scattered field is evaluated and is found to agree exactly with the result previously obtained by means of the quantum fluctuation-regression theorem. A derivation of the fluctuation-regression theorem and of the optical Bloch equations is given which is fully quantum mechanical and which relies upon no assumption of statistical factorization of atom and field states. The accuracy of the result found for the scattered - field spectrum is thus shown to be limited only by the assumption of the smallness of the saturated linewidth compared to the (optical) atomic resonance frequency. The one-photon approximation is analyzed in some detail. The method of adding an imaginary term to the upper-atomic-state energy is clarified, and it is shown how the vacuum and one-photon amplitudes thereby obtained may be used, within a simple and plausible iteration scheme, to construct the complete multiphoton spectrum. A variety of commonly used injection schemes and methods of representing atomic relaxation are discussed, and comparisons are made with results found by other authors. The entire analysis is performed with the aid of a canonical transformation which replaces the applied field by a ccc number. It is thus proved quite rigorously and generally that the use of a ccc-number applied field is a fully quantum-mechanical procedure, provided only that radiation-reaction terms are retained.
Spontaneous emission competes with stimulated emission in many interactions of light with matter. In the usual analyses which describe the interaction of an atom with a coherent optical field, the spontaneous emission characteristics, e.g., probability and spectral distribution, are not determined. The spontaneous emission from an atom which interacts with a coherent light wave is considered. The competition between coherent photons and spontaneous photons is treated in detail for a system consisting of a stationary atom, an open cavity and spatial fields. In the model chosen, a multilevel atom which spontaneously decays by interacting with spatial fields has two nondegenerate states coupled by an interaction with a single mode of the cavity. The Laplace-transformed Schrodinger equation is solved for specified initial conditions of the system. It is found that the interaction with the coherent field modifies the spectral distribution of spontaneous radiation from the atom. For spontaneous transitions involving an atomic state which interacts with the coherent field, the spectral distributions can no longer be described by Lorentzian functions. The new distributions exhibit a broadening and splitting for strong interactions between the atom and the coherent field. It is shown that the qualitative features of these distributions can be predicted from the energy-level diagram of the atom-cavity system. The net probability of the system gaining a coherent or cavity photon is calculated by integrating over the emitted spontaneous frequencies. The equivalence of this approach to the method of computing probabilities by integrating over time is demonstrated by using Parseval's theorem.
We study the dynamics of a system consisting of a two-level atom and a quantum oscillator coupled by the vacuum radiation field. The oscillator and the atom are assumed to have the same resonance frequency. In contrast to the two-atom or two-oscillator case, the atom-oscillator system leads to an unclosed hierarchy of equations for the operators that determine the radiation pattern emitted by the atom-oscillator system. Instead of using the operator equations, we formulate the problem in terms of density-matrix equations which can be solved once the initial conditions are specified. As an example, we looked at the radiation pattern, the decay dynamics, and the spectrum for an initial condition in which the oscillator is in its n=1n=1n=1 state and the atom is in its excited state. Dressed states (dressed by the static interaction between the atom and oscillator) prove to be especially useful for interpreting the results and comparing them with the two-atom and two-oscillator systems. All calculations are carried out using the resonance or rotating-wave approximation. The relationship of our work to damped Jaynes-Cummings models is noted.
Interaction with a multimode quantized radiation field of an assembly of NNN two-level atoms contained in a small volume is considered for the special cases of (i) highly excited, (ii) weakly excited, and (iii) superradiant atomic assemblies, and solutions of equations of motion are obtained in closed form. For (i) and (ii) we show that, if the atomic assembly is in the Dicke state ∣r,m>|r,m>∣r,m>, the spontaneously emitted radiation is Lorentzian, and its spectral width and the numerical value of the Lamb shift are r+∣m∣r+|m|r+∣m∣ times that for a single excited atom. For (i) the sign of Lamb shift is opposite to that for (ii) and for a single excited atom. Change in the frequency shift gives chirping in the pulse radiation emitted spontaneously by an assembly of atoms. We obtain the reduced density operator for a single mode and for the complete spontaneous emitted radiation, and discuss its characteristic function, weight function in diagonal representation, coherence functions, and normalized variance. We find that the emitted radiation is chaotic if all atoms are excited or if the assembly is weakly excited and is in thermal equilibrium. For a superradiant assembly, the radiation is coherent; it is only amplitude coherent if the initial atomic density operator is nondiagonal. We also study stimulated emission and scattering for the cases (i) and (ii). For case (iii) these phenomena do not take place.
The interaction between the electromagnetic field and a number of identical atomic systems, individually characterized by an electric dipole moment and two energy levels, is analyzed for the case where the atomic systems are inside a lossy cavity and exposed to a coherent driving field, resonance being assumed between atomic system, cavity, and driving field.The problem of introducing loss into a quantum-mechanical formalism is treated first. Formal operator expressions are obtained for the field variables which include the absorption and the fluctuation (both thermal and quantum-mechanical) effects of the loss mechanism. Expectation values are then obtained for the field strength and the field energy which are valid for times short compared to the lifetime of the excited state. It is shown that the spontaneous-emission energy in the field increases initially as the square of the time and approaches a steady-state value after a transient period which is of the order of the cavity relaxation time. The induced emission contains two parts: incoherent emission induced by the thermal field, and coherent emission induced by the driving field. The incoherent induced-emission energy has the same time dependence as the spontaneous-emission energy, and the ratio of the former to the latter is the number of photons in the thermal (inducing) field. The coherent induced-emission energy does not approach a steady-state value, but, after a transient period, increases linearly with the time. The ratio of the coherent induced-emission energy to the spontaneous-emission energy is equal, initially, to the number of photons in the driving-field energy, but becomes $\ensuremath{\beta}t$ times as large after the transient period, where $\ensuremath{\beta}$ is the reciprocal of the cavity relaxation time.The expectation value of the rate of energy emission by the atomic systems is also obtained. It is shown that the ratio of the downward to the upward transition probabilities has the well-known value of (n+1)n\frac{(n+1)}{n}n(n+1)​, where nnn is the field energy in units of the photon energy, only in the absence of a coherent field.
The excitation and decay probabilities for resonance scattering of radiation from an atom with two coupled excited states in an external static field are calculated as a function of time and frequency. Various oscillatory terms are found in the probabilities. These oscillations depend on the frequency of radiation, the external coupling and the energy difference between the excited states. Two special cases are investigated in detail. In the first case where one of the excited states does not decay a 'hole' appears in the emission line at a frequency equal to the frequency difference between the ground state and the unperturbed non-decaying excited state. In the second case where the two excited states decay with the same rate, one of the two lines in the emission spectrum is suppressed and the other is enhanced.