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Physical Review A

Pure-state analysis of resonant light scattering: Radiative damping, saturation, and multiphoton effects

B. R. Mollow

Published Nov 1, 1975• 396 citations
Publisher

Abstract

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 $c$ number. It is thus proved quite rigorously and generally that the use of a $c$-number applied field is a fully quantum-mechanical procedure, provided only that radiation-reaction terms are retained.

DOI
10.1103/physreva.12.1919

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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.
A quantum statistical theory of resonant optical phenomena is developed for the case when the fluctuations of the laser, used for exciting transitions, are important. The general equations describing the dynamics of a relaxing two-level atom (TLA) are solved exactly for different types of mean values and the two-time amplitude and intensity correlations. The phase-diffusion model is adopted for laser fluctuations. The exact results are used to analyze the effect of laser fluctuations on a number of optical effects-optical free-induction decay, adiabatic following, the spectrum of the scattered light from a relaxing TLA, the energy-absorption spectrum from a weak field, Hanle resonances, etc. In each case, the laser fluctuations are found to affect in an important way the characteristics of the above optical-resonance phenomena. For example, the spectrum of scattered radiation from a TLA has the usual three-peak structure for fields at resonance and with strengths $\ensuremath{\alpha}$ above the threshold and for $\ensuremath{\alpha}\ensuremath{\gg}{\ensuremath{\gamma}}_{c}$; however, now the peak heights (widths) are in the ratio 3x3x3x (23x\frac{2}{3x}3x2​), $x=\frac{[{\ensuremath{\gamma}}_{c}+\frac{({T}_{1}^{\ensuremath{-}1}+{T}_{2}^{\ensuremath{-}1})}{3}]}{[2{\ensuremath{\gamma}}_{c}+{T}_{2}^{\ensuremath{-}1}]}$, where ${\ensuremath{\gamma}}_{c}^{\ensuremath{-}1}$ is the correlation time for laser phase fluctuations. For ${\ensuremath{\gamma}}_{c}\ensuremath{\gg}\ensuremath{\alpha}$, one gets a single-peak spectrum. The laser field is treated as a second-quantized field with excitation in either a coherent state or a Fock state. The results, obtained by straightforward perturbation theory, but valid for arbitrary values of the relaxation parameters, detuning, and the laser correlation time, are also presented.
We study interactions of light with a sample of two-level atoms. Quantum statistical effects of degenerate boson and fermion gases are described by using the quantum field theory of atom-photon interactions, fully including the angular momentum degeneracies. Coupled propagation equations are given for light and matter fields, and plausible general simplifications are enumerated.^ In the limit of large atom-field detuning, multiple scattering of light and QED linewidths and line shifts may be ignored, and the propagation equations of light and matter fields may be decoupled. A general expression for the spectrum of the scattered light is derived, complete with the dependence on atomic level scheme, on various light polarizations, and on the geometry of the experiment. With these simplifications we are able to find distinct qualitative features in the spectrum of the scattered light in the case of both fermions and bosons that depend on the statistics of atoms. This is because for bosons (fermions), those scattering events in which an atom recoils to an already occupied state are enhanced (inhibited).^ As the driving light gets closer to the atomic resonance, multiple scattering and vacuum fluctuations of the electromagnetic fields should also be taken into account. We write the equations of motion for the excited state field operators by eliminating the vacuum electromagnetic field. It is always assumed that the driving external laser field is in the coherent state. We find in the limit of low light intensity, a hierarchy of equations of motion for correlation functions that contain one excited-atom field and one, two, three, etc., ground state atom fields. It is conjectured that the entire linear hierarchy may be solved by solving numerically the classical equations for the coupled system of electromagnetic fields and charged harmonic oscillators. We discuss the emergence of resonant dipole-dipole interactions and collective linewidths, and delineate the limits of validity of the column density approach in terms of non-cooperative atoms by presenting a mathematical example in which this approach is exact. ^
In this theoretical paper, we investigate coherence properties of the near-resonant light scattered by two atoms exposed to a strong monochromatic field. To properly incorporate saturation effects, we use a quantum Langevin approach. In contrast to the standard optical Bloch equations, this method naturally provides the inelastic spectrum of the radiated light induced by the quantum electromagnetic vacuum fluctuations. However, to get the right spectral properties of the scattered light, it is essential to correctly describe the statistical properties of these vacuum fluctuations. Because of the presence of the two atoms, these statistical properties are not Gaussian: (i) the spatial two-points correlation function displays a specklelike behavior and (ii) the three-points correlation function does not vanish. We also explain how to incorporate in a simple way propagation with a frequency-dependent scattering mean-free path, meaning that the two atoms are embedded in an average scattering dispersive medium. Finally we show that saturation-induced nonlinearities strongly modify the atomic scattering properties and, as a consequence, provide a source of decoherence in multiple scattering. This is exemplified by considering the coherent backscattering configuration where interference effects are blurred by this decoherence mechanism. This leads to a decrease of the so-called coherent backscattering enhancement factor.
Resonant two-photon absorption is discussed for the case in which the exciting field may be intense enough and near enough to resonance to cause appreciable saturation. A single pair of levels in an otherwise quite general atom is assumed to satisfy the appropriate resonance condition, and equations are derived governing the time evolution of the associated 2 \ifmmode\times\else\texttimes\fi{} 2 submatrix of the full atomic density matrix. Atomic relaxation is treated explicitly. The analysis, which treats both inversion-symmetric and inversion-nonsymmetric cases within the same general formalism, is developed systematically, the necessary approximations receiving careful discussion. The results are analogous to those for the corresponding one-photon process, but with a shift in the resonance frequency proportional to the intensity of the exciting field. This frequency shift is not identical to the one calculated by time-independent (second-order) perturbation theory, and becomes large when the energy of an intermediate state of the atom approaches the mean of the energies of the active states.
The resonant response of a multilevel atomic system to strong coherent radiation is analyzed using an extension of the methods of time-independent scattering theory, adapted to the density-matrix formalism in order to include thermal bath effects. General steady-state expressions are derived for self-attenuation and resonance scattering rates in strong saturating fields, as functions of the coupling strengths, relaxation parameters, and frequency detunings. Formal expressions are given for radiative-damping and collision-broadening relaxation parameters, relating the latter to scattering amplitudes. Modifications of collision-broadening parameters by the presence of very strong fields are discussed. The Bloch equations are derived by transformation to the time domain, under specified conditions.
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.