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Physical Review

Stochastic Theory of the Resonant Scattering of Photons

David L. Huber

Published Jun 10, 1968• 75 citations
Publisher

Abstract

The resonant scattering of photons from a perturbed two-level system is studied in detail. Adiabatic perturbations are approximated by a randomly fluctuating term in the level splitting. Off-diagonal perturbations are accounted for in the linewidth and the time dependence of the correlation functions. Explicit expressions for the cross section are obtained in the statistical and motional-narrowing limits. The detailed-balancing symmetry of the scattering is established. Minor modifications of the approximate expressions for the cross sections are proposed in order to preserve this symmetry. The effects of off-diagonal perturbations, which couple the atom to a thermal bath, are investigated at length for a model interaction.

DOI
10.1103/physrev.170.418

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We investigate the resonant scattering of photons from an atom in the thermal equilibrium with a phonon bath. A two-level model of the atom is discussed in detail. In the model problem, the atom is coupled directly to the lattice through a diagonal interaction which is bilinear in the lattice quanta. Relaxation effects are introduced indirectly via correlation functions. In the limit in which the relaxation time is much shorter than the radiative lifetime, the frequency spectrum of the scattered radiation consists of three parts: (1) a coherent, elastic term weighted by the factor ${tanh}^{2}(\frac{\ensuremath{\hbar}{\ensuremath{\omega}}_{0}}{2KT})$, (2) an incoherent quasielastic term weighted by the factor [$1\ensuremath{-}{tanh}^{2}(\frac{\ensuremath{\hbar}{\ensuremath{\omega}}_{0}}{2KT})$], (3) a fluorescent term characterizing emission at the natural frequency ${\ensuremath{\omega}}_{0}$, which arises from an effective two-photon-two-phonon interaction. The extension of the analysis to the problem of resonant scattering from paramagnetic ions in crystals is outlined with particular emphasis on the influence of neighboring ionic levels and the relative importance of the one- and two-phonon processes.
A theoretical study is presented of the effects of collisional perturbations on the time-resolved resonant and near-resonant photon scattering from a molecular system. The photon counting rate is formulated in terms of tetradic Green's functions in Liouville space. The collisional and radiative damping effects are handled by an effective-Liouvillian formalism. The formal expressions are disentangled by invoking a series of successive approximations, assuming short correlation times of the thermal bath, neglecting relaxation processes in the ground electronic state, considering rotational relaxation as providing the dominant damping mechanism in the excited electronic manifold, specializing to weak electromagnetic fields, neglecting some off-resonance processes and disregarding collision-induced radiative processes. The photon counting rate is expressed as a triple convolution of the photon counting rate for the free molecule with the Doppler Gaussian profile and with a Lorentz profile. The latter incorporates purely collisional effects due to intrastate cross relaxations and proper T2{T}_{2}T2​ processes. The theory accounts well for the recent experimental data of Williams, Rousseau, and Dworetsky on collisionally perturbed I2{\mathrm{I}}_{2}I2​ molecules.
We present a general microscopic theory for near resonance light scattering (RLS) from collisionally perturbed atoms and molecules. The theory is based on the tetradic scattering formalism of Fano and Ben-Reuven. We perform a systematic density expansion and show that the four-time, many-body, dipole correlation functions necessary for the evaluation of the RLS cross section may be rigorously expressed (to lowest order in pressure) in terms of three single-particle, two-time, correlation functions, two of which are associated with the absorption and emission line broadening and the third is a cross correlation function. Our most general expressions are valid for an arbitrary value of the bath correlation time (relative to the broadening), and interpolate smoothly all the way from the static limit of inhomogenous broadening up to the reverse, the Markovian (homogenous) limit. The stochastic Gaussian model of Takagahara, Hanamura, and Kubo is obtained also as a special case of the present formulation.
Quantum stochastic differential equations have been used to describe the dynamics of an atom interacting with the electromagnetic field via absorption/emission processes. Here, by using the full quantum stochastic Schrödinger equation proposed by Hudson and Parthasarathy, we show that such models can be generalized to include other processes into the interaction. In the case of a two-level atom we construct a model on the basis of some physical requirements, the main being a balance equation on the fluxes of the ingoing and outgoing photons; in this model the atom-field interaction turns out to be due either to absorption/emission processes either to direct scattering processes, which simulate the interaction due to virtual transitions to the levels which have been eliminated from the description. To see the effects of the new terms, we consider both direct and heterodyne detection of the fluorescence light emitted by an atom stimulated by a monochromatic coherent laser and we deduce from these two detection schemes the expressions of the total, elastic and inelastic electromagnetic cross sections and the spectral distribution of the fluorescence light. The total cross section, as a function of the frequency of the stimulating laser, can present not only a Lorentzian shape, but the full variety of Fano profiles; intensity dependent widths and shifts are obtained. The fluorescence spectrum can present complicated shapes, according to the values of the various parameters; when the direct scattering is not important the usual symmetric triplet structure of the Mollow spectrum appears (for high intensity of the stimulating laser), while a strong contribution of the direct scattering process can distort such a triplet structure or can even make it to disappear.
The behaviour of a two-level atom saturated by a resonant fluctuating laser beam is studied. A classical description of the light wave is used, corresponding to a laser well above threshold. Two different approximations are introduced for treating the effects of slow and fast fluctuations; slow fluctuations are followed adiabatically by the atom and fast fluctuations appear as a relaxation mechanism for the population difference and for the optical dipole moment obeying the motional-narrowing condition. The perturbation of the spectral distribution of the fluorescence light is determined quantitatively and the great sensitivity of this spectrum to higher order correlation functions of the light wave is exhibited.