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Physical Review

Effective Operator Formalism in Optical Pumping

W. Happer, B.S. Mathur

Published Nov 5, 1967• 249 citations
Publisher

Abstract

Real and virtual absorption of weak monochromatic light is analyzed with semiclassical radiation theory. The influence of the light on the atoms is described by an effective ground-state Hamiltonian operator, and the effect of the atoms on the light is described by a dielectric susceptibility operator. These operators are expressed explicitly in terms of familiar ground-state observables, angular factors, oscillator strengths, and plasma dispersion functions. The theory gives a comprehensive description of optical pumping, light shifts, and light modulation due to real and virtual absorption of light, and several new effects are predicted. Repopulation of the atomic ground state from a polarized excited state is not considered in this paper.

DOI
10.1103/physrev.163.12

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Physical Review A•Oct 1, 1970•31 citations
Real and virtual absorption of weak monochromatic light is analyzed with semiclassical radiation theory. The influence of the light on the atoms is described by an effective ground-state Hamiltonian operator, and the effect of the atoms on the light is described by a dielectric susceptibility operator. These operators are expressed explicitly in terms of familiar ground-state observables, angular factors, oscillator strengths, and plasma dispersion functions. The theory gives a comprehensive description of optical pumping, light shifts, and light modulation due to real and virtual absorption of light, and several new effects are predicted. Repopulation of the atomic ground state from a polarized excited state is not considered in this paper.
The propagation of light in an optically pumped vapor is determined semiclassically by the expectation value of a dielectric susceptibility operator. We present explicit formulas for the dielectric susceptibility of a vapor of alkali atoms. The qualitative features of the susceptibility are illustrated for the specific case of Rb87{\mathrm{Rb}}^{87}Rb87. The theory of this paper is essential for a clear understanding of phenomena such as the birefringence of alkali vapors and the microwave modulation of light by alkali vapors. Some experimental observations of birefringence in rubidium vapor are interpreted with the semiclassical theory.
Abstract This present paper is an attempt to describe the operation of a laser by a method patterned closely after the classical theory of dispersion. There, the electromagnetic field is treated as a classical system interacting with a collection of classical harmonic oscillators which are at rest. In the present case the radiation field is still treated classically, but, in accordance with the correspondence principle, the oscillators are now virtual oscillators associated with the up-and-down transitions in effective two-state atoms which are described quantum mechanically. The atoms carrying these virtual oscillators are not at rest but move with different velocities. We show how the Lorentz averaging can be performed for such systems, and derive a closed set of equations linking the average electric field E, with the average polarization density P„ and the average population inversion density Mp associated with atoms moving with the velocity v. Next, we investigate the conditions for the existence of a steady state if pumping is present, and if the electric field is represented by a standing wave, or a travelling wave of a single frequency (single-mode case). It turns out that, notwithstanding the nonlinear nature of the equations, the steady-state conditions give a simple complex dispersion relation; moreover, the real and imaginary part of this dispersion relation are equivalent to the usual heuristic expressions which specify the operating frequency in terms of the index of refraction and cavity length, and which balance the gain against the losses. The single-mode case is analysed in detail without any smallness assumptions for the resultant intensity. The small-intensity case gives the usual results exhibiting the tuning dip. For high intensities the relative depth of the dip tends to zero. At the end of the paper we discuss proposed extensions and additional applications.
Optical pumping of the electronic ground state of molecules has been investigated under conditions of plane, elliptically, and circularly polarized light broadband excitation. The analysis has been performed assuming arbitrary angular momentum values, and applying the apparatus of polarization moments, the latter forming the coefficients in the expansion of the density matrix over irreducible tensor operators, including simplifications due to asymptotic limits for large momentum values. In addition to accounting for the external magnetic field, attention has been also given to the dynamical Stark effect arising from the absence of coincidence between the centers of the exciting line and the absorption line. An alternative classical description is also proposed using multiple moments as coefficients of the expansion of a classical quasidensity of states over spherical harmonics. The equivalence of both approaches of description in the limit of infinitely large angular moments is demonstrated, and the meaning of the origin of coherence is clarified, as well as its destruction by the magnetic field in the classical description of the system.
According to the quantum theory of the optical-pumping cycle, one can describe the effect of a nonresonant light beam on the different Zeeman sublevels of an atomic ground state by an effective Hamiltonian He{\mathcal{H}}_{e}He​ which depends on the polarization and spectral profile of the incident light. In order to check the structure of He{\mathcal{H}}_{e}He​, we have performed a detailed experimental study of the ground-state energy sublevels of various kinds of atoms perturbed by different types of nonresonant light beams. Attention is paid to the modification of the Zeeman structure due to He{\mathcal{H}}_{e}He​. We have been able to obtain experimentally in the ground state of 199Hg^{199}\mathrm{Hg}199Hg, 201Hg^{201}\mathrm{Hg}201Hg, and 87Rb^{87}\mathrm{Rb}87Rb, Zeeman light shifts that are larger than the width of the levels due to the thermal relaxation. The removal of the Zeeman degeneracy in zero external field, due to a nonresonant light irradiation, is observed by different optical-pumping techniques; the full Zeeman diagram of the perturbed atoms is also determined when a static field ${\stackrel{\ensuremath{\rightarrow}}{\mathrm{H}}}_{0}$ is added. We have checked that the effect of He{\mathcal{H}}_{e}He​ can be described in terms of fictitious static electric or magnetic fields. These fictitious fields can be used to act selectively on a given atomic level.
The absorption of light by optically pumped atoms undergoing magnetic resonance is calculated from expressions based on a simplification of Barrat and Cohen-Tannoudji's theory of optical pumping. The density matrix for the system is first derived in orders of approximation which correspond to successive cycles of pumping. The off-diagonal elements of the matrix, and consequently the absorption of light, are modulated. The amplitudes of modulation are resonance functions which are, in general, more complicated than solutions of the Bloch equations. The selection rules for electric dipole radiation limit the possible frequencies of modulation to ω0 and 2ω0 for primary interactions (ω0 is the applied frequency), but modulation at higher frequencies can arise through the circulation of coherence in optical pumping cycles. The functions which represent the amplitude of modulation at 4ω0 are derived in first and second order, for comparison with experiment.
An improved form of semiclassical radiation theory is developed which includes the effect of the atom's radiation field back on the atom. This formalism is applied to the problem of a single two-level atom interacting with a monochromatic field. The resulting equations are solved without resorting to time-dependent perturbation theory, and are found to predict the behavior of the system over times long compared with the lifetime for spontaneous transitions. Not only stimulated emission and absorption, but also spontaneous emission with the proper Einstein AAA coefficient, and a frequency shift which agrees at least semiquantitatively with the Lamb shift are described. In addition, several nonlinear effects involving the interference between spontaneous and stimulated radiation are described, and new experiments which might detect such effects are suggested.