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Density matrix formalism applied to light beat experiments

J. P. BARRATt

Published Jan 1, 2016• 0 citations
OpenAlex

Abstract

Recent experiments (Dodd, Fox, Series & Taylor, I959; Colegrove, Franken, Lewis & Sands, i959) have shown that coherence effects can be observed between the Zeeman components of an optical line provided some coherence exists in the excited state. This coherence may be due to a radio-frequency field inducing transitions between the Zeeman sublevels of this excited state, or to the excitation process itself or to both. These effects are actually more or less a generalization of the well-known Hanle's experiments on the polarization of resonance radiation.: In the case of 'double resonance' experiments (Dodd et al. I959), they appear as a modulation of the intensity of the fluorescence radiation at one of the harmonics of the r.f. field; they can be interpreted as interference between the radiations of different frequencies emitted by the atoms which are submitted to the 'double resonance' ('light beat'). These coherence effects are related to those observed in the trapping of resonance radiation. In this paper, the methods used in former papers (Barrat I959 a, b and c, hereafter referred to as I, II, III) for the problem of light trapping are applied to the light beats experiments, using a density matrix formalism. The expression for the density matrix representing the states of the atoms just after the excitation will first be derived; then the intensity of the re-emitted light will be calculated. It will be shown finally how this method can be applied to practical problems. Notation unexplained in this paper is the same as in papers on coherence in light trapping (papers I, II and III).

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Recent experiments (Dodd, Fox, Series & Taylor, I959; Colegrove, Franken, Lewis & Sands, i959) have shown that coherence effects can be observed between the Zeeman components of an optical line provided some coherence exists in the excited state. This coherence may be due to a radio-frequency field inducing transitions between the Zeeman sublevels of this excited state, or to the excitation process itself or to both. These effects are actually more or less a generalization of the well-known Hanle's experiments on the polarization of resonance radiation.: In the case of 'double resonance' experiments (Dodd et al. I959), they appear as a modulation of the intensity of the fluorescence radiation at one of the harmonics of the r.f. field; they can be interpreted as interference between the radiations of different frequencies emitted by the atoms which are submitted to the 'double resonance' ('light beat'). These coherence effects are related to those observed in the trapping of resonance radiation. In this paper, the methods used in former papers (Barrat I959 a, b and c, hereafter referred to as I, II, III) for the problem of light trapping are applied to the light beats experiments, using a density matrix formalism. The expression for the density matrix representing the states of the atoms just after the excitation will first be derived; then the intensity of the re-emitted light will be calculated. It will be shown finally how this method can be applied to practical problems. Notation unexplained in this paper is the same as in papers on coherence in light trapping (papers I, II and III).
Abstract A theory is formulated to describe the modulation which has been observed in fluorescent light from atoms subjected simultaneously to optical and radio-frequency radiation. The optical field stimulates one or more of a set of excited states of the atom, between which the radio-frequency field establishes coherence. This coherence is manifest in the fluorescent radiation. Interference between radiations of different frequency leads to modulation. General expressions are given for the intensity of the fluorescent light as a function of time. The Zeeman structure of the transition (63P1 — 6 1S0), A2537 A, in mercury is studied in detail. Modulation at frequencies, 1, 2, 3 and 4 times that of the radio-frequency field, w0, is predicted, and resonant effects at static magnetic fields, 0, 1/2, 1, 3/2, 2 and 3 times H0, the field for which w0 is the Larm or frequency. Resonances at fields other than H0 are due to excitation with light of mixed polarization. Most of the predicted effects have been found experimentally. A ‘frequency diagram’ is introduced and discussed, to represent the combined effects of static and radio-frequency magnetic fields. To each excited state belong a set of r frequencies, where r is the number of states linked by the radio-frequency perturbation. The 9 levels are drawn, as functions of H, for the states mJ = 0, ± 1, of 3P1. The resonances at fields other than H0 may be associated with intersections of frequency levels belonging to different mJ.
From resonance equations using density matrix formalism, we obtain several features of rf or mw optical double resonance experiments at zero field. Resonance signal intensity formulas are derived. The question of the spatial and polarization dependence is then reduced to a minimum number of parameters through the use of multipole tensors; the effect of a resonance within the excited state is formulated as a redistribution of excited state multipole moments. In the case of transitions between hyperfine sublevels which are separated on the order of the natural linewidth, coherence is produced by interference between different rf-optical transition pathways. Depending on the method of detection, such interference may lead to a dispersion-shaped contribution to the ODR line shape, as observed in the experiments on the NO A state (Bergeman and Zare, accompanying paper). Second order radiation field corrections for multiplet transitions (generalizations of the Bloch-Siegert shift) are also derived.
The theory of double-resonance phenomena, or the simultaneous action of optical transitions and rf perturbations between the Zeeman sublevels of an atom, is extended to the induced emission and absorption processes effected by the monochromatic radiation and the discrete resonances involved in the gas laser. Expressions for the probability amplitudes of the Zeeman sublevels under such conditions are derived from time-dependent perturbation theory, the lifetimes of the states being introduced in a phenomenological way. Zeeman splittings of both upper and lower states involved in the laser transition are considered, and an effective term diagram used to discuss the results. Small signal approximations are applied to consider some specific cases, which show that the light beats seen in spontaneous emission when the rf frequency ${\ensuremath{\omega}}_{0}$ equals the Larmor frequency, and in other instances, do not occur in induced emission unless such frequencies coincide with axial resonances of the laser cavity. Variations in the intensity and resonance effects are indicated at Zeeman splittings corresponding to ${\ensuremath{\omega}}_{0}$, with similar variations in the amplitude of any beat frequencies due to multiple axial resonances. Additional coherence effects occur where levels cross, which will give rise to changes in the intensity and polarization of the induced emission at the corresponding frequency.
Abstract This work is an experimental study of the modulation which has been found in resonance radiation when the fluorescing vapour is subjected to static and radio-frequency magnetic fields, as in the double resonance experiment of Brossel & Bitter. The particular example chosen for study in this work also was the resonance line λ 2537 Å of mercury. The experimental observations are compared with the predictions of a theoretical treatment which has already been published. The phenomenon was studied under a variety of geometrical configurations. When the polarization of the exciting light allowed excitation to only one excited state (a component of a Zeeman multiplet), the depth of modulation was found to depend on the closeness to resonance of the frequency, ω0, of the radio-frequency field to the Larmor precessional frequency, ω = γH , in the static field H. When the polarization of the exciting light allowed excitation to more than one component of the multiplet, resonance effects were found in the depth of modulation and in the mean intensity of the fluorescent light at fields where the applied frequency was equal, not to the Larmor frequency alone, but to combinations of the Larmor frequency with the nutational frequency. From a quantum-mechanical point of view, these new phenomena are related to the interference effects which are found in resonance fluorescence when there is degeneracy between excited states: in the present case the degeneracy is induced by the radio-frequency field. The ease with which the geometrical conditions could be altered allowed the theory to be tested in considerable detail without quantitative assessment of the resonance line contours: nevertheless, a quantitative study was made of one particular feature. The predictions of the theory were confirmed at all points where they were tested.
Coherent-population-trapping resonance in vapor cell is a quantum interference effect that appears in the two-photon transitions between the ground-state hyperfine levels of alkali-metal atoms and is often utilized in miniature and centimeter-scale clock devices. To quantitatively understand and predict the performance of this phenomenon, it is necessary to consider the transitions and relaxations between all hyperfine Zeeman sublevels involved in the different excitation processes of the atom. In this paper, we constructed a computational multilevel atomic model of the Liouville density-matrix equation for 32 Zeeman sublevels involved in the D1{D}_{1}D1​ line of 133Cs^{133}\mathrm{Cs}133Cs irradiated by two frequencies with circularly polarized components and then simulated the amplitude and shape of the resonance spectrum of the transmitted light through centimeter-scale Cs-vapor cells. We show that the numerical solutions of the equation and analytical investigations adequately explain a variety of the characteristics observed in the experiment.