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Proceedings of the Physical Society

Theory of resonance fluorescence excited by modulated or pulsed light

Alan Corney, George William Series

Published Feb 1, 1964• 101 citations
Publisher

Abstract

When resonance fluorescence is excited in atoms whose excited states have Zeeman or hyperfine structure, it is to be expected that the character of the fluorescent light will be affected if the intensity of the exiciting light is modulated or pulsed. An earlier theory of resonance fluorescence is developed to take account of such variations of the intensity of the exciting light. Resonance effects are predicted if the light is modulated at a frequency which coincides with a characteristic frequency of the atoms. A particular case, which has been studied experimentally, is worked out in detail. If the exciting light is pulsed, the prediction is that the fluorescent light will be modulated, in addition to being damped at the ordinary rate for spontaneous emission.

DOI
10.1088/0370-1328/83/2/304

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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.

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Resonance fluorescence

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The phenomenon of resonance fluorescence provides an interesting manifestation of the quantum theory of light and is a “real world” application of the material of the Chapters 8 and 9. In this process, a two-level atom is typically driven by a resonant continuous-wave laser field and the spectral and quantum statistical properties of the fluorescent light emitted by the atom are measured. Experimentally this can be achieved by scattering a laser off a collimated atomic beam such that the directions of the laser beam, atomic beam, and detector axis are mutually perpendicular as shown in Fig. 10.1. If the driving field is monochromatic, then at low excitation intensity the atom absorbs a photon at the excitation frequency and reemits it at the same frequency as a consequence of conservation of energy. The spectral width of the fluorescent light is therefore very narrow. The situation, however, is considerably more complicated when the excitation intensity increases and the Rabi frequency associated with the driving field becomes comparable to, or larger than, the atomic linewidth. At such intensity levels, the Rabi oscillations show up as a modulation of the quantum dipole moment and sidebands start emerging in the spectrum of the emitted radiation. This so-called dynamic Stark splitting is an interesting feature of the atom–field interaction. In addition to that, the fluorescent light exhibits certain nonclassical properties including photon antibunching and squeezing. In this chapter, we develop a theory of resonance fluorescence to explain these phenomena.

Cambridge University Press eBooks•Sep 4, 1997•0 citations
When resonance fluorescence is excited in atoms whose excited states have Zeeman or hyperfine structure, it is to be expected that the character of the fluorescent light will be affected if the intensity of the exiciting light is modulated or pulsed. An earlier theory of resonance fluorescence is developed to take account of such variations of the intensity of the exciting light. Resonance effects are predicted if the light is modulated at a frequency which coincides with a characteristic frequency of the atoms. A particular case, which has been studied experimentally, is worked out in detail. If the exciting light is pulsed, the prediction is that the fluorescent light will be modulated, in addition to being damped at the ordinary rate for spontaneous emission.
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.
A treatment of resonance fluorescence is given in which the properties of the incident and scattered light are expressed in terms of coherency matrices. Calculations are made for two successive scattering processes corresponding to the experiments described in an accompanying paper. For the first process the scattering atoms are subjected to a magnetic field consisting of parallel static and oscillating components. The fluorescent light is frequency-modulated and may also be polarization-modulated. This light excites fluorescence in a second cell in which the atoms are subjected to a static magnetic field. The equations show under what conditions the second fluorescence is intensity-modulated and describe the resonances in the amplitude of modulation which occur when the modulation frequency matches a Zeeman interval of the excited atoms.
Frequency-modulated light was generated by the application of a magnetic field oscillating at frequencies in the range 1-10 MHz to mercury vapour undergoing resonance fluorescence. The characteristics of the fluorescent light have been studied. When the primary illumination in the plane perpendicular to the field is anisotropic the sigma components are coherently excited. The light emitted along the field is then polarization-modulated. It becomes intensity-modulated if it is passed through a linear analyser. The light emitted obliquely to the magnetic field is intensity-modulated without passing through an analyser. The amplitudes of these modulations show resonance behaviour under the application of an additional static field parallel to the oscillating field. The polarization-modulated light was used to excite resonance fluorescence in a second cell of mercury vapour. The fluorescent light is intensity-modulated. The amplitude of modulation shows resonance behaviour when harmonics of the driving frequency coincide with Zeeman intervals in the excited atoms. These resonances have been explored in detail. They are satisfactorily interpreted by a theory given in an accompanying paper.
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.
The phenomenon of resonance fluorescence provides an interesting manifestation of the quantum theory of light and is a “real world” application of the material of the Chapters 8 and 9. In this process, a two-level atom is typically driven by a resonant continuous-wave laser field and the spectral and quantum statistical properties of the fluorescent light emitted by the atom are measured. Experimentally this can be achieved by scattering a laser off a collimated atomic beam such that the directions of the laser beam, atomic beam, and detector axis are mutually perpendicular as shown in Fig. 10.1. If the driving field is monochromatic, then at low excitation intensity the atom absorbs a photon at the excitation frequency and reemits it at the same frequency as a consequence of conservation of energy. The spectral width of the fluorescent light is therefore very narrow. The situation, however, is considerably more complicated when the excitation intensity increases and the Rabi frequency associated with the driving field becomes comparable to, or larger than, the atomic linewidth. At such intensity levels, the Rabi oscillations show up as a modulation of the quantum dipole moment and sidebands start emerging in the spectrum of the emitted radiation. This so-called dynamic Stark splitting is an interesting feature of the atom–field interaction. In addition to that, the fluorescent light exhibits certain nonclassical properties including photon antibunching and squeezing. In this chapter, we develop a theory of resonance fluorescence to explain these phenomena.