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Proceedings of the Royal Society of London A Mathematical and Physical Sciences

The modulation of light in a double resonance experiment

John N. Dodd, George William Series, Martin John Taylor

Published Apr 23, 1963• 34 citations
Publisher

Abstract

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.

DOI
10.1098/rspa.1963.0074

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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.

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B P Kibble, George William Series

Abstract This is an investigation, at low frequencies, of the modulation of fluorescent light which has already been found a t higher frequencies in a double resonance experiment. In the earlier work, in which the frequency of magnetic resonance was of order 10 Mc/s, the Zeeman levels of the excited atom s were well separated compared with their natural width (1 M c/s): in the present work they are completely unresolved at the centre of the magnetic resonance, which is studied a t 1 kc/s. The principal resonance phenomena are observed as before under the new conditions: they are centred on a field near to zero, while their width is greater than 1G. New resonance phenomena are also studied, which do not appear when the resonance frequency is greater than the natural width of the levels. A theory, previously published, is applied to predict the form of the new resonance curves. An identical result is predicted by the use of a classical model.

Proceedings of the Royal Society of London A Mathematical and Physical Sciences•Jul 23, 1963•15 citations
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.
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 type of double resonance experiment is reported in which resonance fluorescence from an atomic vapour is excited by modulated light. The amplitude of modulation of the fluorescent light undergoes changes which indicate an atomic resonance when the frequency of modulation is equal to the Larmor frequency of the atoms in an applied magnetic field, or equal to twice that frequency. The effects have been studied in the intercombination line, λ 3261 A, of cadmium. They are in good agreement with theoretical predictions. The method could be applied to the spectroscopy of 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.
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.
Further experiments are reported in which resonance fluorescence of an atomic vapour is excited by modulated light. The system studied was the 3 P 1 level of cadmium excited by the λ 3261 λ intercombination line modulated at 462 kHz. Resonant changes in the amplitude of modulation of the fluorescent light have been observed in both static and time-dependent magnetic fields whenever the modulation frequency matches a frequency separation between the states of the excited atoms. Quantitative investigations of the shape and position of the observed resonances show good agreement between theory and experiment. The application of the technique to the spectroscopy of excited atoms is considered.
Abstract This is an investigation, at low frequencies, of the modulation of fluorescent light which has already been found a t higher frequencies in a double resonance experiment. In the earlier work, in which the frequency of magnetic resonance was of order 10 Mc/s, the Zeeman levels of the excited atom s were well separated compared with their natural width (1 M c/s): in the present work they are completely unresolved at the centre of the magnetic resonance, which is studied a t 1 kc/s. The principal resonance phenomena are observed as before under the new conditions: they are centred on a field near to zero, while their width is greater than 1G. New resonance phenomena are also studied, which do not appear when the resonance frequency is greater than the natural width of the levels. A theory, previously published, is applied to predict the form of the new resonance curves. An identical result is predicted by the use of a classical model.