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Proceedings of the Physical Society

Line Shapes in the Method of Intersecting Energy Levels

B P Kibble, George William Series

Published Jul 1, 1961• 9 citations
Publisher

Abstract

The first part of this work is a study of the changes of intensity of the resonance fluorescence from mercury vapour as a small magnetic field H is applied either parallel or anti-parallel to the direction of the incident light. The changes follow either a Lorentzian or a dispersion-type function of the Zeeman splitting of the excited state, according to the orientations of polarizer and analyser in the beams of light. In an experiment with an additional oscillatory field at a frequency ω 0 , similar curves are observed in the region H = H 0 /2. ( H 0 is the field for which ω 0 is the Larmor frequency.) The observations are relevant to a recently developed technique in which intensity changes of this sort are used to make precision measurements in spectroscopy. The Lorentzian line shape is usually observed. The possibility of obtaining line profiles of other shapes was pointed out by Franken.

DOI
10.1088/0370-1328/78/1/311

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Frequency- and polarization-modulated light in double resonance experiments on mercury vapour

G. D. Chapman, George William Series

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.

Journal of Physics B Atomic and Molecular Physics•Jan 1, 1970•11 citations

The modulation of light in a double resonance experiment

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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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Laser line-shape effects in resonance fluorescence

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The effects of different laser line shapes on the intensity and spectrum of resonance fluorescence from a two-level atom are investigated. The laser model considered is that of an ideal single-mode laser operating high above threshold, with constant amplitude and undergoing phase-frequency fluctuations analogous to Brownian motion. As the correlation time of the frequency fluctuations increases from zero to infinity, the laser line shape changes from Lorentzian to Gaussian in a continuous way. It is shown that for intermediate and strong fields, the average intensity of fluorescence in the case of a resonant broadband Lorentzian line shape is higher than that in the case of a Gaussian line shape with the same bandwidth and total power. This is in contrast to the weak-field case where the higher peak power of the Gaussian line shape makes it more effective than the Lorentzian line shape. It is also shown that in the case of a nonzero frequency correlation time (non-Lorentzian line shape) the intensity of fluorescence undergoes non-Markovian fluctuations. In relation to the spectrum of resonance fluorescence, it is shown that as the line shape is varied from Lorentzian to Gaussian the following changes take place: In the case of off-resonance excitation, the asymmetry of the spectrum decreases. In the case of resonant excitation, the center-peak to side-peak height ratio for the triplet structure increases. Moreover, the recently predicted center-line dip, which develops in the spectrum in the case of broadband excitation when the Rabi frequency and the bandwidth are nearly equal, becomes increasingly deeper.

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Fluorescent emission of the mercury line 2537 A at pressures between 10-3 and 10-1 mm

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Abstract In his first papers on the resonance radiation of mercury and sodium Wood describes how the character of the emission changes with increasing pressure of the fluorescent vapour. At low pressure (p = 10-3 mm) the emission comes wholly from a narrow well-defined beam corresponding to the path of the primary light (beam fluorescence). With increasing density of the vapour the beam becomes diffuse until the luminosity fills the whole volume (volume fluorescence) and finally at pressures of about 0·1 mm it withdraws entirely to the spot of entrance of the primary light (surface fluorescence). In all three cases the absorption and emission of light are due to normal atoms; the phenomenon is that of normal or true resonance radiation. For the D-lines of sodium, Lord Rayleigh showed as early as 1919 that, even at pressures at which the true resonance radiation is concentrated on the surface, an emission can in addition be observed within the volume along the path of the primary light, if the D-lines in the spectrum of the exciting source are not too narrow. This new fluorescence beam which can only be excited by the outer parts of the D-lines is partially polarized. Later Jablonsky and Pringsheim found that though the normal resonance radiation observed on the surface is unpolarized under these conditions, the degree of polarization of the new fluorescence beam can be as high as 30% and is practically unaltered by the action of a magnetic field. For the mercury resonance line 2537 A it was Rayleigh who again studied the phenomena at higher pressures but with his main interest concentrated on the duration of the processes and on the appearance of the well-known mercury bands. In his paper, the continuous change of the fluorescence in the vapour volume is studied from room temperature up to 200°C. He used as a source of excitation a “not fully cooled” mercury lamp, giving a somewhat broadened and partially self-reversed line at 2537 A, which produces the effect called by Rayleigh “core­ effect”. The latter is in Rayleigh’s terminology the fluorescence of mercury vapour produced by the more central part of the 2537 A line while the very different fluorescence emission which is excited by a much broadened and self-reversed line is called by him the wing effect. The core effect always shows a line which, with the available dispersion, seems to coincide with the resonance line itself; when the pressure increases, a number of bands appear which have no importance for the present paper. Since in saturated vapour at 100° C the normal resonance radiation has withdrawn to the surface, it is improbable that the core effect is produced by the most central region of the primary line by which the normal resonance radiation at the lowest pressures is excited.

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Further studies of double resonance excited by modulated light

Alan Corney

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.

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On the influence of magnetic fields on the polarisation of resonance radiation

Robert Williams Wood, A. Ellett

Abstract The emission of polarised light by fluorescent sodium and iodine vapours was discovered by one of the present writers many years ago, and a similar phenomenon was looked for repeatedly, but without success, in the case of the much simpler (presumably) type of emission which occurs when a gas or vapour re-emits without change of wave-length the energy which it abstracts from the incident beam, as when the monochromatic radiation 2536 from a mercury arc traverse as exhausted quartz bulb containing a drop of mercury at room temperature, or the light of a sodium flame falls upon a glass bulb containing highly rarefied sodium vapour. Lord Rayleigh has recently discovered, however, that the resonance radiation of mercury vapour shows fairly strong polarisation, and reported results which apparently indicated that the polarisation becomes stronger as the exciting radiation penetrates to greater and greater depths of the vapour, being practically absent at the point where the radiation enters the bulb or tube. This would mean that polarisation of the light results only when the excitation is, by frequencies, a little out of tune with the natural frequency of the mercury atom, a matter of great theoretical interest. In a report of some work done last year by one of us this last observation of Lord Rayleigh was not confirmed, the polarisation appearing of full strength right up to the entrance window of the exciting beam. A possible explanation of Lord Rayleigh's results will be offered in the present paper in which it will be shown that a very weak magnetic field, properly oriented, destroys completely all traces of polarisation.

Proceedings of the Royal Society of London Series A Containing Papers of a Mathematical and Physical Character•Jun 1, 1923•48 citations
The first part of this work is a study of the changes of intensity of the resonance fluorescence from mercury vapour as a small magnetic field H is applied either parallel or anti-parallel to the direction of the incident light. The changes follow either a Lorentzian or a dispersion-type function of the Zeeman splitting of the excited state, according to the orientations of polarizer and analyser in the beams of light. In an experiment with an additional oscillatory field at a frequency ω 0 , similar curves are observed in the region H = H 0 /2. ( H 0 is the field for which ω 0 is the Larmor frequency.) The observations are relevant to a recently developed technique in which intensity changes of this sort are used to make precision measurements in spectroscopy. The Lorentzian line shape is usually observed. The possibility of obtaining line profiles of other shapes was pointed out by Franken.
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 effects of different laser line shapes on the intensity and spectrum of resonance fluorescence from a two-level atom are investigated. The laser model considered is that of an ideal single-mode laser operating high above threshold, with constant amplitude and undergoing phase-frequency fluctuations analogous to Brownian motion. As the correlation time of the frequency fluctuations increases from zero to infinity, the laser line shape changes from Lorentzian to Gaussian in a continuous way. It is shown that for intermediate and strong fields, the average intensity of fluorescence in the case of a resonant broadband Lorentzian line shape is higher than that in the case of a Gaussian line shape with the same bandwidth and total power. This is in contrast to the weak-field case where the higher peak power of the Gaussian line shape makes it more effective than the Lorentzian line shape. It is also shown that in the case of a nonzero frequency correlation time (non-Lorentzian line shape) the intensity of fluorescence undergoes non-Markovian fluctuations. In relation to the spectrum of resonance fluorescence, it is shown that as the line shape is varied from Lorentzian to Gaussian the following changes take place: In the case of off-resonance excitation, the asymmetry of the spectrum decreases. In the case of resonant excitation, the center-peak to side-peak height ratio for the triplet structure increases. Moreover, the recently predicted center-line dip, which develops in the spectrum in the case of broadband excitation when the Rabi frequency and the bandwidth are nearly equal, becomes increasingly deeper.
Abstract In his first papers on the resonance radiation of mercury and sodium Wood describes how the character of the emission changes with increasing pressure of the fluorescent vapour. At low pressure (p = 10-3 mm) the emission comes wholly from a narrow well-defined beam corresponding to the path of the primary light (beam fluorescence). With increasing density of the vapour the beam becomes diffuse until the luminosity fills the whole volume (volume fluorescence) and finally at pressures of about 0·1 mm it withdraws entirely to the spot of entrance of the primary light (surface fluorescence). In all three cases the absorption and emission of light are due to normal atoms; the phenomenon is that of normal or true resonance radiation. For the D-lines of sodium, Lord Rayleigh showed as early as 1919 that, even at pressures at which the true resonance radiation is concentrated on the surface, an emission can in addition be observed within the volume along the path of the primary light, if the D-lines in the spectrum of the exciting source are not too narrow. This new fluorescence beam which can only be excited by the outer parts of the D-lines is partially polarized. Later Jablonsky and Pringsheim found that though the normal resonance radiation observed on the surface is unpolarized under these conditions, the degree of polarization of the new fluorescence beam can be as high as 30% and is practically unaltered by the action of a magnetic field. For the mercury resonance line 2537 A it was Rayleigh who again studied the phenomena at higher pressures but with his main interest concentrated on the duration of the processes and on the appearance of the well-known mercury bands. In his paper, the continuous change of the fluorescence in the vapour volume is studied from room temperature up to 200°C. He used as a source of excitation a “not fully cooled” mercury lamp, giving a somewhat broadened and partially self-reversed line at 2537 A, which produces the effect called by Rayleigh “core­ effect”. The latter is in Rayleigh’s terminology the fluorescence of mercury vapour produced by the more central part of the 2537 A line while the very different fluorescence emission which is excited by a much broadened and self-reversed line is called by him the wing effect. The core effect always shows a line which, with the available dispersion, seems to coincide with the resonance line itself; when the pressure increases, a number of bands appear which have no importance for the present paper. Since in saturated vapour at 100° C the normal resonance radiation has withdrawn to the surface, it is improbable that the core effect is produced by the most central region of the primary line by which the normal resonance radiation at the lowest pressures is excited.
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 The emission of polarised light by fluorescent sodium and iodine vapours was discovered by one of the present writers many years ago, and a similar phenomenon was looked for repeatedly, but without success, in the case of the much simpler (presumably) type of emission which occurs when a gas or vapour re-emits without change of wave-length the energy which it abstracts from the incident beam, as when the monochromatic radiation 2536 from a mercury arc traverse as exhausted quartz bulb containing a drop of mercury at room temperature, or the light of a sodium flame falls upon a glass bulb containing highly rarefied sodium vapour. Lord Rayleigh has recently discovered, however, that the resonance radiation of mercury vapour shows fairly strong polarisation, and reported results which apparently indicated that the polarisation becomes stronger as the exciting radiation penetrates to greater and greater depths of the vapour, being practically absent at the point where the radiation enters the bulb or tube. This would mean that polarisation of the light results only when the excitation is, by frequencies, a little out of tune with the natural frequency of the mercury atom, a matter of great theoretical interest. In a report of some work done last year by one of us this last observation of Lord Rayleigh was not confirmed, the polarisation appearing of full strength right up to the entrance window of the exciting beam. A possible explanation of Lord Rayleigh's results will be offered in the present paper in which it will be shown that a very weak magnetic field, properly oriented, destroys completely all traces of polarisation.