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Resonance Broadening of the Sodium D-Lines in Absorption

Kenichi Watanabe

Published Feb 21, 2025• 0 citations
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Abstract

The resonance broadening of the sodium D-lines in absorption was determined by measuring the contour of the line wings directly. The vapor pressures of sodium ranged from 10-3 to 75 mm Hg, with negligible amount of foreign gases. Over nearly the entire range, the half-intensity width varied linearly with the density of the absorbing atoms; i.e. Δν1/2/N = 0.78 x 10-7 sec-1cm3 --the constant being about twice that predicted by Houston, but much less than the experimental result by Hughes and LLoyd. Above 5 mm pressure, the half-intensity width appeared to increase slightly faster than N. Somewhat in contradiction to theory, the relative width, Δν1/2,s/Δν1/2,1' was 1.16. The natural width measured was, within experimental error, consistent with previous values. The inverse square contour for the absorption coefficient was satisfactory up to 5 mm Hg; beyond this pressure an inverse cube contour fitted better. No definite evidence of van der Waal force was observed at high pressures; likewise, no appreciable shifts and asymmetries. MgO windows were used and the temperature determination was made reliable.

DOI
10.7907/tzfa-n362

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By direct measurement of the contours of the line wings, the resonance broadening of the sodium $D$ lines in absorption was determined for vapor pressures of sodium ranging from ${10}^{\ensuremath{-}3}$ to 70 mm Hg with negligible amount of foreign gases. Over nearly the entire range, the half-intensity width varied linearly with the density of the absorbing atoms; i.e., $\frac{\ensuremath{\Delta}{\ensuremath{\nu}}_{\frac{1}{2}}}{N}=0.80\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}7}$ ${\mathrm{sec}.}^{\ensuremath{-}1}$ ${\mathrm{cm}}^{\ensuremath{-}3}$---the constant being 1.6 times that predicted by theory but much less than the corresponding experimental results for potassium. Above 5 mm pressure, $\ensuremath{\Delta}{\ensuremath{\nu}}_{\frac{1}{2}}$ increased slightly faster than $N$; moreover, the contour for the absorption coefficient was more adequately represented by an inverse cube contour than by the inverse square. Somewhat in contradiction to theory, the relative width, $\frac{\ensuremath{\Delta}{\ensuremath{\nu}}_{\frac{1}{2},8}}{\ensuremath{\Delta}{\ensuremath{\nu}}_{\frac{1}{2},l}}$ was 1.12. No definite evidence of van der Waals force was observed at the higher pressures; likewise no appreciable shifts or asymmetries. The natural width measured was consistent with previous results.

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It is pointed out that the usual theories of pressure broadening disagree with direct experimental measurements of the widths of resonance-broadened alkali doublet lines, although the theories are at least qualitatively confirmed for the wings of resonance lines and for foreign-gas broadening. There are also two conflicting sets of experimental data (both in strong disagreement with theory). Some qualitative arguments are given for doubting the validity, near the center of a resonance line, of the "two-body" approximation generally used in theoretical treatments, and some formal objections to the usual procedure are also presented. The basic equation relating the susceptibility to a resolvent operator matrix element is derived from a more fundamental point of view than usual; the result contains in principle all effects due to translational motion, to the quantized nature of the radiation field, and to "spatial dispersion." In the limit of large absorber mass it is proved rigorously that the two-body approximation can never be valid near the center of a line, even for very low densities. By using different approximations for the wings and the line center, we obtain satisfactory agreement with experiments in both regions for the alkali doublet lines. We are also able to decide between the two conflicting experiments, favoring the square-root density dependence of the line-width observed by Lauriston and Welsh.

Physical Review•Feb 1, 1965•63 citations
The resonance broadening of the sodium D-lines in absorption was determined by measuring the contour of the line wings directly. The vapor pressures of sodium ranged from 10-3 to 75 mm Hg, with negligible amount of foreign gases. Over nearly the entire range, the half-intensity width varied linearly with the density of the absorbing atoms; i.e. Δν1/2/N = 0.78 x 10-7 sec-1cm3 --the constant being about twice that predicted by Houston, but much less than the experimental result by Hughes and LLoyd. Above 5 mm pressure, the half-intensity width appeared to increase slightly faster than N. Somewhat in contradiction to theory, the relative width, Δν1/2,s/Δν1/2,1' was 1.16. The natural width measured was, within experimental error, consistent with previous values. The inverse square contour for the absorption coefficient was satisfactory up to 5 mm Hg; beyond this pressure an inverse cube contour fitted better. No definite evidence of van der Waal force was observed at high pressures; likewise, no appreciable shifts and asymmetries. MgO windows were used and the temperature determination was made reliable.
By direct measurement of the contours of the line wings, the resonance broadening of the sodium DDD lines in absorption was determined for vapor pressures of sodium ranging from ${10}^{\ensuremath{-}3}$ to 70 mm Hg with negligible amount of foreign gases. Over nearly the entire range, the half-intensity width varied linearly with the density of the absorbing atoms; i.e., $\frac{\ensuremath{\Delta}{\ensuremath{\nu}}_{\frac{1}{2}}}{N}=0.80\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}7}$ ${\mathrm{sec}.}^{\ensuremath{-}1}$ ${\mathrm{cm}}^{\ensuremath{-}3}$---the constant being 1.6 times that predicted by theory but much less than the corresponding experimental results for potassium. Above 5 mm pressure, $\ensuremath{\Delta}{\ensuremath{\nu}}_{\frac{1}{2}}$ increased slightly faster than NNN; moreover, the contour for the absorption coefficient was more adequately represented by an inverse cube contour than by the inverse square. Somewhat in contradiction to theory, the relative width, $\frac{\ensuremath{\Delta}{\ensuremath{\nu}}_{\frac{1}{2},8}}{\ensuremath{\Delta}{\ensuremath{\nu}}_{\frac{1}{2},l}}$ was 1.12. No definite evidence of van der Waals force was observed at the higher pressures; likewise no appreciable shifts or asymmetries. The natural width measured was consistent with previous results.
The resonance broadening of homogeneous Cs vapor in absorption was studied by means of the contour method. The intensities were obtained via the method of "astigmatic photometry" by utilizing the astigmatism of the Rowland grating. The pressure of the homogeneous absorbing vapor ranged from ${10}^{\ensuremath{-}2}$ to 17.5 mm Hg. The half breadth $\ensuremath{\gamma}$ varied rather linearly with the number of atoms per unit volume, with $(\frac{{\ensuremath{\gamma}}_{1}}{N})\ifmmode\times\else\texttimes\fi{}{10}^{7}=1.45$, $(\frac{{\ensuremath{\gamma}}_{2}}{N})\ifmmode\times\else\texttimes\fi{}{10}^{7}$ for the 2P32^{2}P_{\frac{3}{2}}2P23​​ and 2P12^{2}P_{\frac{1}{2}}2P21​​ eomponents of the resonance lines, respectively. The average value of the ratio of half breadths $\frac{{\ensuremath{\gamma}}_{1}}{{\ensuremath{\gamma}}_{2}}$ was found to be 1.8. The experimental half-width $\ensuremath{\gamma}$ is found to be about 1\textonehalf{} times larger than that predicted by W. V. Houston. Below pressures of 10 mm Hg the lines exhibited symmetrical broadening according to the "dispersion" formula. At higher pressures indications of a violet and red asymmetry are present for the 2P32^{2}P_{\frac{3}{2}}2P23​​ and 2P12^{2}P_{\frac{1}{2}}2P21​​ components, respectively. A definite band on the red side of the 2P32^{2}P_{\frac{3}{2}}2P23​​ and one on the violet side of the 2P12^{2}P_{\frac{1}{2}}2P21​​ was observed.
The broadening of the resonance lines of rubidium in absorption under pressures up to 150 mm of its own homogeneous vapor was studied by means of a 21-foot grating. Under pressures below 1 mm the broadening of the lines was very symmetrical and the line contours could be described by the dispersion formula, but when the pressure was high the lines exhibited asymmetrical broadening of van der Waals type. The 2P12^{2}P_{\frac{1}{2}}2P21​​ component showed red, while the 2P32^{2}P_{\frac{3}{2}}2P23​​ component showed violet asymmetry. Both lines showed the proportionality of the width with NNN, the concentration of Rb atoms. The experimental width at half-maximum is greater than that predicted by Houston's theory by a factor of 1.5 and the width of the transition from 3P32^{3}P_{\frac{3}{2}}3P23​​ is greater than that from 3P12^{3}P_{\frac{1}{2}}3P21​​ by a factor of 1.6. A narrow diffuse band was observed near the shorter wave-length side of the 2P12^{2}P_{\frac{1}{2}}2P21​​ component and a similar one near the longer wave-length side of the 2P32^{2}P_{\frac{3}{2}}2P23​​ component.
Spectrograms of the DDD lines of sodium in absorption were obtained and measured on a densitometer, thus determining an optical constant which was uncertain in former work. Absolute contours in terms of transmitted intensity against wave-length were obtained. Possible sources of error were studied in detail. The observed contours were compared with the classical formula. The contours were found to have the theoretical inverse square variation of opacity with wave-length distance from resonance; they showed the theoretical variation of width with the square root of the number of atoms in the line of sight, and the 2:1 ratio between the two DDD lines. The width of the lines was, however, about five times that which classical radiation damping accounts for. A detailed further experimental study of this discrepancy is planned.
Selective reflection from sodium, potassium, rubidium, and caesium vapors in the neighborhood of the resonance lines was observed for vapor pressures between 10 mm. and 1 atm., using a steel tube with a window of transparent magnesium oxide. Reflecting power as a function of frequency was measured by using incident light of continuous spectral distribution. The reflection contour for pressures up to ½ atm. is in good agreement with the theory of reflection from an absorbing medium. For each line the damping constant in the dispersion equations varies as the square root of the number of atoms per cubic centimeter, as was found previously for mercury and cadmium. For the two members of the resonance doublet the damping constants are proportional to the square roots of the oscillator strengths. In a region about 5 cm.−1 wide about each resonance frequency the reflected intensity measured experimentally is greater than that calculated. These lines of residual intensity may be due to a second kind of selective reflection. At pressures above ½ atm. the observed reflection contour cannot be explained by the simple anomalous dispersion theory.
It is pointed out that the usual theories of pressure broadening disagree with direct experimental measurements of the widths of resonance-broadened alkali doublet lines, although the theories are at least qualitatively confirmed for the wings of resonance lines and for foreign-gas broadening. There are also two conflicting sets of experimental data (both in strong disagreement with theory). Some qualitative arguments are given for doubting the validity, near the center of a resonance line, of the "two-body" approximation generally used in theoretical treatments, and some formal objections to the usual procedure are also presented. The basic equation relating the susceptibility to a resolvent operator matrix element is derived from a more fundamental point of view than usual; the result contains in principle all effects due to translational motion, to the quantized nature of the radiation field, and to "spatial dispersion." In the limit of large absorber mass it is proved rigorously that the two-body approximation can never be valid near the center of a line, even for very low densities. By using different approximations for the wings and the line center, we obtain satisfactory agreement with experiments in both regions for the alkali doublet lines. We are also able to decide between the two conflicting experiments, favoring the square-root density dependence of the line-width observed by Lauriston and Welsh.