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Broadening and Shifting of the Alkali-Metal Resonance Lines by Collisions of Like Monatoms

Moncef Bouledroua, A. Dalgarno, E Robin

Published Jan 1, 2006• 0 citations
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Abstract

The purpose of this work is the evaluation of the linewidth w and lineshift d of the sodium resonance line 3p − → 3s when the excited atoms are evolving in their parent gas. Assuming the Baranger impact approximation, these two quantities are given in terms of the phase shifts of the ground Na(3s) + Na(3s) and the excited Na(3p)+Na(3s) states. The quantal calculations and the semi-classical method, developed by Mott and Massey and Landau and Lifshitz, show that the cross sections σ and λ vary with the energy like E−1/2, the width w and the shift d do not depend on the temperature, the long-range interactions have a big influence on w and d, and the rate coefficients depend on the dispersion coefficients like w/n ≈ +7.298 × 10−8C3(Σ) and d/n ≈ +8.893 × 10−9C3(Σ). The study also shows that the sodium results can be extended to the other alkali-metal atoms (Li, K, Rb, Cs, and Fr) by a simple scaling. Keywords: potential energy curve, broadening cross section, rate coefficient, linewidth, lineshift, dispersion coefficient

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Physical Review A•Sep 1, 1978•16 citations
The purpose of this work is the evaluation of the linewidth w and lineshift d of the sodium resonance line 3p − → 3s when the excited atoms are evolving in their parent gas. Assuming the Baranger impact approximation, these two quantities are given in terms of the phase shifts of the ground Na(3s) + Na(3s) and the excited Na(3p)+Na(3s) states. The quantal calculations and the semi-classical method, developed by Mott and Massey and Landau and Lifshitz, show that the cross sections σ and λ vary with the energy like E−1/2, the width w and the shift d do not depend on the temperature, the long-range interactions have a big influence on w and d, and the rate coefficients depend on the dispersion coefficients like w/n ≈ +7.298 × 10−8C3(Σ) and d/n ≈ +8.893 × 10−9C3(Σ). The study also shows that the sodium results can be extended to the other alkali-metal atoms (Li, K, Rb, Cs, and Fr) by a simple scaling. Keywords: potential energy curve, broadening cross section, rate coefficient, linewidth, lineshift, dispersion coefficient
The broadening of the Na resonance lines, due to collisions with Rb and with Cs, has been measured with the use of the normalized fluorescence-intensity method of Chatham, Lewis, and Gallagher. Several Na resonance-radiation diffusion and absorption corrections were necessary in the Rb case, due to an unavoidable excess of Na density in the Rb vapor. The line-broadening rate coefficients k1{k}_{1}k1​ and k2{k}_{2}k2​ for the D1{D}_{1}D1​ and D2{D}_{2}D2​ resonance lines are ${k}_{1}(\mathrm{Rb})=(6.2\ifmmode\pm\else\textpm\fi{}0.4)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{s}}^{\ensuremath{-}1}$, ${k}_{2}(\mathrm{Rb})=(5.5\ifmmode\pm\else\textpm\fi{}0.6)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{s}}^{\ensuremath{-}1}$, ${k}_{1}(\mathrm{Cs})=(6.9\ifmmode\pm\else\textpm\fi{}1.0)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{s}}^{\ensuremath{-}1}$, and ${k}_{2}(\mathrm{Cs})=(5.5\ifmmode\pm\else\textpm\fi{}0.9)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{s}}^{\ensuremath{-}1}$ at $T\ensuremath{\simeq}300$\ifmmode^\circ\else\textdegree\fi{} C. The leading (${C}_{6}{R}^{\ensuremath{-}6}$) dipole-dipole long-range dispersion forces for the Na-Rb and Na-Cs interactions are calculated, and are used in the impact-theory formula to obtain theoretical line-broadening rate coefficients. These are in poor agreement with the measurements, indicating that as suggested by Vadla, the higher-order (${C}_{8}{R}^{\ensuremath{-}8}$) dispersion terms are also important at the very long range responsible for this line broadening.
This work reports pressure-broadening line-wing and line-core of the lithium Li (2 p ← 2 s) resonance line perturbed by ground sodium Na (3s) atoms. In far-wing regions, the calculations are performed quantum-mechanically and are intended to examine the photoabsorption coefficients at diverse temperatures. The results show the existence of three satellites, in the blue wing near the wavelengths 470 nm and in the red wing around 862 nm and 1070 nm. For the line-core region, by adopting the simplified Baranger model, the line-width and line-shift rates are determined, and their variation law with temperature is examined. No published data were found to compare these results with.
The dencity of sodium was determined from measurement of optical absorption of the resonance line. Sodium vapour, in the dencity 3×10~(11) to 1.2×10~(12)cm~(-3), was excited by a cw dye laser, tuned 70 GHz from D_2 resonance line. We recorded signal intensities, consisting of The Rayleigh component at the laser frequency and the two fluorescence components (direct and sensitized) at the atomic resonance-line frequencies. D_2 line self-broadening rate coefficient [k_(br,2)=5.44×10~(-7)cm~3/s(±15%)] was yielded. Combined with the effective radiative decay rates in the presence of radiation trapping, we measured excitation-transfer rates in different dencities, for the excitation transfer process Na(3P_(3/2))+Na(3S) Na (3P_(1/2))+Na(3S). The fine-structure collisional-mining cross section [σ_(21)(3P_(3/2)→3P_(1/2))=19.9nm~2(±29%)3 at T 184℃ was obtained. Our results were compared to other experiments and to theory.
The theory of impact broadening of the isolated spectral lines of the Rydberg atomic series perturbed by neutral particles is developed within the framework of the impulse approximation. The analysis of the broadening process is based on the consideration of the inelastic nl to n' transitions between highly excited states of the Rydberg atom. The role of the potential and resonance scattering of the quasifree electron by a perturbing particle in the impact broadening of the Rydberg nl levels is investigated. It is shown that the general expressions for the broadening cross sections presented in this paper contain the results of asymptotic Alekseev and Sobel'man theory (1965) as special cases. Both elastic and inelastic scattering contributions of the perturber by the parent core of Rydberg atom to the broadening cross sections are also considered within the framework of the 'shake' model. The results obtained are used for a quantitative explanation of experimental data on the broadening of Rydberg atomic levels perturbed by alkali-metal atoms. The energies and widths of the 3 P resonances on the quasidiscrete levels of the negative K - and Rb - ions are determined.
The broadening and shift of two-photon $S\ensuremath{-}S$ transitions (e.g., in alkali-metal atoms perturbed by rare gases) are shown to be readily calculable. These calculations employ (a) newly available expressions for alkalimetal-rare-gas long-range potential coefficients C6{C}_{6}C6​, C8{C}_{8}C8​, and C10{C}_{10}C10​; and (b) the (herein discussed) appropriate form of impact theory (particularly simple since only a single potential curve is involved and inelastic processes are not usually important). It is demonstrated in particular that the influence of C8{C}_{8}C8​ and C10{C}_{10}C10​ terms on the broadening and shift is significant though not dominant. Comparison with recent experimental data on the Na-rare-gas pairs shows reasonable agreement for the heavy rare gases.