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The Journal of Chemical Physics

Observation of pair absorption and self-broadening in Ba vapor

Kiyoshi Ueda, Hikaru Sotome, Yamato Sato

Published Feb 1, 1991• 5 citations
Publisher

Abstract

Reduced absorption coefficients γBaBa were measured for the far-wing absorption of the self-broadened Ba6s2 1S0–5d6p 1P1 line, Ba(6s2 1S0) +Ba(6s2 1S0)+ℏω → Ba*(5d6p 1P1)+Ba(6s21 S0)and the pair absorption Ba(6s2 1S0)+Ba(6s2 1 S0) +ℏω→Ba*(6s6p 1P1 +Ba*(6s5d 1D2). The self-broadening shows the red-shaded asymmetric profile: γBaBa on the red wing is proportional to Δν−3/2, where Δν is the detuning from the line center. The pair absorption shows a broad asymmetric peak having a blue tail and a blue satellite. The estimated γBaBa, which is based on the quasistatic line-broadening theory and the long-range dipole–dipole interaction between the relevant atomic excited levels, shows reasonable agreement for the red wing of the self-absorption whereas it gives larger values by a factor of 3 for the blue tail of the main peak for the pair absorption.

DOI
10.1063/1.459911

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Reduced absorption coefficients γBaBa were measured for the far-wing absorption of the self-broadened Ba6s2 1S0–5d6p 1P1 line, Ba(6s2 1S0) +Ba(6s2 1S0)+ℏω → Ba*(5d6p 1P1)+Ba(6s21 S0)and the pair absorption Ba(6s2 1S0)+Ba(6s2 1 S0) +ℏω→Ba*(6s6p 1P1 +Ba*(6s5d 1D2). The self-broadening shows the red-shaded asymmetric profile: γBaBa on the red wing is proportional to Δν−3/2, where Δν is the detuning from the line center. The pair absorption shows a broad asymmetric peak having a blue tail and a blue satellite. The estimated γBaBa, which is based on the quasistatic line-broadening theory and the long-range dipole–dipole interaction between the relevant atomic excited levels, shows reasonable agreement for the red wing of the self-absorption whereas it gives larger values by a factor of 3 for the blue tail of the main peak for the pair absorption.
16 lines of the principal series of Cs(6 2 s 1/2 to 7-16 2 p 3/2 and 6 2 s 1/2 to 7-12 2 p 1/2 ) were investigated in absorption. Cesium vapour density was varied from 10 13 up to 10 17 cm -3 . Red asymmetries of all lines (extended red wings) were detected. This can be understood if electron transitions in the long-range interaction region follow the selection rules of molecules. It was established that the red and the blue wings of the lines each can be fitted to lorentzian profiles in small wavelength intervals. With the help of quasistatic theory the interaction constants from the long-range interaction potential Delta omega =C 3 /r 3 multiplied by the oscillator strength were determined from measurements. For all lines the ratio of C 3 (red)/C 3 (blue) was found to equal 2 in accordance with earlier theoretical calculations. In the far line wing, deviation from a lorentzian profile occurs. This was interpreted as a consequence of electron transition in the short-range region of interatomic potentials.
The total absorption, AG, was measured as a function of absorbing gas pressure, P, for the 1S0–3P1 (1236 Å) and 1S0–1P1 (1165 Å) resonance transitions in Kr. For P=0.006–0.06 torr, self-broadening was negligible compared to the natural width. For P=0.06–0.75 torr, self-broadening contributed significantly to the linewidth, and the line shape was essentially symmetrical. For P = 1.0–7.0 torr, the. asymmetric Van der Waals broadening was apparent. The component of the linewidth due to self-broadening, ΓSB, was calculated from the measurements of AG, for P=0.06–0.75 torr, and was found to vary linearly with the number density of absorbers, N, as predicted by theory. The ratio, ΓSB/N, was found to be in reasonably good agreement with theoretical predictions.
This is the first reported demonstration of the use of pair-absorption transitions for optically pumping lasers. In a mixture of barium and thallium metal vapors, single-photon absorption of 3867-A laser light caused simultaneous excitation of colliding ground-state atoms to the Ba(6s6p 1P1(o)) and Tl(6p 2P(3/2)(o)) excited states. Excited-state densities of about 10(14) cm(-3) were created, and subsequent laser emission on the Ba(6s6p 1PI(o)) - Ba(6s5d 1D2) atomic transition at 1.5 microm was observed.
In addition to previous absorption measurements of Cs resonance lines, new investigations on Na, K and Rb also showed definitely that beyond symmetrical Lorentzian central parts of the lines, the stronger components of the resonance lines have blue and the weaker components red asymmetry. This behaviour can be explained by a quasistatic treatment of the self-broadening mechanism taking interatomic interaction potentials into account. But with additional data it is now possible to give a different interpretation of the origin of observed asymmetries than suggested in the previous paper on Cs resonance lines (see abstr. A5740 of 1975). The asymmetries are shown to arise from the mutual repulsion of two potential curves of the same species.
The far wing absorption profiles for excitation on the Ca(4s2 1S0–4s5p 1P01) atomic transition, broadened in collisions with He are measured. We observe strong absorption in both wings and a blue wing satellite near Δ∼125 cm−1. We tentatively identify this satellite as due to a maximum in the CaHe(4s2 1∑+–4s5p 1∑+) difference potential. These line-broadening techniques are used to study electronic energy transfer in the spin-changing collisions of Ca with He: Ca(5p 1P01) +He→Ca(5p 3P0J)+He+ΔE. Measurements of the ‘‘single collision’’ triplet–singlet branching ratio as a function of laser detuning from the atomic resonance frequency indicate a clear red wing/blue wing asymmetry. We interpret this asymmetry in terms of a preferential orbital alignment effect in the energy transfer process [Phys. Rev. Lett. 53, 2296 (1984)]. No clear structure is observed in the range of detunings probed that might indicate the curve crossing responsible for the energy transfer.
The close-coupled theory of collisions in a radiation field is used to calculate the absorption profile for the Sr $^{1}\ensuremath{\leftarrow}^{1}$S resonance line broadened by collisions with Ar. The calculations predict the polarization ratios of Sr 1P^{1}\mathrm{P}1P fluorescence following line wing excitation by either linear or circular polarized light. Ab initio calculations were used to obtain the ground and excited SrAr molecular-potential curves, which were adjusted to give improved agreement with experiment. The radiative-scattering theory gives a unified description of the absorption coefficient and polarization redistribution from the small detuning impact limit region to the far spectral wings. The cross sections for elastic and inelastic depolarizing collisions of Sr 1P1^{1}\mathrm{P}_{1}1P1​+Ar were also calculated. The calculated absorption coefficient, impact-broadening rate, linear- and circular-polarization ratios, and depolarization rate coefficients are for the most part in good agreement with experiment.