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Journal of Experimental and Theoretical Physics Letters

Satellite Transition of the Resonance Doublet of the Na Atom in a Mixture with CF4

Vadim A. Alekseev, A. A. Pastor, Pavel Yu. Serdobintsev, T. A. Vartanyan

Published Jul 1, 2021• 3 citations
Publisher

Abstract

The excitation spectrum of the resonance luminescence of Na atoms in a mixture with CF4 exhibits a satellite transition corresponding to the simultaneous optical excitation of the colliding atom and molecule, Na(2S1/2) + CF4( $${{v}_{3}}$$ = 0) + h $$v$$ → Na(2P1/2, 3/2) + CF4( $${{v}_{3}}$$ = 1), where $${{v}_{3}}$$ is the infrared active mode of CF4 with a vibrational quantum energy of 1283 cm–1. It is shown that the optical coupling between the upper and lower states of this asymptotically $$({{R}_{{{\text{Na}} - {\text{C}}{{{\text{F}}}_{4}}}}} \to \infty )$$ forbidden transition can be explained within a model that takes into account the polarization of the atom in the field of the molecule and the interaction of the dipole moment of the CF4( $${{v}_{3}}$$ = 1 ↔ $${{v}_{3}}$$ = 0) transition with the dipole moments of electronic transitions in the atom. The results of calculations based on this model are in satisfactory agreement with the experiment. It is noted that CF4 may be of interest as a component of a working medium of diode pumped alkali lasers.

DOI
10.1134/s0021364021140034

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The excitation spectrum of the resonance luminescence of Na atoms in a mixture with CF4 exhibits a satellite transition corresponding to the simultaneous optical excitation of the colliding atom and molecule, Na(2S1/2) + CF4( v3{{v}_{3}}v3​ = 0) + h vvv → Na(2P1/2, 3/2) + CF4( v3{{v}_{3}}v3​ = 1), where v3{{v}_{3}}v3​ is the infrared active mode of CF4 with a vibrational quantum energy of 1283 cm–1. It is shown that the optical coupling between the upper and lower states of this asymptotically (RNa−CF4→∞)({{R}_{{{\text{Na}} - {\text{C}}{{{\text{F}}}_{4}}}}} \to \infty )(RNa−CF4​​→∞) forbidden transition can be explained within a model that takes into account the polarization of the atom in the field of the molecule and the interaction of the dipole moment of the CF4( v3{{v}_{3}}v3​ = 1 ↔ v3{{v}_{3}}v3​ = 0) transition with the dipole moments of electronic transitions in the atom. The results of calculations based on this model are in satisfactory agreement with the experiment. It is noted that CF4 may be of interest as a component of a working medium of diode pumped alkali lasers.
The luminescence excitation spectra of the D1 resonance line of atoms K, Rb, and Cs in gas mixtures with CF4 are found to contain satellite transitions, which correspond to the transition of an atom to the states (n – 1)d 2D3/2,5/2 and (n + 1)s 2S1/2, where n = 4, 5, and 6 for K, Rb, and Cs, respectively, with the simultaneous excitation of CF4 molecule vibrations at the IR active mode frequency ν3 with a quantum energy of 1283 cm–1. These satellite transitions are A(ns 2S1/2) + CF4(ν3 = 0) + hν → A((n – 1)d 2D3/2,5/2) + CF4(ν3 = 1) and A(ns 2S1/2) + CF4(ν3 = 0) + hν → A((n + 1)s 2S1/2) + CF4(ν3 = 1), where A = K, Rb, and Cs. The appearance of an optical coupling between the upper and lower states of these asymptotically (at RA−CF4{{R}_{{{\text{A}} - {\text{C}}{{{\text{F}}}_{4}}}}}RA−CF4​​ → ∞) forbidden transitions is shown to be caused by the interaction of the dipole moment of the ν3 = 1 ↔ ν3 = 0 vibrational transition in the CF4 molecule with the dipole moments of the electronic transitions np 2P1/2,3/2 ↔ (n – 1)d 2D3/2,5/2 and np 2P1/2,3/2 ↔ (n + 1)s 2S1/2 in an alkali metal atom; as a result of this interaction, the upper state of the satellite transition acquires admixtures of the A(np 2P1/2,3/2)CF4(ν3 = 0) resonance states.
3 2P1/2 ↔ 3 2P3/2 excitation transfer in sodium, induced in inelastic collisions with ground-state N2, H2, HD, and D2 molecules, has been investigated in a series of sensitized fluorescence experiments. Mixtures of sodium vapor at a pressure of 5 × 10−7 Torr, and the gases, were irradiated with each NaD component in turn, and the fluorescence which contained both D components was monitored at right angles to the direction of the exciting beam. Measurements of the relative intensities of the NaD fluorescent components yielded the following collision cross sections for excitation transfer. For Na–N2 collisions: Q12(2P1/2 → P3/2) = 144 Å2, Q21(2P1,2 ← 2P3/2) = 76 Å2 for Na–H2 collisions: Q12 = 80 Å2, Q21 = 42 Å2. For Na–HD collisions: Q12 = 84 Å2, Q21 = 44 Å2. For Na–D2 collisions: Q12 = 98 Å2, Q21 = 52 Å2. The cross sections Q21 exhibit a slight resonance effect between the atomic and molecular rotational transitions.
Lasing on the 62P1/2→62S1/2(D1) resonance transition of atomic Cs at 894.3 nm has been demonstrated in mixtures of Ar, ethane, and Cs vapor by the photoexcitation of ground state Cs-Ar collision pairs and subsequent dissociation of diatomic, electronically-excited CsAr molecules (exciplexes or excimers). The blue satellites of the alkali D2 lines provide a pathway for optically pumping atomic alkali lasers on the principal series (resonance) transitions with broad linewidth (>2 nm) semiconductor diode lasers. In this paper we discuss different variations of this new laser system and the experiments of the initial demonstration.
6 2P1/2 ↔ 6 2P3/2 mixing and 6 2S1/2 ← 6 2P1/2,3/2 quenching in cesium, induced in collisions with ground state N2, H2, HD, and D2 molecules, have been investigated using techniques of sensitized fluorescence. Mixtures of cesium vapor and the gases, in which the cesium vapor pressure was kept very low to avoid multiple scattering, were irradiated with each component of the cesium resonance doublet in turn. The fluorescence which contained both components of the doublet was observed in a direction perpendicular to that of the exciting beam. Measurements of the relative intensities of the fluorescent components yielded the following cross sections for mixing and quenching. For Cs–N2 collisions: Q12(2P1/2 → 2P3/2) = 4.7 Å2, Q21(2P1/2 ← 2P3/2) = 25 Å2, Q10(2S1/2 ← 2P1/2) = 77 Å2, Q20(2S1/2 ← 2P3/2) = 69 Å2. For Cs–H2 collisions: Q12 = 6.7 Å2, Q21 = 44 Å2, Q10 = 7 Å2, Q20 = 5 Å2. For Cs–HD collisions: Q12 = 4.8 Å2, Q21 = 32 Å2, Q10 = 4 Å2, Q20 = 3 Å2. For Cs–D2 collisions: Q12 = 4.2 Å2, Q21 = 28 Å2, Q10 = 8 Å2, Q20 = 7 Å2. The Cs–N2 and Cs–H2 cross sections supersede the values published previously (McGillis and Krause 1967). The cross sections Q21 appear to exhibit resonances with molecular rotational transitions.
The cross sections for the excitation energy transfer in the collisional processes Na*(3P 1 2/)+M(nS 1 2/) to or from Na*(3p 3 2/)+m(Ns 3 2/), m being ground-state Rb (n=5) or Cs (n=6) atom, have been measured by laser fluorescence method. With either of the two sodium 3P fine-structure states optically excited, the intensity ratio of the sensitized to direct fluorescence was measured. The polarization effects due to partially polarized and anisotropic direct fluorescence were investigated. The measured cross sections (T=530 K) for the sodium 3P fine-structure excitation transfer induced by collisions with Rb are: sigma ( 1 / 2 to 3 / 2 )=170 AA 2 , with an overall accuracy of 20%. The corresponding values in the Cs case are: sigma ( 1 / 2 to 3 / 2 )=140 AA 2 , sigma ( 3 / 2 to 1 / 2 )=83 AA 2 . The theoretical calculations reveal the decisive role of the dipole-quadrupole interaction. The obtained values are in satisfactory agreement with the experiment only if both the dipole-dipole and dipole-quadrupole interactions are taken into account, while the calculations involving the dipole-dipole term alone yield the cross section values which are as much as one order of magnitude lower than the experimentally observed ones.