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Journal of Quantitative Spectroscopy and Radiative Transfer

Satellites of the resonance transitions of alkali atoms in mixtures with CF4

Vadim A. Alekseev, A. A. Pastor, Anatoly S. Pazgalev, P.A. Petrov, Pavel Yu. Serdobintsev, T. A. Vartanyan

Published Sep 16, 2020• 5 citations
Publisher
DOI
10.1016/j.jqsrt.2020.107339

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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( $${{v}_{3}}$$ = 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.

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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 $${{R}_{{{\text{A}} - {\text{C}}{{{\text{F}}}_{4}}}}}$$ → ∞) 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.

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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.
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.