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Physical Review A

Role of rotational-energy defect in collisional transfer between the 52P1/2,3/2 levels in rubidium

Matthew D. Rotondaro, Glen P. Perram

Published May 1, 1998• 21 citations
Publisher

Abstract

Steady-state laser-induced fluorescence techniques have been used to study the rates for energy transfer between the $5{}^{2}{P}_{1/2,3/2}$ levels in rubidium. The cross sections for collisions with the molecular species ${\mathrm{H}}_{2},$ ${\mathrm{D}}_{2},$ ${\mathrm{N}}_{2},$ ${\mathrm{CH}}_{4},$ and ${\mathrm{CF}}_{4}$ have been measured as ${\ensuremath{\sigma}}_{2}{(}^{2}{\stackrel{\ensuremath{\rightarrow}}{{P}_{1/2}}}^{2}{P}_{3/2})=10.0,$ 21.4, 13.2, 29.5, and $9.5\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}16}{\mathrm{cm}}^{2}$ and ${\ensuremath{\sigma}}_{1}{(}^{2}{\stackrel{\ensuremath{\rightarrow}}{{P}_{3/2}}}^{2}{P}_{1/2})=13.9,$ 29.8, 18.4, 41.0, and $13.2\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}16}{\mathrm{cm}}^{2},$ respectively. Correlation of these spin-orbit transfer probabilities with rotational-energy defect is demonstrated.

DOI
10.1103/physreva.57.4045

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Inelastic Collisions between Excited Alkali Atoms and Molecules. VIII. 62P1/2–62P3/2 Mixing and Quenching in Mixtures of Rubidium with H2, HD, D2, N2, CH4, and CD4

I. N. Siara, L. Krause

Excitation transfer between the 62P fine-structure substates in rubidium, induced in inelastic collisions with ground-state molecules, has been studied using techniques of sensitized fluorescence. Rubidium vapor in mixtures with various molecular gases was irradiated with each component of the 2P rubidium doublet in turn, and measurements of sensitized-to-resonance fluorescent intensity ratios yielded the following mixing cross sections Q12(2P1/2 → 2P3/2) and Q21(2P1/2 ← 2P3/2), as well as effective quenching cross sections Q1X(2P1/2 → 2XJ″) and Q2X(2P3/2 → 2XJ″). For collisions with H2: Q12(2P1/2 → 2P3/2) = (41 ± 5) Å2; Q21(2P1/2 ← 2P3/2) = (26 ± 3) Å2; Q1X(2P1/2 → 2XJ″) = (36 ± 9) Å2; Q2X(2P3/2 → 2XJ″) = (31 ± 8) Å2. For HD: Q12 = (42 ± 5) Å2; Q21 = (27 ± 4) Å2; Q1X = (47 ± 13) Å2; Q2X = (38 ± 10) Å2. For D2: Q12 = (42 ± 5) Å2; Q21 = (27 ± 4) Å2; Q1X = (28 ± 8) Å2; Q2X = (21 ± 7) Å2. For N2: Q12 = (107 ± 15) Å2; Q21 = (70 ± 10) Å2; Q1X = (128 ± 44) Å2; Q2X = (126 ± 33) Å2. For CH4: Q12 = (38 ± 6) Å2; Q21 = (24 ± 3) Å2; Q1X = (129 ± 41) Å2; Q2X = (114 ± 37) Å2. For CD4: Q12 = (52 ± 7) Å2; Q21 = (34 ± 5) Å2; Q1X = (82 ± 30) Å2; Q2X = (76 ± 22) Å2. An analysis of these results suggests the possibility of resonances with various molecular rotational and vibrational transitions.

Canadian Journal of Physics•Feb 1, 1973•19 citations
Steady-state laser-induced fluorescence techniques have been used to study the rates for energy transfer between the 52P1/2,3/25{}^{2}{P}_{1/2,3/2}52P1/2,3/2​ levels in rubidium. The cross sections for collisions with the molecular species H2,{\mathrm{H}}_{2},H2​, D2,{\mathrm{D}}_{2},D2​, N2,{\mathrm{N}}_{2},N2​, CH4,{\mathrm{CH}}_{4},CH4​, and CF4{\mathrm{CF}}_{4}CF4​ have been measured as \ensuremathσ2(2P1/2\ensuremath→2P3/2)=10.0,{\ensuremath{\sigma}}_{2}{(}^{2}{\stackrel{\ensuremath{\rightarrow}}{{P}_{1/2}}}^{2}{P}_{3/2})=10.0,\ensuremathσ2​(2P1/2​\ensuremath→​2P3/2​)=10.0, 21.4, 13.2, 29.5, and 9.5\ifmmode×\else\texttimes\fi10\ensuremath−16cm29.5\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}16}{\mathrm{cm}}^{2}9.5\ifmmode×\else\texttimes\fi10\ensuremath−16cm2 and \ensuremathσ1(2P3/2\ensuremath→2P1/2)=13.9,{\ensuremath{\sigma}}_{1}{(}^{2}{\stackrel{\ensuremath{\rightarrow}}{{P}_{3/2}}}^{2}{P}_{1/2})=13.9,\ensuremathσ1​(2P3/2​\ensuremath→​2P1/2​)=13.9, 29.8, 18.4, 41.0, and 13.2\ifmmode×\else\texttimes\fi10\ensuremath−16cm2,13.2\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}16}{\mathrm{cm}}^{2},13.2\ifmmode×\else\texttimes\fi10\ensuremath−16cm2, respectively. Correlation of these spin-orbit transfer probabilities with rotational-energy defect is demonstrated.
Abstract : The collisional dynamics of the 5(2)P levels in rubidium has been examined using steady-state laser absorption nd spectrally-resolved laser induced fluorescence techniques. State-to-state cross-sections for energy transfer between Zeeman split levels ranged from 16-248 A2 for collisions with nitrogen and rare gases. These energy transfer cross-sections exhibit a significant dependence on (J,mj) state and certain symmetry relationships are demonstrated. A sub-Doppler spectrum of the Zeeman split levels indicating the isotopic shift in the D1 line of 106 plus or minus 35 was obtained using laser saturation spectroscopy.
The collisional dynamics of the Zeeman-split levels of Rb(52P1/2,52P3/2)\mathrm{Rb}(5{}^{2}{P}_{1/2},5{}^{2}{P}_{3/2})Rb(52P1/2​,52P3/2​) has been studied in the presence of a strong magnetic field (1.65 T) using steady-state, spectrally resolved laser-induced fluorescence techniques. State-to-state cross sections for transitions between (J,m)(J,m)(J,m) levels ranged from $1.6\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}15}$ to $2.5\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}{\mathrm{cm}}^{2}$ for collisions with nitrogen and rare gases. The cross sections indicate a significant dependence on (J,m)(J,m)(J,m) states and certain symmetry relations such as $\ensuremath{\sigma}(J,\stackrel{\ensuremath{\rightarrow}}{m}{J,m}^{\ensuremath{'}})=\ensuremath{\sigma}(J,\ensuremath{-}\stackrel{\ensuremath{\rightarrow}}{m}J,\ensuremath{-}{m}^{\ensuremath{'}})$ and $\ensuremath{\sigma}(J,\stackrel{\ensuremath{\rightarrow}}{m}{J,}^{\ensuremath{'}}m)=\ensuremath{\sigma}(J,\ensuremath{-}\stackrel{\ensuremath{\rightarrow}}{m}{J}^{\ensuremath{'}},\ensuremath{-}m)$ are demonstrated. The results also agree favorably with theoretical predictions of the relative decay rates for orientation, alignment, and octupole moment. The cross sections for rare-gas collision partners scale with polarizability as predicted.
The temperature dependence of cross sections for 52P1/2 ↔ 52P3/2 excitation transfer in rubidium, induced in collisions with CH4, CH2D2, and CD4 molecules, has been investigated using methods of sensitized fluorescence over a temperature range 300–650 K. The cross sections, which are of the order of 30 Å2 and which exceed similar cross sections for collisions with noble gas atoms by at least two orders of magnitude, exhibit an isotope effect which is ascribed to the phenomenon of electronic-to-rotational energy transfer.
The following energy-transfer reactions have been observed in a Sr vapor following pulsed excitation of the 5 1^{1}1P1{\mathit{P}}_{1}P1​ state: Sr∗{\mathrm{Sr}}^{\mathrm{*}}Sr∗(5 1^{1}1P1{\mathit{P}}_{1}P1​)+Sr∗{\mathrm{Sr}}^{\mathrm{*}}Sr∗(5 1^{1}1P1{\mathit{P}}_{1}P1​)\ensuremath{\rightarrow}Sr(5 1^{1}1S0{\mathit{S}}_{0}S0​)+Sr∗∗{\mathrm{Sr}}^{\mathrm{*}\mathrm{*}}Sr∗∗(n2S+1{\mathit{n}}^{2\mathit{S}+1}n2S+1L)-\ensuremath{\Delta}E, Sr∗{\mathrm{Sr}}^{\mathrm{*}}Sr∗(4 1^{1}1D2{\mathit{D}}_{2}D2​) +Sr∗{\mathrm{Sr}}^{\mathrm{*}}Sr∗(4 1^{1}1D2{\mathit{D}}_{2}D2​)\ensuremath{\rightarrow}Sr(5 1^{1}1S0{\mathit{S}}_{0}S0​)+Sr∗∗{\mathrm{Sr}}^{\mathrm{*}\mathrm{*}}Sr∗∗(n2S+1{\mathit{n}}^{2\mathit{S}+1}n2S+1L)-\ensuremath{\Delta}E. The 4 1^{1}1D2{\mathit{D}}_{2}D2​ state was populated by a nonlinear stimulated process. By measuring the rate coefficients for these reactions for over 40 final states n2S+1{\mathit{n}}^{2\mathit{S}+1}n2S+1L, we look for insight into how these reactions depend on energy defect, spin, and angular momentum. It is found that there is not a very strong dependence on the energy defect, and that singlet and triplet final states are produced in comparable amounts. The final states tend to be populated more effectively as their angular momentum increases. Total rate coefficients are of the order of gas-kinetic rates.
Cross sections for $7^{2}D_{\frac{3}{2}}\ensuremath{\leftrightarrow}7^{2}D_{\frac{5}{2}}$ transfer in Rb, induced in collisions with He, Ne, Ar, and with ground-state Rb atoms, have been determined using methods of atomic fluorescence. Rb vapor, pure or mixed with a noble gas, was irradiated in a glass fluorescence cell with pulses of 660-nm radiation from a N2{\mathrm{N}}_{2}N2​-laser-pumped dye laser, populating one of the 2D^{2}D2D states by two-photon absorption. The resulting fluorescence included a direct component emitted in the decay of the optically excited state and a sensitized component arising from the collisionally populated state. Relative intensities of the components yielded the cross sections for 72D7^{2}D72D mixing: $Q(^{2}D_{\frac{3}{2}}\ensuremath{\rightarrow}^{2}D_{\frac{5}{2}})=8.8,6.5,10.4, \mathrm{and} 30$; $Q(^{2}D_{\frac{3}{2}}\ensuremath{\leftarrow}^{2}D_{\frac{5}{2}})=5.8,4.0,6.9, \mathrm{and} 18$, in units of ${10}^{\ensuremath{-}14}$ cm2{\mathrm{cm}}^{2}cm2 for He, Ne, Ar, and Rb, respectively. Cross sections for the effective quenching of the 2D^{2}D2D states were also determined.
Excitation transfer between the 62P fine-structure substates in rubidium, induced in inelastic collisions with ground-state molecules, has been studied using techniques of sensitized fluorescence. Rubidium vapor in mixtures with various molecular gases was irradiated with each component of the 2P rubidium doublet in turn, and measurements of sensitized-to-resonance fluorescent intensity ratios yielded the following mixing cross sections Q12(2P1/2 → 2P3/2) and Q21(2P1/2 ← 2P3/2), as well as effective quenching cross sections Q1X(2P1/2 → 2XJ″) and Q2X(2P3/2 → 2XJ″). For collisions with H2: Q12(2P1/2 → 2P3/2) = (41 ± 5) Å2; Q21(2P1/2 ← 2P3/2) = (26 ± 3) Å2; Q1X(2P1/2 → 2XJ″) = (36 ± 9) Å2; Q2X(2P3/2 → 2XJ″) = (31 ± 8) Å2. For HD: Q12 = (42 ± 5) Å2; Q21 = (27 ± 4) Å2; Q1X = (47 ± 13) Å2; Q2X = (38 ± 10) Å2. For D2: Q12 = (42 ± 5) Å2; Q21 = (27 ± 4) Å2; Q1X = (28 ± 8) Å2; Q2X = (21 ± 7) Å2. For N2: Q12 = (107 ± 15) Å2; Q21 = (70 ± 10) Å2; Q1X = (128 ± 44) Å2; Q2X = (126 ± 33) Å2. For CH4: Q12 = (38 ± 6) Å2; Q21 = (24 ± 3) Å2; Q1X = (129 ± 41) Å2; Q2X = (114 ± 37) Å2. For CD4: Q12 = (52 ± 7) Å2; Q21 = (34 ± 5) Å2; Q1X = (82 ± 30) Å2; Q2X = (76 ± 22) Å2. An analysis of these results suggests the possibility of resonances with various molecular rotational and vibrational transitions.