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Physical Review A

6P13−6P03 Excitation Transfer in Mercury, Induced in Collisions with N2 Molecules

John M. Pitre, K. Hammond, L. Krause

Published Dec 1, 1972• 39 citations
Publisher

Abstract

The cross section for the transition $6^{3}P_{0}\ensuremath{\rightarrow}6^{3}P_{1}$ in mercury, induced in collisions with ${\mathrm{N}}_{2}$ molecules, has been determined by the method of delayed coincidences. The Hg $^{3}P_{1}$ state was excited by pulses of 2537-\AA{} Hg resonance radiation and the decay of the long-lived 2537-\AA{} afterglow was studied in relation to ${\mathrm{N}}_{2}$ pressure. The resulting cross section ${Q}_{12}(^{3}P_{0}\ensuremath{\rightarrow}^{3}P_{1})=4.18\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}4}$ ${\mathrm{\AA{}}}^{2}$ was found to be good agreement with the prediction of the principle of detailed balancing when compared with the cross section ${Q}_{21}(^{3}P_{1}\ensuremath{\rightarrow}^{3}P_{0})$. It was also found that, within the sensitivity of the method, collisions with ${\mathrm{N}}_{2}$ molecules do not quench $^{3}P_{1}$ or $^{3}P_{0}$ Hg atoms to the ground state.

DOI
10.1103/physreva.6.2101

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The cross section for the transition 63P0\ensuremath→63P16^{3}P_{0}\ensuremath{\rightarrow}6^{3}P_{1}63P0​\ensuremath→63P1​ in mercury, induced in collisions with N2{\mathrm{N}}_{2}N2​ molecules, has been determined by the method of delayed coincidences. The Hg 3P1^{3}P_{1}3P1​ state was excited by pulses of 2537-\AA{} Hg resonance radiation and the decay of the long-lived 2537-\AA{} afterglow was studied in relation to N2{\mathrm{N}}_{2}N2​ pressure. The resulting cross section Q12(3P0\ensuremath→3P1)=4.18\ifmmode×\else\texttimes\fi10\ensuremath−4{Q}_{12}(^{3}P_{0}\ensuremath{\rightarrow}^{3}P_{1})=4.18\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}4}Q12​(3P0​\ensuremath→3P1​)=4.18\ifmmode×\else\texttimes\fi10\ensuremath−4 A˚2{\mathrm{\AA{}}}^{2}A˚2 was found to be good agreement with the prediction of the principle of detailed balancing when compared with the cross section Q21(3P1\ensuremath→3P0){Q}_{21}(^{3}P_{1}\ensuremath{\rightarrow}^{3}P_{0})Q21​(3P1​\ensuremath→3P0​). It was also found that, within the sensitivity of the method, collisions with N2{\mathrm{N}}_{2}N2​ molecules do not quench 3P1^{3}P_{1}3P1​ or 3P0^{3}P_{0}3P0​ Hg atoms to the ground state.
The excitation transfer cross sections to several of the excited states of thallium from the 63P16^{3}P_{1}63P1​ and 63P06^{3}P_{0}63P0​ states of mercury have been obtained at various temperatures in the range 800\ifmmode^\circ\else\textdegree\fi{}C to 900\ifmmode^\circ\else\textdegree\fi{}C. Analysis of the equilibrium rates of absorption, emission, and collision processes allows the calculation of excitation transfer cross sections from experimentally determined ratios of intensities of thallium-sensitized fluorescence lines to the intensity of mercury resonance fluorescence, using calculated values of the thallium transition probabilities. The values obtained for the excitation transfer cross sections are comparable in magnitude with collision cross sections based on considerations of gas kinetics.
When a mercury atom in the resonance 63P16^{3}P_{1}63P1​ state collides with a nitrogen molecule, it may be transferred to the metastable 63P06^{3}P_{0}63P0​ state. The cross section for this reaction has been measured by a new method. Mercury vapor, in the presence of a known pressure of nitrogen gas, is excited by 2537A radiation. After the source of the excitation is cut off, the decay time of the imprisoned radiation is observed. The quenching collision cross section ${\ensuremath{\sigma}}_{Q}$ is calculated from the measured decay time and the known value of the imprisonment time in the absence of the quenching gas. Measurements have been taken over the temperature range 325-525\ifmmode^\circ\else\textdegree\fi{}K; ${\ensuremath{\sigma}}_{Q}$ is found to increase from 5.0\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}17}$ cm2{\mathrm{cm}}^{2}cm2 at the lower temperature to 1.0\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}16}$ cm2{\mathrm{cm}}^{2}cm2 at the upper temperature.
The quenching and depolarization of mercury resonance radiation (2537 Å), induced in collisions of Hg(63P1) atoms with various molecules has been investigated using the method of delayed coincidences. The following total quenching cross sections have been obtained for the process Hg(63P1) → Hg(63P0, 61S0): Hg–H2, 24.6 Å2; Hg–D2, 22.7 Å2; Hg–CO, 21.7 Å2; Hg–CO2, 10.2 Å2; Hg–O2, 60.5 Å2; Hg–14N2, 0.73 Å2; Hg–15N2, 0.78 Å2; and Hg–Xe, < 0.002 Å2. A cross section of 267 Å2 has been measured for the depolarization of the resonance radiation by collisions with CO2 molecules.
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Excitation transfer between the 62P126 ^{2}P_{\frac{1}{2}}62P21​​ and 62P326 ^{2}P_{\frac{3}{2}}62P23​​ resonance states in cesium, induced by Cs-N2{\mathrm{N}}_{2}N2​ and Cs-H2{\mathrm{H}}_{2}H2​ collisions, was observed in the first experiment of its kind, in which techniques of sensitized fluorescence are used to investigate collisional mixing between resonance states of alkali atoms in mixtures with molecular gases. The cesium-vapor-gas system, in which the cesium vapor pressure was low enough to avoid radiation trapping, was irradiated with a single component of the resonance doublet. The fluorescent light, which contained both components of the doublet, was monitored at right angles to the direction of excitation. Measurements of relative intensities of the fluorescent components yielded the following cross sections for excitation transfer and for quenching of resonance radiation. For Cs-N2{\mathrm{N}}_{2}N2​ collisions: ${Q}_{12}(^{2}P_{\frac{1}{2}}\ensuremath{\rightarrow}^{2}P_{\frac{3}{2}})=3.6$ A˚2{\mathrm{\AA{}}}^{2}A˚2, ${Q}_{21}(^{2}P_{\frac{1}{2}}\ensuremath{\leftarrow}^{2}P_{\frac{3}{2}})=16.2$ A˚2{\mathrm{\AA{}}}^{2}A˚2, ${Q}_{10}(^{2}S_{\frac{1}{2}}\ensuremath{\leftarrow}^{2}P_{\frac{1}{2}})=55.2$ A˚2{\mathrm{\AA{}}}^{2}A˚2, ${Q}_{20}(^{2}S_{\frac{1}{2}}\ensuremath{\leftarrow}^{2}P_{\frac{3}{2}})=63.5$ A˚2{\mathrm{\AA{}}}^{2}A˚2. For Cs-H2{\mathrm{H}}_{2}H2​ collisions: Q12=6.7{Q}_{12}=6.7Q12​=6.7 A˚2{\mathrm{\AA{}}}^{2}A˚2, Q21=29.6{Q}_{21}=29.6Q21​=29.6 A˚2{\mathrm{\AA{}}}^{2}A˚2, Q10=11.7{Q}_{10}=11.7Q10​=11.7 A˚2{\mathrm{\AA{}}}^{2}A˚2, Q20=6.7{Q}_{20}=6.7Q20​=6.7 A˚2{\mathrm{\AA{}}}^{2}A˚2. The large sizes of the excitation-transfer cross sections, which are comparable to the corresponding Cs-Cs cross sections, are attributed to resonances with transitions in the molecules.