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Journal of Physics B Atomic and Molecular Physics

Fine-structure transitions in Rb(5P) induced by H2and N2molecules

J.‐M. Mestdagh, P de Pujo, J. Cuvellier, A Binet, P. R. Fournier, J. Berlande

Published Feb 28, 1982• 14 citations
Publisher

Abstract

The energy dependence and the absolute value of the cross section for the P 1/2 to P 3/2 fine-structure transition (FST) in Rb(5P) induced by H 2 or N 2 molecules and He atoms has been measured for the first time in a crossed-beam apparatus. The results for He, in excellent agreement with previous experimental data, are used for comparing atomic and molecular target behaviour with regard to FST processes in heavy alkalis. One observes much larger cross sections for H 2 and N 2 at low energies with a much weaker energy dependence. Theoretical work suggests two seemingly competing mechanisms for including large FST cross sections for molecular targets. One, involving an intermediate ionic complex, accounts for the general trend (absolute value and energy dependence) of the experimental data for N 2 while the other, recently suggested by Hickman seems to play the major role when H 2 is the target.

DOI
10.1088/0022-3700/15/4/017

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Fine-structure transition cross sections in Rb(5P) induced by molecules H2、N2、CO、CO2 having been measured using methods of flourcence are reprented. Experimental results show that values of cross-sections are good agree with Mestdagh's (1982) cross-beam experimental data and 2-4 order of magnitude larger than Rb(5P)-inert gases but less than the geometrical cross sections. It is note that in the case of CO and CO2 are less smaller. Resonant transfers have yet to be confirmed.

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Radiative transport and collisional transfer of excitation energy in Rb(5P)atoms mixed with N_2

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Applying the CW laser absorption and fluorescence method,the cross sections for the fine structure mixing and quenching of the Rb(5P)state,induced by collision with N2 molecules,have been measured.Cesium atoms were optically excited to the 5P3/2 state.The excited atom density and spatial distribution were mapped by monitoring the absorption of a counterpropagating single mode laser beam,turned to the 5PJ→7S1/2 transitions.The effective radiative rates were calculated for the 5PJ→5S transitions.The fluorescence intensity I794 of the sensitized 5P1/2→5S1/2 emission was measured as a function of N2 density in the range 0.5×1016N4×1016cm-3 at constant temperature T=340 K.It was found that the quantity N/I794 exhibited a parabolic dependence on N,confirming that the quenching of the 5PJ states is due to collision with N2 molecules,not Rb ground state atoms.The coefficients of the second-order polynomial fitted through the measured data yielded the cross sections σ3/2→1/2=(10.43±3.54)×10-16cm2 and σD=(9.8±3.4)×10-16cm2 for the 5PJ fine-structure mixing and quenching,respectively,due to collision with N2 atoms.Our values for these cross sections are in agreement,within combined error bars,with values we have recently obtained under different experimental conditions.

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[Measurement of fine-structure branching ratios for Rb-He optical collisions].

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Experimental ratios of branching in the fine-structure levels of the Rb5P multiplet, as a consequence of an optical collision with He, are reported. The process studied is Rb(5S1/2 )+ He + hrv --> Rb(5P(J)) +He, where the pulsed laser frequency v is tuned in the wings of the Rb resonance transitions. The authors defined the detuning delta to be v-v (D2 )(delta > 0) for laser frequency v highter than that of RbD2 transition and to be v-v (D1)(delta < 0) for v lower than the RbD1 transition. As RbHe molecular states are correlated to the two 5 2P(J) states, there is some likelihood that the molecule will dissociate into 5 2P1/2 or 5P3/2 state. The dissociation results in a nonuniform distribution of atomic Rb5P(J) states. The branching ratios are defined as n1/n2, where n1 and n2 are densities of the 5P1/2 and 5P3/2 states dissociated. To determine experimentally the relative cross section for scattering into the two fine-structure states, the relative time-intergrated intensities of the resulting Rb emission lines, I(5P3/2 --> 5P1/2 )[I(D2)] and I(5P1/2 --> 5P3/2) ) [I(D1)], were measured. The ratios are determined by detunings from about 200 cm(-1) in the blue wing to -180 cm(-1) in the red wing of the Rb5P multiplet. A rate equation analysis of the pressure dependence was yielded. The branching ratios and cross sections for collisional 5P1/2 --> 5P3/2 transition were obtained from the slope and intercept. The blue-wing branching ratios show a detuning-dependent approach to limit of 0. 2. The branching was found to be very large (-40) in the red wing, irrespective of the detuning. Fine structure changing cross section (1.1 +/- 0.3) x 10(-17) cm2 was measured from wing excitation, and the result is consistent with the cross section obtained from resonant excitation of the Rb5P(J) state. The measurements show a strong sensitivity to interatomic potentials and to nonadiabatic effects in dissociation dynamics.

•Jul 1, 2009•0 citations
The energy dependence and the absolute value of the cross section for the P 1/2 to P 3/2 fine-structure transition (FST) in Rb(5P) induced by H 2 or N 2 molecules and He atoms has been measured for the first time in a crossed-beam apparatus. The results for He, in excellent agreement with previous experimental data, are used for comparing atomic and molecular target behaviour with regard to FST processes in heavy alkalis. One observes much larger cross sections for H 2 and N 2 at low energies with a much weaker energy dependence. Theoretical work suggests two seemingly competing mechanisms for including large FST cross sections for molecular targets. One, involving an intermediate ionic complex, accounts for the general trend (absolute value and energy dependence) of the experimental data for N 2 while the other, recently suggested by Hickman seems to play the major role when H 2 is the target.
The cross sections for fine-structure transition (FST) of Rb(7 2 D ) atoms induced by collision with molecules of H 2 and CO have been experimentally determined by the method of selective stepwise excitation of Rb atoms and observation of the resulting fluorescence. The cross sections (in units of 10 -14 cm 2 ) for Rb(7 2 D )-H 2 are σ fs *(7 2 D 5/2 → 7 2 D 3/2 ) = 0.16 ± 0.03, σ fs *'(7 2 D 3/2 → 7 2 D 5/2 ) = 0.24 ± 0.05, for Rb(7 2 D )-CO: σ fs * = 0.10 ± 0.06 and σ fs * ' = 0.15 ± 0.09. The cross sections σ tr * for transfer out of the 7 2 D doublet were also determined.
Applying the CW laser absorption and fluorescence method,the cross sections for the fine structure mixing and quenching of the Rb(5P)state,induced by collision with N2 molecules,have been measured.Cesium atoms were optically excited to the 5P3/2 state.The excited atom density and spatial distribution were mapped by monitoring the absorption of a counterpropagating single mode laser beam,turned to the 5PJ→7S1/2 transitions.The effective radiative rates were calculated for the 5PJ→5S transitions.The fluorescence intensity I794 of the sensitized 5P1/2→5S1/2 emission was measured as a function of N2 density in the range 0.5×1016N4×1016cm-3 at constant temperature T=340 K.It was found that the quantity N/I794 exhibited a parabolic dependence on N,confirming that the quenching of the 5PJ states is due to collision with N2 molecules,not Rb ground state atoms.The coefficients of the second-order polynomial fitted through the measured data yielded the cross sections σ3/2→1/2=(10.43±3.54)×10-16cm2 and σD=(9.8±3.4)×10-16cm2 for the 5PJ fine-structure mixing and quenching,respectively,due to collision with N2 atoms.Our values for these cross sections are in agreement,within combined error bars,with values we have recently obtained under different experimental conditions.
Fine-structure mixing cross-sections for the alkalis in collisions with the rare gases are reviewed. Included in the review are all the rare gases in collisions with all of the first excited state of the alkalis, the second excited state for K, Rb and Cs and the third excited state for Rb and Cs. The cross-sections are converted to probabilities for energy transfer using a quantum-defect calculated cross-section and are then presented as a function of adiabaticity. The data shows a clear decreasing trend with adiabaticity but secondary factors prevent the probabilities from decreasing as quickly as expected. Polarizability is introduced as a proxy for the secondary influences on the data as it increases with both rare gas partner and alkali excited state. The polarizability is shown to cause the probability of fine structure transition to be higher than expected. An empirical model is introduced and fit to the data. Future work will develop a model using time-independent perturbation theory in order to further develop a physical rational for the dependence of fine structure cross sections on adiabaticity and to further understand the secondary influences on the probability for fine structure transition.
Employing ultrafast laser excitation and time-correlated single-photon counting, we have measured the fine-structure transfer between Rb 5P states induced by collisions with 4He buffer gas at temperatures up to 150 °C. The temperature dependence of the binary cross section agrees with earlier measurements. Our data show that the temperature dependence of the three-body rate is about the same as that of the binary rate. The three-body rate can be described as arising from the reduction of the rubidium fine-structure splitting due to nearby helium atoms.
Experimental ratios of branching in the fine-structure levels of the Rb5P multiplet, as a consequence of an optical collision with He, are reported. The process studied is Rb(5S1/2 )+ He + hrv --> Rb(5P(J)) +He, where the pulsed laser frequency v is tuned in the wings of the Rb resonance transitions. The authors defined the detuning delta to be v-v (D2 )(delta > 0) for laser frequency v highter than that of RbD2 transition and to be v-v (D1)(delta < 0) for v lower than the RbD1 transition. As RbHe molecular states are correlated to the two 5 2P(J) states, there is some likelihood that the molecule will dissociate into 5 2P1/2 or 5P3/2 state. The dissociation results in a nonuniform distribution of atomic Rb5P(J) states. The branching ratios are defined as n1/n2, where n1 and n2 are densities of the 5P1/2 and 5P3/2 states dissociated. To determine experimentally the relative cross section for scattering into the two fine-structure states, the relative time-intergrated intensities of the resulting Rb emission lines, I(5P3/2 --> 5P1/2 )[I(D2)] and I(5P1/2 --> 5P3/2) ) [I(D1)], were measured. The ratios are determined by detunings from about 200 cm(-1) in the blue wing to -180 cm(-1) in the red wing of the Rb5P multiplet. A rate equation analysis of the pressure dependence was yielded. The branching ratios and cross sections for collisional 5P1/2 --> 5P3/2 transition were obtained from the slope and intercept. The blue-wing branching ratios show a detuning-dependent approach to limit of 0. 2. The branching was found to be very large (-40) in the red wing, irrespective of the detuning. Fine structure changing cross section (1.1 +/- 0.3) x 10(-17) cm2 was measured from wing excitation, and the result is consistent with the cross section obtained from resonant excitation of the Rb5P(J) state. The measurements show a strong sensitivity to interatomic potentials and to nonadiabatic effects in dissociation dynamics.