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Journal of Physics B Atomic Molecular and Optical Physics

Energy dependence of the Rb 52S1/2–52P1/2 noble-gas collision shift

Hunter Kettering, James C. Camparo

Published Mar 8, 2023• 3 citations
Publisher

Abstract

Abstract For more than a century the study of optical-resonance collision shifts in thermal atomic vapors has provided a window into atom/atom and atom/molecule interactions at low energies (i.e. ∼30 meV). Overall, the agreement between theory and experiment has been good, suggesting that an understanding of these interactions at low energies is well in hand. Here, we present evidence that this is not the case. Using an isoclinic-point method we measure the energy dependence of the Rb D1 collision shift in the noble gases (NGs): He, Ne, Ar, Kr and Xe. While agreement between theory and experiment is quite good for the heavy NGs, it is quite poor for the lighter ones: He and Ne. In the case of Rb/He, not only are the theoretical values in gross disagreement with one another, but they are also in significant disagreement with experiment.

DOI
10.1088/1361-6455/acc292

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Rubidium D1 collision shift by heavy noble gases

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Using an isoclinic-point technique, we measured the ${D}_{1}$ collision shift by Xe, $\ensuremath{\partial}[\ensuremath{\delta}\ensuremath{\nu}]/\ensuremath{\partial}P$, and the exponent $\ensuremath{\kappa}$ of the shift's temperature dependence (i.e., $\ensuremath{\delta}\ensuremath{\nu}\ensuremath{\sim}{T}^{\ensuremath{\kappa}}$). As demonstrated in our examination of the Rb-Kr system [N. P. Wells et al., Phys. Rev. A 89, 052516 (2014)], the isoclinic point provides (arguably) the only means of assessing $\ensuremath{\kappa}$ unambiguously: ${\ensuremath{\kappa}}_{\mathrm{Kr}}\phantom{\rule{4pt}{0ex}}=\phantom{\rule{0.16em}{0ex}}0.36\phantom{\rule{0.16em}{0ex}}\ifmmode\pm\else\textpm\fi{}\phantom{\rule{0.16em}{0ex}}0.06$ and in the present work ${\ensuremath{\kappa}}_{\mathrm{Xe}}\phantom{\rule{4pt}{0ex}}=0.32\ifmmode\pm\else\textpm\fi{}0.05$. With our estimate of $\ensuremath{\kappa}$ for the Rb-Kr and Rb-Xe systems, we were able to combine our Kr and Xe collision shift measurements with those of Rotondaro and Perram [M. D. Rotondaro and G. P. Perram, J. Quant. Spectrosc. Radiat. Transfer 57, 497 (1997)] (another set of high quality $\ensuremath{\partial}[\ensuremath{\delta}\ensuremath{\nu}]/\ensuremath{\partial}P$ measurements) to obtain a highly accurate experimental estimate for the ${D}_{1}$ collision shift resulting from Rb's interaction with the heavy noble gases: For the Rb-Kr interaction $\ensuremath{\partial}[\ensuremath{\delta}\ensuremath{\nu}]/\ensuremath{\partial}P{|}_{T=323\phantom{\rule{0.16em}{0ex}}\mathrm{K}}=\ensuremath{-}5.02\ifmmode\pm\else\textpm\fi{}0.07\phantom{\rule{0.16em}{0ex}}\mathrm{MHz}/\mathrm{torr}$ and for the Rb-Xe interaction $\ensuremath{\partial}[\ensuremath{\delta}\ensuremath{\nu}]/\ensuremath{\partial}P{|}_{T=323\phantom{\rule{0.16em}{0ex}}\mathrm{K}}=\ensuremath{-}5.46\ifmmode\pm\else\textpm\fi{}0.09\phantom{\rule{0.16em}{0ex}}\mathrm{MHz}/\mathrm{torr}$. These measured values for the collision-shift coefficient are approximately $20%$ smaller (in magnitude) than the best theoretical estimates, suggesting that there is room for theoretical improvement regarding our present understanding of how noble-gas collisions perturb the alkali-metal ${P}_{1/2}$ state.

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92 D fine-structure mixing in rubidium by collisions with ground-state Rb and noble-gas atoms

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Theoretical calculation of impact broadening rates of Rb ns Rydberg levels by noble gases

J -Q Sun, P. J. West

The impact broadening rates of Rb ns Rydberg levels by He, Ar and Xe atoms measured by Weber and Niemax (1982) and by Ne and Kr atoms observed by Thompson et al. (1987) are quantitatively explained over the whole range of the principal quantum number n. As Rb ns Rydberg levels (quantum defect delta =3.13) are very close to the nearly hydrogenic high l levels, inelastic collisions make as important a contribution to the broadening rates as elastic collisions. The authors derive the cross sections for the elastic and inelastic using a combination of Kaulakys' (1984) and Lebedev and Marchenko's (1985) impact theories. Good agreement between the theoretical and experimental broadening rates is achieved over the whole range of n.

Journal of Physics B Atomic Molecular and Optical Physics•Nov 28, 1990•7 citations
Abstract For more than a century the study of optical-resonance collision shifts in thermal atomic vapors has provided a window into atom/atom and atom/molecule interactions at low energies (i.e. ∼30 meV). Overall, the agreement between theory and experiment has been good, suggesting that an understanding of these interactions at low energies is well in hand. Here, we present evidence that this is not the case. Using an isoclinic-point method we measure the energy dependence of the Rb D1 collision shift in the noble gases (NGs): He, Ne, Ar, Kr and Xe. While agreement between theory and experiment is quite good for the heavy NGs, it is quite poor for the lighter ones: He and Ne. In the case of Rb/He, not only are the theoretical values in gross disagreement with one another, but they are also in significant disagreement with experiment.
Using an isoclinic-point technique, we measured the D1{D}_{1}D1​ collision shift by Xe, $\ensuremath{\partial}[\ensuremath{\delta}\ensuremath{\nu}]/\ensuremath{\partial}P$, and the exponent $\ensuremath{\kappa}$ of the shift's temperature dependence (i.e., $\ensuremath{\delta}\ensuremath{\nu}\ensuremath{\sim}{T}^{\ensuremath{\kappa}}$). As demonstrated in our examination of the Rb-Kr system [N. P. Wells et al., Phys. Rev. A 89, 052516 (2014)], the isoclinic point provides (arguably) the only means of assessing $\ensuremath{\kappa}$ unambiguously: ${\ensuremath{\kappa}}_{\mathrm{Kr}}\phantom{\rule{4pt}{0ex}}=\phantom{\rule{0.16em}{0ex}}0.36\phantom{\rule{0.16em}{0ex}}\ifmmode\pm\else\textpm\fi{}\phantom{\rule{0.16em}{0ex}}0.06$ and in the present work ${\ensuremath{\kappa}}_{\mathrm{Xe}}\phantom{\rule{4pt}{0ex}}=0.32\ifmmode\pm\else\textpm\fi{}0.05$. With our estimate of $\ensuremath{\kappa}$ for the Rb-Kr and Rb-Xe systems, we were able to combine our Kr and Xe collision shift measurements with those of Rotondaro and Perram [M. D. Rotondaro and G. P. Perram, J. Quant. Spectrosc. Radiat. Transfer 57, 497 (1997)] (another set of high quality $\ensuremath{\partial}[\ensuremath{\delta}\ensuremath{\nu}]/\ensuremath{\partial}P$ measurements) to obtain a highly accurate experimental estimate for the D1{D}_{1}D1​ collision shift resulting from Rb's interaction with the heavy noble gases: For the Rb-Kr interaction $\ensuremath{\partial}[\ensuremath{\delta}\ensuremath{\nu}]/\ensuremath{\partial}P{|}_{T=323\phantom{\rule{0.16em}{0ex}}\mathrm{K}}=\ensuremath{-}5.02\ifmmode\pm\else\textpm\fi{}0.07\phantom{\rule{0.16em}{0ex}}\mathrm{MHz}/\mathrm{torr}$ and for the Rb-Xe interaction $\ensuremath{\partial}[\ensuremath{\delta}\ensuremath{\nu}]/\ensuremath{\partial}P{|}_{T=323\phantom{\rule{0.16em}{0ex}}\mathrm{K}}=\ensuremath{-}5.46\ifmmode\pm\else\textpm\fi{}0.09\phantom{\rule{0.16em}{0ex}}\mathrm{MHz}/\mathrm{torr}$. These measured values for the collision-shift coefficient are approximately 2020%20 smaller (in magnitude) than the best theoretical estimates, suggesting that there is room for theoretical improvement regarding our present understanding of how noble-gas collisions perturb the alkali-metal P1/2{P}_{1/2}P1/2​ state.
Measuring the energy dependence of optical-transition collision shifts has proven extremely difficult, in part because of Doppler broadening and the manifold of overlapping hyperfine components that must be disentangled in the spectra. Here, we demonstrate an approach to these measurements based on spectroscopic isoclinic points. To illustrate the approach's efficacy, we investigated the Kr collision shift of the Rb D1{D}_{1}D1​ transition at 795 nm. For the expected Rb-Kr van der Waals interaction, the collision shift should scale like ${(T/{T}_{o})}^{\ensuremath{\kappa}}$, where To{T}_{\mathrm{o}}To​ is a reference temperature and \ensuremath{\kappa}theo{}_{\mathrm{theo}}theo​ = 0.31. Exemplifying the difficulty of \ensuremath{\kappa} determinations, previous alkali-metal--noble-gas experimental measurements of \ensuremath{\kappa} have varied widely, sometimes in striking disagreement with theory (i.e., factor of 2 larger). In the present work, we not only demonstrate a measurement precision better than 10${}^{\ensuremath{-}10}$/\ifmmode^\circ\else\textdegree\fi{}C, but with our technique we validate the theoretical scaling constant, finding ${\ensuremath{\kappa}}_{\mathrm{expt}}$ = 0.36 \ifmmode\pm\else\textpm\fi{} 0.06.
The cross sections for excitation transfer between the 62P fine-structure substates in rubidium, induced in collisions with noble gas atoms, have been determined in a series of sensitized fluorescence experiments. Mixtures of rubidium vapor and noble gases at pressures varying in the range 0–5 Torr were irradiated with each component of the second 2P rubidium doublet in turn and the following cross sections for 2P mixing were obtained from measurements of sensitised-to-resonance fluorescent intensity ratios. Rb–He: Q12(2P1/2 → 2P3/2) = 29.3 Å2; Q21(2P1/2 ← 2P3/2) = 19.0 Å2. Rb–Ne: Q12 = 10.3 Å2; Q21 = 6.4 Å2. Rb–Ar: Q12 = 24.0 Å2; Q21 = 14.9 Å2. Rb–Kr: Q12 = 23.2 Å2; Q21 = 14.6 Å2. Rb–Xe: Q12 = 43.9 Å2; Q21 = 27.7 Å2 In their dependence on the magnitude of the fine-structure splitting, the values are consistent with previously determined cross sections for mixing in the first and third 2P doublets of alkali atoms.
Normalized emission spectra of the optically excited Rb resonance lines (7800 \AA{}, 7948 \AA{}) have been measured in the presence of He, Ne, Ar, Kr, and Xe for about 50 \AA{} on either side of the lines. The perturber gas pressures were in the range 100-1100 Torr and the temperature was 318 \ifmmode^\circ\else\textdegree\fi{}K. The spectra, normalized to the total emission, are shown to be due to binary collisions. Shifts and widths of the Lorentzian cores of the lines were obtained, at pressures sufficiently low for impact theory to apply. The widths are corrected for the Rb hfs and the instrument function. Various power-law fits to the near-wing intensities are presented and compared to theoretical expectations. The red satellites reported by other authors are found to be, in the low-pressure limit, mere shoulders on the line wing for Ar and Kr, while Xe barely produces an actual peak. The measured linewidths and shifts are compared to previous measurements.
The following cross sections for 92{9}^{2}92D3/2{D}_{3/2}D3/2​\ensuremath{\leftrightarrows}92{9}^{2}92D5/2{D}_{5/2}D5/2​ fine-structure mixing in Rb, induced in collisions with ground-state Rb and noble-gas atoms, have been measured using methods of atomic fluorescence spectroscopy: Q(92{(9}^{2}(92D3/2{D}_{3/2}D3/2​\ensuremath{\rightarrow}92{9}^{2}92D5/2{D}_{5/2}D5/2​) =93, 9, 6, 26, and 42; Q(92{(9}^{2}(92D3/2{D}_{3/2}D3/2​\ensuremath{\leftarrow}92{9}^{2}92D5/2{D}_{5/2}D5/2​) =62, 6, 3, 17, and 23, for Rb, He, Ne, Ar, and Kr, respectively, in units of ${10}^{\mathrm{\ensuremath{-}}14}$ cm2{\mathrm{cm}}^{2}cm2. The measured cross sections are in good agreement with recent theoretical calculations of Sirko and Rosi\ifmmode \acute{n}\else \'{n}\fi{}ski.
The impact broadening rates of Rb ns Rydberg levels by He, Ar and Xe atoms measured by Weber and Niemax (1982) and by Ne and Kr atoms observed by Thompson et al. (1987) are quantitatively explained over the whole range of the principal quantum number n. As Rb ns Rydberg levels (quantum defect delta =3.13) are very close to the nearly hydrogenic high l levels, inelastic collisions make as important a contribution to the broadening rates as elastic collisions. The authors derive the cross sections for the elastic and inelastic using a combination of Kaulakys' (1984) and Lebedev and Marchenko's (1985) impact theories. Good agreement between the theoretical and experimental broadening rates is achieved over the whole range of n.