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Physical Review A

Rubidium D1 collision shift by heavy noble gases

N. P. Wells, Travis U. Driskell, James C. Camparo

Published Oct 13, 2015• 2 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.92.042509

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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.
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.
For years, inelastic, fine-structure-changing collisions between excited alkali-metal atoms and noble-gas perturbers have been a source of information on the alkali-metal--noble-gas interaction. Here, we consider the role of elastic fine-structure-mixing collisions on alkali-metal absorption cross sections. Specifically, we consider the four optical hyperfine transitions of the D1{D}_{1}D1​ absorption spectrum for 87Rb^{87}\mathrm{Rb}87Rb, and in particular the doublet corresponding to $5^{2}S_{1/2}({F}_{g}=2)\ensuremath{-}5^{2}P_{1/2}({F}_{e}=1,2)$ transitions. Although ideally the amplitudes of the doublet's absorption cross sections are identical, we find that fine-structure mixing of D2{D}_{2}D2​ oscillator strength into the D1{D}_{1}D1​ spectrum breaks the cross sections' equality and leads to doublet asymmetry. We obtain a fine-structure mixing parameter $\ensuremath{\lambda}$ of $(5.4\ifmmode\pm\else\textpm\fi{}0.3)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}21}\phantom{\rule{0.16em}{0ex}}\mathrm{c}{\mathrm{m}}^{3}$, and estimate a 52P1/25^{2}P_{1/2}52P1/2​ hyperfine-splitting density shift $\ensuremath{\zeta}$ in the 87Rb^{87}\mathrm{Rb}87Rb-Xe system of $+0.71\ifmmode\pm\else\textpm\fi{}0.03\phantom{\rule{0.16em}{0ex}}\mathrm{GHz}/\mathrm{amagat}$. These results have implications for spectroscopic applications of the 87Rb^{87}\mathrm{Rb}87Rb isoclinic point, which we consider as part of our conclusions.
Inelastic collisional processes in fine-structure-state mixing have been studied by selective stepwise excitation and observation of the resulting fluorescence during collisions of excited rubidium 62D526^{2}D_{\frac{5}{2}}62D25​​ state atoms with various noble-gas atoms. It is shown that for intermediately excited rubidium atoms the fine-structure-state mixing cross sections are generally increasing from helium to xexon. The cross sections for the process $\mathrm{Rb}(6^{2}D_{\frac{5}{2}})+A(n^{1}S_{0})\ensuremath{\rightarrow}\mathrm{Rb}(6^{2}D_{\frac{3}{2}})+A(n^{1}S_{0})+\ensuremath{\Delta}E$ have the values ${\ensuremath{\sigma}}_{\mathrm{fs}}^{*}=2.4\ifmmode\pm\else\textpm\fi{}0.9, 3.1\ifmmode\pm\else\textpm\fi{}1.2, 2.6\ifmmode\pm\else\textpm\fi{}1.0, 5.8\ifmmode\pm\else\textpm\fi{}2.2, \mathrm{and} 9.3\ifmmode\pm\else\textpm\fi{}5.6$ in units of ${10}^{\ensuremath{-}14}$ cm2{\mathrm{cm}}^{2}cm2, where AAA denotes in sequence any one of the noble gas atoms He, Ne, Ar, Kr, and Xe, respectively. Transfer cross sections for the transfer of excited Rb62D6^{2}D62D-state atoms out of the doublet were also determined and are about an order of magnitude smaller than the fine-structure-mixing cross sections.
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.