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Physical Review A

Multiperturber effects in the Faraday spectrum of Rb atoms immersed in a high-density Xe gas

J. P. Woerdman, F.J. Blok, M. Kristensen, C. A. Schrama

Published Feb 1, 1996• 6 citations
Publisher

Abstract

We have measured the ${\mathit{D}}_{1}$ and ${\mathit{D}}_{2}$ Faraday spectrum and absorption spectrum of Rb atoms immersed in high-density Xe buffer gas in the range ${\mathit{n}}_{\mathrm{Xe}}$=0.8--4.5\ifmmode\times\else\texttimes\fi{}${10}^{20}$ ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}$. We find that the shape of the Faraday spectrum obeys the Becquerel relation over this whole density range; however the relative strength of the Faraday effect compared to absorption changes rather abruptly near ${\mathit{n}}_{\mathrm{Xe}}$=1\ifmmode\times\else\texttimes\fi{}${10}^{20}$ ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}$. This is ascribed to the onset of a many-body nature (overlapping collisions) of the Rb:Xe line broadening; the number of perturbers within the Weisskopf sphere is unity at ${\mathit{n}}_{\mathrm{Xe}}$\ensuremath{\sim}1\ifmmode\times\else\texttimes\fi{}${10}^{20}$ ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}$. \textcopyright{} 1996 The American Physical Society.

DOI
10.1103/physreva.53.1183

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Fine-structure mixing in Rb-Xe elastic collisions and isoclinic point asymmetry

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Fine-structure mixing in 72D and 82D Rb atoms, induced in collisions with ground-state atoms and molecules

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Cross sections for ${7}^{2}D$ and ${8}^{2}D$ fine-structure mixing in Rb, induced by collisions with various ground-state atoms and ${\mathrm{N}}_{2}$ molecules, have been determined using methods of atomic fluorescence. Rb vapor, pure or mixed with a buffer gas, was irradiated in a glass fluorescence cell with pulses of radiation from a ${\mathrm{N}}_{2}$ laser-pumped dye laser, populating a $^{2}D$ fine-structure state by two-photon absorption. The resulting fluorescence included a direct component arising from the optically excited state and a sensitized component due to the collisionally populated fine-structure state. Measurements of relative intensities of the two components in relation to buffer-gas pressure yielded the following cross sections (in units of ${10}^{\ensuremath{-}14}$ ${\mathrm{cm}}^{2}$): $Q({7}^{2}{D}_{\frac{3}{2}}\ensuremath{\rightarrow}{7}^{2}{D}_{\frac{5}{2}})=14.1,15.5,\mathrm{and}10.0$; $Q({7}^{2}{D}_{\frac{3}{2}}\ensuremath{\leftarrow}{7}^{2}{D}_{\frac{5}{2}})=9.0,10.5,\mathrm{and}6.9$, for Kr, Xe, and ${\mathrm{N}}_{2}$, respectively; $Q({8}^{2}{D}_{\frac{3}{2}}\ensuremath{\rightarrow}{8}^{2}{D}_{\frac{5}{2}})=8.9,4.9,12.4,24.9,25.8,12.1,\mathrm{and}43.1$; $Q({8}^{2}{D}_{\frac{3}{2}}\ensuremath{\leftarrow}{8}^{2}{D}_{\frac{5}{2}})=5.8,3.2,9.4,15.1,17.6,8.3,\mathrm{and}28.5$, for He, Ne, Ar, Kr, Xe, ${\mathrm{N}}_{2}$, and Rb, respectively. Cross sections for the effective depopulation of the $^{2}D$ states were also determined.

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Rb and Cs broadening of the Na resonance lines

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The broadening of the Na resonance lines, due to collisions with Rb and with Cs, has been measured with the use of the normalized fluorescence-intensity method of Chatham, Lewis, and Gallagher. Several Na resonance-radiation diffusion and absorption corrections were necessary in the Rb case, due to an unavoidable excess of Na density in the Rb vapor. The line-broadening rate coefficients ${k}_{1}$ and ${k}_{2}$ for the ${D}_{1}$ and ${D}_{2}$ resonance lines are ${k}_{1}(\mathrm{Rb})=(6.2\ifmmode\pm\else\textpm\fi{}0.4)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9}$ ${\mathrm{cm}}^{3}$ ${\mathrm{s}}^{\ensuremath{-}1}$, ${k}_{2}(\mathrm{Rb})=(5.5\ifmmode\pm\else\textpm\fi{}0.6)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9}$ ${\mathrm{cm}}^{3}$ ${\mathrm{s}}^{\ensuremath{-}1}$, ${k}_{1}(\mathrm{Cs})=(6.9\ifmmode\pm\else\textpm\fi{}1.0)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9}$ ${\mathrm{cm}}^{3}$ ${\mathrm{s}}^{\ensuremath{-}1}$, and ${k}_{2}(\mathrm{Cs})=(5.5\ifmmode\pm\else\textpm\fi{}0.9)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9}$ ${\mathrm{cm}}^{3}$ ${\mathrm{s}}^{\ensuremath{-}1}$ at $T\ensuremath{\simeq}300$\ifmmode^\circ\else\textdegree\fi{} C. The leading (${C}_{6}{R}^{\ensuremath{-}6}$) dipole-dipole long-range dispersion forces for the Na-Rb and Na-Cs interactions are calculated, and are used in the impact-theory formula to obtain theoretical line-broadening rate coefficients. These are in poor agreement with the measurements, indicating that as suggested by Vadla, the higher-order (${C}_{8}{R}^{\ensuremath{-}8}$) dispersion terms are also important at the very long range responsible for this line broadening.

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High-field measurement of the 129Xe−Rb spin-exchange rate due to binary collisions

Yuan‐Yu Jau, Nicholas N. Kuzma, W. Happer

We have measured the binary spin-exchange rate coefficient for collisions between Rb and ${}^{129}\mathrm{Xe}$ atoms at a magnetic field $B=9.4\mathrm{T}$ and in the temperature range $160<T<200\ifmmode^\circ\else\textdegree\fi{}\mathrm{C}.$ The longitudinal spin-relaxation rate ${1/T}_{1}$ of ${}^{129}\mathrm{Xe}$ is dominated by ${}^{129}\mathrm{Xe}\ensuremath{-}\mathrm{Rb}$ binary collisions. We measured ${1/T}_{1}$ using the methods of conventional nuclear magnetic resonance, with no spin enhancement by optical pumping. At the high magnetic field and large gas pressures used in this work, the contribution of ${}^{129}\mathrm{Xe}\ensuremath{-}\mathrm{Rb}$ molecules to the spin-exchange rate was less than 0.1% of the binary-collision rate. The Rb atomic number density [Rb] was measured directly from the large Faraday rotation of the polarization of near-resonant light passing through the sample cells. The rate coefficient is $\ensuremath{\kappa}{=d(1/T}_{1})/d[\mathrm{Rb}]=(1.75\ifmmode\pm\else\textpm\fi{}0.12)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}16}{\mathrm{cm}}^{3}/\mathrm{s}.$

Physical Review A•Nov 15, 2002•40 citations
We have measured the D1{\mathit{D}}_{1}D1​ and D2{\mathit{D}}_{2}D2​ Faraday spectrum and absorption spectrum of Rb atoms immersed in high-density Xe buffer gas in the range nXe{\mathit{n}}_{\mathrm{Xe}}nXe​=0.8--4.5\ifmmode\times\else\texttimes\fi{}1020{10}^{20}1020 cm\ensuremath−3{\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}cm\ensuremath−3. We find that the shape of the Faraday spectrum obeys the Becquerel relation over this whole density range; however the relative strength of the Faraday effect compared to absorption changes rather abruptly near nXe{\mathit{n}}_{\mathrm{Xe}}nXe​=1\ifmmode\times\else\texttimes\fi{}1020{10}^{20}1020 cm\ensuremath−3{\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}cm\ensuremath−3. This is ascribed to the onset of a many-body nature (overlapping collisions) of the Rb:Xe line broadening; the number of perturbers within the Weisskopf sphere is unity at nXe{\mathit{n}}_{\mathrm{Xe}}nXe​\ensuremath{\sim}1\ifmmode\times\else\texttimes\fi{}1020{10}^{20}1020 cm\ensuremath−3{\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}cm\ensuremath−3. \textcopyright{} 1996 The American Physical Society.
We compare the Faraday spectrum with the dispersion spectrum near the D2{\mathit{D}}_{2}D2​ line of Rb atoms immersed in a high density Xe buffer gas. We observe deviations from the standard Becquerel relation, which relates the Faraday effect of an atomic gas to its dispersion. The deviations are due to coupling of the Rb valence electron to the Xe environment. The Rb D2{\mathit{D}}_{2}D2​ transition dipole moment becomes rotationally locked to the instantaneous collision axes at Xe densities of \ensuremath{\sim}1020{10}^{20}1020 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}$.
We investigate, theoretically and experimentally, the onset of modified electronic precession due to quasimolecular behavior in dense atomic gases. The close connection between the angular coupling of collision pairs and a modification of the Faraday effect is pointed out. We have observed the onset of this quasimolecular modification of the atomic Faraday effect with high-resolution laser measurements of the absorption and Faraday spectra near the D2{\mathit{D}}_{2}D2​ line of Rb atoms immersed in high-density buffer gases. The atomic Faraday effect itself is also affected by the presence of nuclear spin; this modifies the electronic precession through angular-momentum coupling. We describe how to separate the effect of nuclear spin from the effects due to quasimolecular behavior. In this way we establish the existence of angular coupling of the Rb valence electrons to neighboring buffer-gas atoms at densities above \ensuremath{\sim}2\ifmmode\times\else\texttimes\fi{}1019{10}^{19}1019 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}$ in Xe buffer gas. In He buffer gas, quasimolecular modifications of the Faraday effect are approximately two times smaller than for Xe.
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.
Cross sections for 72D{7}^{2}D72D and 82D{8}^{2}D82D fine-structure mixing in Rb, induced by collisions with various ground-state atoms and N2{\mathrm{N}}_{2}N2​ molecules, have been determined using methods of atomic fluorescence. Rb vapor, pure or mixed with a buffer gas, was irradiated in a glass fluorescence cell with pulses of radiation from a N2{\mathrm{N}}_{2}N2​ laser-pumped dye laser, populating a 2D^{2}D2D fine-structure state by two-photon absorption. The resulting fluorescence included a direct component arising from the optically excited state and a sensitized component due to the collisionally populated fine-structure state. Measurements of relative intensities of the two components in relation to buffer-gas pressure yielded the following cross sections (in units of ${10}^{\ensuremath{-}14}$ cm2{\mathrm{cm}}^{2}cm2): $Q({7}^{2}{D}_{\frac{3}{2}}\ensuremath{\rightarrow}{7}^{2}{D}_{\frac{5}{2}})=14.1,15.5,\mathrm{and}10.0$; $Q({7}^{2}{D}_{\frac{3}{2}}\ensuremath{\leftarrow}{7}^{2}{D}_{\frac{5}{2}})=9.0,10.5,\mathrm{and}6.9$, for Kr, Xe, and N2{\mathrm{N}}_{2}N2​, respectively; $Q({8}^{2}{D}_{\frac{3}{2}}\ensuremath{\rightarrow}{8}^{2}{D}_{\frac{5}{2}})=8.9,4.9,12.4,24.9,25.8,12.1,\mathrm{and}43.1$; $Q({8}^{2}{D}_{\frac{3}{2}}\ensuremath{\leftarrow}{8}^{2}{D}_{\frac{5}{2}})=5.8,3.2,9.4,15.1,17.6,8.3,\mathrm{and}28.5$, for He, Ne, Ar, Kr, Xe, N2{\mathrm{N}}_{2}N2​, and Rb, respectively. Cross sections for the effective depopulation of the 2D^{2}D2D states were also determined.
The broadening of the Na resonance lines, due to collisions with Rb and with Cs, has been measured with the use of the normalized fluorescence-intensity method of Chatham, Lewis, and Gallagher. Several Na resonance-radiation diffusion and absorption corrections were necessary in the Rb case, due to an unavoidable excess of Na density in the Rb vapor. The line-broadening rate coefficients k1{k}_{1}k1​ and k2{k}_{2}k2​ for the D1{D}_{1}D1​ and D2{D}_{2}D2​ resonance lines are ${k}_{1}(\mathrm{Rb})=(6.2\ifmmode\pm\else\textpm\fi{}0.4)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{s}}^{\ensuremath{-}1}$, ${k}_{2}(\mathrm{Rb})=(5.5\ifmmode\pm\else\textpm\fi{}0.6)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{s}}^{\ensuremath{-}1}$, ${k}_{1}(\mathrm{Cs})=(6.9\ifmmode\pm\else\textpm\fi{}1.0)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{s}}^{\ensuremath{-}1}$, and ${k}_{2}(\mathrm{Cs})=(5.5\ifmmode\pm\else\textpm\fi{}0.9)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{s}}^{\ensuremath{-}1}$ at $T\ensuremath{\simeq}300$\ifmmode^\circ\else\textdegree\fi{} C. The leading (${C}_{6}{R}^{\ensuremath{-}6}$) dipole-dipole long-range dispersion forces for the Na-Rb and Na-Cs interactions are calculated, and are used in the impact-theory formula to obtain theoretical line-broadening rate coefficients. These are in poor agreement with the measurements, indicating that as suggested by Vadla, the higher-order (${C}_{8}{R}^{\ensuremath{-}8}$) dispersion terms are also important at the very long range responsible for this line broadening.
We have measured the binary spin-exchange rate coefficient for collisions between Rb and 129Xe{}^{129}\mathrm{Xe}129Xe atoms at a magnetic field B=9.4TB=9.4\mathrm{T}B=9.4T and in the temperature range $160<T<200\ifmmode^\circ\else\textdegree\fi{}\mathrm{C}.$ The longitudinal spin-relaxation rate 1/T1{1/T}_{1}1/T1​ of 129Xe{}^{129}\mathrm{Xe}129Xe is dominated by ${}^{129}\mathrm{Xe}\ensuremath{-}\mathrm{Rb}$ binary collisions. We measured 1/T1{1/T}_{1}1/T1​ using the methods of conventional nuclear magnetic resonance, with no spin enhancement by optical pumping. At the high magnetic field and large gas pressures used in this work, the contribution of ${}^{129}\mathrm{Xe}\ensuremath{-}\mathrm{Rb}$ molecules to the spin-exchange rate was less than 0.1% of the binary-collision rate. The Rb atomic number density [Rb] was measured directly from the large Faraday rotation of the polarization of near-resonant light passing through the sample cells. The rate coefficient is $\ensuremath{\kappa}{=d(1/T}_{1})/d[\mathrm{Rb}]=(1.75\ifmmode\pm\else\textpm\fi{}0.12)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}16}{\mathrm{cm}}^{3}/\mathrm{s}.$