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Physical Review

Optical-Pumping Transients in Rubidium-87 and Application to Excited-State Disorientation Cross Sections

Richard Marrus, Joseph Yellin

Published Jan 7, 1966• 15 citations
Publisher

Abstract

Detailed studies have been made of the light transmitted through rubidium-87 vapor during the optical-pumping process, both with and without buffer gas present. The observed transients are single exponentials with no buffer gas present, and double exponentials with buffer gas present, over a wide range of pumping intensities and relaxation times. These results are in excellent agreement with the predictions based on phenomenological equations in which nuclear spin is included and a single relaxation time is assumed. From a study of the amplitudes of the two exponential components of the optical-pumping transient, an effective cross section ${\ensuremath{\sigma}}_{\mathrm{eff}}$ is deduced for the disorientation of rubidium-87 within the $5^{2}P_{\frac{1}{2}}$ state as a result of its collision with a buffer-gas atom. It is shown that ${\ensuremath{\sigma}}_{\mathrm{eff}}={\ensuremath{\sigma}}_{\frac{1}{2}}+{\ensuremath{\sigma}}_{\frac{3}{2}}$, where ${\ensuremath{\sigma}}_{\frac{1}{2}}$ is the cross section for disorientation within the $5^{2}P_{\frac{1}{2}}$ level, and ${\ensuremath{\sigma}}_{\frac{3}{2}}$ is the cross section for transfer from the $5^{2}P_{\frac{1}{2}}$ level to the $5^{2}P_{\frac{3}{2}}$ level by means of collisions with the buffer gas. On the basis of recently measured values for ${\ensuremath{\sigma}}_{\frac{3}{2}}$, values are deduced for ${\ensuremath{\sigma}}_{\frac{1}{2}}$. The cross sections are: ${\ensuremath{\sigma}}_{\frac{1}{2}}(\mathrm{R}\mathrm{b}\ensuremath{-}\mathrm{H}\mathrm{e})=1.5(0.8)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}17}$ ${\mathrm{cm}}^{2}$, ${\ensuremath{\sigma}}_{\frac{1}{2}}(\mathrm{R}\mathrm{b}\ensuremath{-}\mathrm{N}\mathrm{e})=4.4(2.2)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}17}$ ${\mathrm{cm}}^{2}$, and ${\ensuremath{\sigma}}_{\frac{1}{2}}(\mathrm{R}\mathrm{b}\ensuremath{-}\mathrm{A}\mathrm{r})=3.5(1.8)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}16}$ ${\mathrm{cm}}^{2}$. These cross sections are deduced from a model in which the probabilities for ${\mathrm{Rb}}^{87}$ to relax from any hyperfine level to any other are all equal. This model gives a better fit with the observed transients than the assumption that the electron spin only is randomized in the ${P}_{\frac{1}{2}}$ state with the nuclear spin unaffected. We show that accurate relaxation-time measurements can be made by measuring the time constants associated with the double exponentials as a function of light intensity, and extrapolating them to zero light intensity. Moreover, since no shutter is required, relaxation times ${10}^{\ensuremath{-}3}$ sec can be easily observed.

DOI
10.1103/physrev.141.130

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•Sep 4, 1964•0 citations
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Detailed studies have been made of the light transmitted through rubidium-87 vapor during the optical pumping process, both with and without buffel" gas present.The observed transients are single expo .. nentials with no buffer gas present, and double exponentials with buf'fel" gas present over a wide range of pumping intensities and relaxation times.These results are in excellent agreement with the predictions based on phenomenological equations in which nuclear spin in included a.nd a single relaxation time is assumed.From a study of the amplitudes of the two exponential components of the optical-pumping transient, an effective cross section (] eff is deduced for the disorientation of 2 .' .'•.• I'..
The hyperfine relaxation of a population difference, produced by optical pumping, between the F=1F=1F=1 mF=0{m}_{F}=0mF​=0 and F=2F=2F=2 mF=0{m}_{F}=0mF​=0 energy levels of the ground state of Rb87{\mathrm{Rb}}^{87}Rb87, has been studied in cells containing neon, argon, helium, or krypton as a buffer gas. The relaxation times T1{T}_{1}T1​ and T2{T}_{2}T2​ have been measured as a function of the rubidium vapor pressure in the cell. The relaxation rate due to spin exchange in Rb87{\mathrm{Rb}}^{87}Rb87-Rb87{\mathrm{Rb}}^{87}Rb87 collisions has been found equal to 65 ${\mathrm{sec}}^{\ensuremath{-}1}$ at 44\ifmmode^\circ\else\textdegree\fi{}C, and the diffusion coefficients of Rb87{\mathrm{Rb}}^{87}Rb87 atoms in He, Ne, and Ar evaluated as 0.6, 0.31, and 0.22 cm2{\mathrm{cm}}^{2}cm2 ${\mathrm{sec}}^{\ensuremath{-}1}$, respectively. The cross section for Rb87{\mathrm{Rb}}^{87}Rb87-Ne and Rb87{\mathrm{Rb}}^{87}Rb87-Ar collisions are found to be 1.6\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}22}$ cm2{\mathrm{cm}}^{2}cm2 and 9\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}22}$ cm2{\mathrm{cm}}^{2}cm2. These values are in general agreement with values previously obtained by other methods. The extrapolated values of 1T2\frac{1}{{T}_{2}}T2​1​ for zero vapor pressure of rubidium are 185, 237, and 318 ${\mathrm{sec}}^{\ensuremath{-}1}$ for Ne, He, or Ar, respectively. Relaxations by the pumping light or by the magnetic field inhomogeneities are also discussed.
In a hyperfine-optical-pumping experiment we employed the Franzen transient method to determine the total spin-exchange cross sections for Rb87{\mathrm{Rb}}^{87}Rb87-Rb87{\mathrm{Rb}}^{87}Rb87 and Rb87{\mathrm{Rb}}^{87}Rb87-Cs133{\mathrm{Cs}}^{133}Cs133 collisions at 78\ifmmode^\circ\else\textdegree\fi{}C. Values determined in this way were: $\ensuremath{\sigma}({\mathrm{Rb}}^{87}\ensuremath{-}{\mathrm{Rb}}^{87})=(1.9\ifmmode\pm\else\textpm\fi{}0.2)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}$ cm2{\mathrm{cm}}^{2}cm2 and $\ensuremath{\sigma}({\mathrm{Rb}}^{87}\ensuremath{-}{\mathrm{Cs}}^{133})=(2.3\ifmmode\pm\else\textpm\fi{}0.2)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}$ cm2{\mathrm{cm}}^{2}cm2. A large difference between the ground-state hyperfine populations was established by pumping with light absorbable by atoms in only one hyperfine level. In the presence of a second unpumped species, the resulting polarization relaxed with a characteristic rate of $\frac{1}{\ensuremath{\tau}}=\frac{1}{T}+\frac{1}{{T}_{S1}}+\frac{1}{{T}_{E1}}$, where TTT is the non-spin-exchange relaxation time and TS1{T}_{S1}TS1​ and TE1{T}_{E1}TE1​ are the self- and cross-exchange times. Then $\ensuremath{\tau}$ was obtained by fitting the signal to a single exponential and applying a small correction ($\ensuremath{\approx}10%$) to account for the fact that the signal is only approximately proportional to the polarization (and hence to a single exponential). The relaxation measurement utilized rapid data accumulation with a Kerr-cell shutter and pulse-height analyzer. The cross section can be easily deduced from the relaxation times if the corresponding densities are known. Each density was measured by determining the integral over all frequencies of the absorption coefficient by means of a scanning Fabry-Perot interferometer. We describe how to remove the effect of the Fabry-Perot on the true emission and absorption profiles.
The spin relaxation of optically pumped rubidium vapor induced by rubidium-rare-gas atomic collisions has been investigated in an ultraclean environment. The experiment was performed under conditions such that the partial pressure of nonrare-gas impurities was less than 1\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}8}$ Torr, and that the time between Rb-Rb spin exchange collisions was short compared to the spin relaxation time. The cross sections (in cm2{\mathrm{cm}}^{2}cm2) for disorientation of rubidium were found to be: He, 3.3\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}25}$; Ne, 3.3\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}24}$; Ar, 1.1\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}22}$; Kr, 7.3\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}21}$; Xe, 1.3\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}19}$. The fact that these cross sections are considerably smaller than previously reported values is attributed primarily to the low degree of impurity contamination in the present work. When compared with already existing values for cesium and sodium, the disorientation cross sections of these three alkali metals are seen to have a remarkably similar dependence on buffer-gas atomic number. The new experimental values are also compared with recent theoretical calculations.
A new optical method for studying the spin relaxation of optically aligned rubidium vapor is described. In this method, the pumping radiation, consisting of circularly polarized D1{D}_{1}D1​ resonance radiation, is suddenly shut off and then turned on again after a known time interval. The relaxation which takes place during the interval of darkness causes the vapor to become more opaque to the pumping radiation at a rate which is determined by the relaxation time. A large degree of alignment, as well as a relaxation time of about 80 milliseconds, were observed in a closed-off evacuated cylindrical glass cell completely lined, except for 1200\frac{1}{200}2001​ of the wall area, with a thin film of tetracontane (C40{\mathrm{C}}_{40}C40​H82{\mathrm{H}}_{82}H82​). The variation of relaxation time with buffer gas pressure was studied in this cell and in an unlined glass cell. From the observations with the unlined cell, diffusion coefficients for rubidium in neon and argon of 0.31 cm2{\mathrm{cm}}^{2}cm2/sec and 0.24 cm2{\mathrm{cm}}^{2}cm2/sec, respectively, can be deduced. Observed cross sections for disorientation collisions between aligned ground-state rubidium atoms and neon, argon, krypton, and xenon atoms are 5.2\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}23}$ cm2{\mathrm{cm}}^{2}cm2, 3.7\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}22}$ cm2{\mathrm{cm}}^{2}cm2, 5.9\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}21}$ cm2{\mathrm{cm}}^{2}cm2, and 1.3\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}20}$ cm2{\mathrm{cm}}^{2}cm2, respectively. In the evacuated tetracontane-lined cell, the relaxation time decreased by 30% for a tenfold increase in rubidium vapor pressure. An explanation for this relatively weak dependence is suggested. The longest observed relaxation time was approximately 0.4 seconds in a tetracontanelined cell filled with neon to a pressure of 3 cm Hg.