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Physical Review

Measurement of Spin-Exchange Cross Sections for Cs133 , Rb87 , Rb85 , K39 , and Na23

N Ressler, Richard H. Sands, Thomas Edison. Stark

Published Aug 5, 1969• 69 citations
Publisher

Abstract

This paper reports measurements to determine the spin-exchange cross section for collisions between like alkali atoms. The spin-exchange cross section is determined for ${\mathrm{Cs}}^{133}$, ${\mathrm{Rb}}^{87}$, ${\mathrm{Rb}}^{85}$, ${\mathrm{K}}^{39}$, and ${\mathrm{Na}}^{23}$. The lifetime of the alkali atoms in the Zeeman sublevels of the ground-state hyperfine levels is dominated by spin-exchange collisions. The spin-exchange collision rate is therefore reflected by the linewidth of the microwave absorption spectrum observed in the magnetic dipole transitions between various of the Zeeman sublevels. The measurements employed an $X$-band electron paramagnetic resonance spectrometer. The alkali metal was distilled into a sample bulb which was placed inside a Dewar in a resonant cavity. The bulb was then heated to a temperature corresponding to an equilibrium vapor density of approximately ${10}^{15}$ alkali atoms/c.c. and the microwave absorption spectrum was recorded. In order to relate the spin-exchange rate to a cross section, it is necessary to determine the alkali density. This was done by comparing the intensity of the alkali EPR absorption to that of a weighed and oriented copper sulfate crystal. For ${\mathrm{Cs}}^{133}$ and ${\mathrm{Rb}}^{87}$, interpretation of the linewidth data is complicated by the fact that the transitions occur in a region where there is appreciable mixing of the high-field spin states by the hyperfine interaction. A density-matrix description of spin exchange which corrects for this intermediate field mixing is discussed, and the corrections are applied to the measured cross sections for two transitions in ${\mathrm{Cs}}^{133}$ and ${\mathrm{Rb}}^{87}$. Relative cross sections, referred to that of ${\mathrm{Na}}^{23}$, are also given.

DOI
10.1103/physrev.184.102

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Optics and Spectroscopy•Nov 1, 2010•15 citations
This paper reports measurements to determine the spin-exchange cross section for collisions between like alkali atoms. The spin-exchange cross section is determined for Cs133{\mathrm{Cs}}^{133}Cs133, Rb87{\mathrm{Rb}}^{87}Rb87, Rb85{\mathrm{Rb}}^{85}Rb85, K39{\mathrm{K}}^{39}K39, and Na23{\mathrm{Na}}^{23}Na23. The lifetime of the alkali atoms in the Zeeman sublevels of the ground-state hyperfine levels is dominated by spin-exchange collisions. The spin-exchange collision rate is therefore reflected by the linewidth of the microwave absorption spectrum observed in the magnetic dipole transitions between various of the Zeeman sublevels. The measurements employed an XXX-band electron paramagnetic resonance spectrometer. The alkali metal was distilled into a sample bulb which was placed inside a Dewar in a resonant cavity. The bulb was then heated to a temperature corresponding to an equilibrium vapor density of approximately 1015{10}^{15}1015 alkali atoms/c.c. and the microwave absorption spectrum was recorded. In order to relate the spin-exchange rate to a cross section, it is necessary to determine the alkali density. This was done by comparing the intensity of the alkali EPR absorption to that of a weighed and oriented copper sulfate crystal. For Cs133{\mathrm{Cs}}^{133}Cs133 and Rb87{\mathrm{Rb}}^{87}Rb87, interpretation of the linewidth data is complicated by the fact that the transitions occur in a region where there is appreciable mixing of the high-field spin states by the hyperfine interaction. A density-matrix description of spin exchange which corrects for this intermediate field mixing is discussed, and the corrections are applied to the measured cross sections for two transitions in Cs133{\mathrm{Cs}}^{133}Cs133 and Rb87{\mathrm{Rb}}^{87}Rb87. Relative cross sections, referred to that of Na23{\mathrm{Na}}^{23}Na23, are also given.
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.
In this paper we calculate the effect of spin-exchange collisions in alkali-metal vapors. In the framework of the high-energy approximation, we evaluate the spin-exchange cross sections related to the line broadening and to the frequency shift of the ground state hyperfine transition. We do the calculation for the four isotopes, 23Na^{23}\mathrm{Na}23Na, 39K^{39}\mathrm{K}39K, 87Rb^{87}\mathrm{Rb}87Rb, and 133Cs^{133}\mathrm{Cs}133Cs. The results are used in particular to evaluate the spin-exchange frequency shift in Rb vapor cell frequency standards used in many applications. It turns out that, due to possible fluctuations in the atomic density, spin exchange may affect significantly the medium and long term frequency stability of the frequency standard.
Collisions of alkali-metal atoms in the ground state with the electron spin S = 1/2 are accompanied by exchange of electron coordinates between colliding particles, which leads to polarization transfer between them (i.e., to the well-known phenomenon of spin exchange). In addition, along with the polarization transfer from one partner to another, the magnetic resonance lines of colliding atoms are broadened and shifted in spin-exchange collisions. In particular the last two processes depend on the complex spin-exchange cross section. The real part of the cross section determines the so-called "spin-exchange cross section," which is responsible for the broadening of magnetic resonance lines, while the imaginary part determines the shift cross section, which governs the frequency shift of magnetic resonance. In order to describe the spin-exchange process one have to know complex spin-exchange cross sections. Complex spin-exchange cross sections are calculated on the basis of the data on the singlet (X 1 Σ + ) and triplet (a 3 Σ + ) potentials describing the interaction alkali-metal atoms in the ground state. Collisions of alkali-metal atoms Cs, Rb, K, Na in the ground state are considered in the energy interval of 10 −4 −10 −2 au.
The spin-exchange cross section for Rb85{\mathrm{Rb}}^{85}Rb85-Rb87{\mathrm{Rb}}^{87}Rb87 collisions has been measured to be (1.70\ifmmode\pm\else\textpm\fi{}0.21)\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}14}$ cm2{\mathrm{cm}}^{2}cm2 using the techniques of optical pumping and an interferometric method for measuring the Rb vapor density. The Rb87{\mathrm{Rb}}^{87}Rb87 constituent in a vapor of natural Rb was polarized through absorption of circularly polarized resonance radiation, and the Rb87{\mathrm{Rb}}^{87}Rb87 polarization was partially transferred to the Rb85{\mathrm{Rb}}^{85}Rb85 constituent through spin-exchange collisions. A phenomenological theory of the optical pumping plus the exchange polarization process which neglects nuclear spin was used to relate the cross section to the ratio of the signal strengths for the Rb87{\mathrm{Rb}}^{87}Rb87 and Rb85{\mathrm{Rb}}^{85}Rb85 Zeeman resonances, the relaxation time, and the Rb87{\mathrm{Rb}}^{87}Rb87 vapor density. The density was measured by comparing spectral profiles of the resonance radiation transmitted through the optical pumping cell at room temperature with the resonance radiation transmitted at the temperature at which the signal strengths were measured. These spectral profiles were obtained through use of a scanning Fabry-Perot interferometer.