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Journal of the Physical Society of Japan

Spin Relaxation of Optically Pumped Cesium Atoms in Some Aromatic Gases

Teinosuke Kanda, Takumi Minemoto

Published Oct 1, 1966• 3 citations
Publisher

Abstract

Spin relaxation times of the ground state of atomic cesium were measured by the use of optical pumping- and pulse-techniques. Relaxation times in benzene, toluene, o-, m-, p-xylene, and mesitylene are all dependent on temperature. They can be expressed as 1/ T 1 = A exp ( B / T ). From B values the binding energies between Cs atom and the aromatic molecules can be obtained: 0.082 eV (benzene), 0.103 eV (toluene), 0.154 eV (o-xylene), 0.125 eV (m-xylene), 0.171 eV (p-xylene) and, 0.162 eV (mesitylene). From A values, and by consideration of the molecular state of cesium-aromatic complex, it is inferred that the relaxation is caused by spin-orbit coupling, as was proposed by Bernheim for the case of relaxation due to collision with rare gas atoms. Comparison of three isomers of xylene revealed that the molecular electric dipole moment was ineffective for the relaxation.

DOI
10.1143/jpsj.21.1990

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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 ${\mathrm{cm}}^{2}$) 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.

Physical Review•Aug 2, 1965•33 citations
Spin relaxation times of the ground state of atomic cesium were measured by the use of optical pumping- and pulse-techniques. Relaxation times in benzene, toluene, o-, m-, p-xylene, and mesitylene are all dependent on temperature. They can be expressed as 1/ T 1 = A exp ( B / T ). From B values the binding energies between Cs atom and the aromatic molecules can be obtained: 0.082 eV (benzene), 0.103 eV (toluene), 0.154 eV (o-xylene), 0.125 eV (m-xylene), 0.171 eV (p-xylene) and, 0.162 eV (mesitylene). From A values, and by consideration of the molecular state of cesium-aromatic complex, it is inferred that the relaxation is caused by spin-orbit coupling, as was proposed by Bernheim for the case of relaxation due to collision with rare gas atoms. Comparison of three isomers of xylene revealed that the molecular electric dipole moment was ineffective for the relaxation.
Short spin relaxation times for rubidium atoms, oriented by optical pumping, have been observed in the presence of benzene, ammonia, and dimethyl ether buffer gases. The disorientation cross sections of these gases in rubidium are obtained from relaxation times measured in mixtures with molecular nitrogen. The partial pressures of the gases were low compared to the nitrogen pressures in the mixtures, and the diffusion coefficient of rubidium in the mixtures was assumed to be the same as in pure nitrogen. The disorientation cross sections at 55°C are 7±1×10—19 cm2 for benzene, 8±2×10—18 cm2 for ammonia, and 3±1×10—18 cm2 for dimethyl ether. The cross section of carbon monoxide has also been obtained from the longer rubidium spin relaxation time in this gas. These measurements, complicated by a slow reaction of carbon monoxide with liquid rubidium, yield a cross section of 1±0.5×10—22 cm2 for carbon monoxide. The cross sections of ammonia, dimethyl ether, and benzene are much larger than cross sections of other molecular buffer gases. A discussion of the relaxation processes in these gases is given. The large cross sections of polar gases with appreciable dipole moments are found to result from an interaction of the rubidium atoms with the electric field of the polar molecules during a collision. Virtual excitation to the p states of the atom by the electric field gives rise to an interaction of the spin of the valence electron with the orbital angular momentum of the p states. The direct contribution of the magnetic field of the moving polar molecule is also considered and found to be small compared to the electric interaction. The large cross section of benzene is assumed to result from a spin exchange interaction with a charge transfer complex of rubidium and benzene formed in very small amounts. If the assumed complex is responsible for the large benzene cross section, the equilibrium constant for its formation can be calculated from an estimate of the spin exchange cross section.
Cross sections for relaxation of circular and linear polarization of 62P326^{2}P_{\frac{3}{2}}62P23​​ cesium atoms, induced in collisions with ground-state He, Ne, Ar, and Xe, have been determined by Zeeman scanning techniques. A fluorescence cell containing low-pressure cesium vapor together with a buffer gas was irradiated with circularly or linearly polarized 8521-\AA{} Cs resonance radiation, producing excited and polarized Cs atoms which became depolarized in subsequent collisions with the buffer-gas atoms. The resulting depolarization of the cesium resonance fluorescence was monitored in relation to buffer-gas pressure (0-10 Torr) and to the strength of the ambient magnetic field (0-10 kG). At low fields at which the nuclear spin $\stackrel{\ensuremath{\rightarrow}}{\mathrm{I}}$ is coupled to the electronic angular momentum $\stackrel{\ensuremath{\rightarrow}}{\mathrm{J}}$, the measurements yielded depolarization cross sections Q(circ.)Q(\mathrm{circ}.)Q(circ.) and Q(lin.)Q(\mathrm{lin}.)Q(lin.), which agree within experimental error with theoretical values calculated for spin-coupled conditions. At kilogauss fields with $\stackrel{\ensuremath{\rightarrow}}{\mathrm{I}}$ and $\stackrel{\ensuremath{\rightarrow}}{\mathrm{J}}$ decoupled, the experiments produced cross sections for disorientation and disalignment, which are also in satisfactory agreement with the appropriate theoretical predictions. The results indicate that the nuclear spin has a more pronounced effect on the collisional relaxation of the atomic dipole than of the quadrupole.
NMR signals from diatomic alkali molecules have been observed in optically pumped cesium and rubidium vapors. The nuclear relaxation times were found to be strongly dependent on the temperature and buffer-gas pressure. The relaxation time seems to be determined by at least two and possibly three major factors: motional narrowing of the molecular hyperfine structure, breakup of the diatomic molecules by collisions with buffer-gas atoms, and possibly chemical exchange of free atoms with atoms bound in the molecules.
Relaxation experiments have been performed between 0–200 G on optically polarized Rb atoms in argon, krypton or xenon, at pressures ranging from 0.1 to 20 torr. They clearly show the existence of Rb–Ar, Rb–Kr and Rb–Xe molecules of low binding energy (smaller than kT). Molecular parameters such as lifetime, spin-orbit coupling constant, formation rate, constant of mass action, etc., are measured, or evaluated when they cannot be directly measured. Experimental values of the diffusion coefficient of Rb in the gas (except xenon) and of the disorientation cross sections by usual binary collisions are also obtained.
The influence of optical pumping on the transverse spin relaxation of 133 Cs atoms in different ground-state hyperfine levels is investigated. Transverse relaxation times for 133 Cs atoms in the two ground-state hyperfine levels are detected separately under different intensities and frequencies of pump light, and a statistical model is adopted to analyze the experimental results. Theory and experiment show that optical pumping changes the populations of the two ground-state hyperfine levels, thereby influencing the transverse spin relaxation due to spin-exchange collisions. As a result, an unusual phenomenon that the transverse relaxation time for 133 Cs atoms in the upper ground-state hyperfine level increases with the pump-light intensity is observed.
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.