Relaxation time constants of electron polarization, 〈Sz〉, for optically pumped rubidium atoms in a drifilm coated glass cell have been investigated with the Faraday rotation method. The dependence of the 〈Sz〉 relaxation time on pump cell temperature, rubidium density and applied magnetic field has been determined with high precision. The measurements allow the determination of the local magnetic field on the surface, alkali-wall binding energy and wall-dwell time. Furthermore, the change of relaxation time caused by admixtures of molecular hydrogen, nitrogen and oxygen has been investigated. No influence due to the addition of hydrogen could be detected up to a density of 3.3×1014 cm−3 at typical rubidium densities of several 1011 cm−3. The cross section for depolarizing collisons with molecular oxygen has been determined to be 7.50×10−15 cm2. The corresponding cross section for nitrogen was found to be two orders of magnitude lower. The experimental results are discussed in respect to the performance of spin exchange sources for nuclear polarized hydrogen and deuterium.
We have produced highly spin-polarized atomic hydrogen by spin-exchange optical pumping. A tunable ring dye laser is used to polarize rubidium atoms by optical pumping. The cell containing the rubidium vapor is coated with paraffin in order to reduce spin relaxation due to wall collisions. Hydrogen gas is dissociated in an inductive discharge and flows continuously through the cell, in which the hydrogen atoms are polarized by spin-exchange collisions with the polarized rubidium atoms. Atomic-hydrogen polarization as high as 2〈
Jz〉H=0.72(6) has been observed, which is the highest polarization yet produced by this method. However, the rubidium polarization may be limited to this value due to radiation trapping at higher rubidium densities. The spin-relaxation rate of atomic hydrogen on a paraffin-coated cell is also measured and corresponds to about 7600 wall bounces between wall 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.
I studied the effect of wall collisions on the electron paramagnetic resonance (EPR) of gas phase alkali metal atoms (87Rb). Two types of walls were studied: antirelaxation-coated walls and RbH-coated walls. I measured the dwell times of spin polarized Rb atoms on the two most common antirelaxation coatings, octadecyltrichlorosilane (OTS)- and paraffin. I found that at a cell temperature of 72 C the dwell times for OTS- and paraffin-coated walls are 0.9 ± 0.1 μs and 1.8 ± 0.2 μs, respectively. The implication of these dwell times, which are much longer than what was previously reported in the literature, is discussed in connection with the relaxing property of these coatings. In cells coated with RbH salt I made the first observation of the EPR frequency shift of the gas phase 87Rb atoms. Due to collisions with the RbH salt, which was nuclear spin polarized by spin exchange with optically pumped Rb vapor. The measured EPR frequency shifts are of the order of several hundred Hz in a millimeter-sized cell. By measuring the dependence of the EPR frequency shifts on cell length and by comparing the EPR frequency shifts in RbH-coated cells with those in OTS-coated cells, I provided convincing evidence that the observed EPR frequency shifts are due to collisions with RbH-coated walls, and not due to gas phase processes. The EPR frequency shift is due to the Fermi contact interaction between the s-electron of the adsorbed 87Rb atom and the polarized nucleus on the salt surface. The measured EPR frequency shifts allowed me to calculate the ensemble-averaged phase shift experienced by the Rb atom while adsorbed on the walls. Under our experimental condition this is about 70 mrad. My experiment opens up the possibility of studying surface NMR using gas phase EPR. The phase shift is proportional to the surface nuclear polarization, thus provides an interesting method for measuring the surface nuclear polarization using gas phase EPR. My observation will alert the high precision miniature atomic magnetometry community that collisions with cell walls may cause a systematic error and line broadening in the magnetic resonance frequency.
The interaction of spin polarized cesium atoms on coated surfaces is examined. Coated surfaces find extensive applications in atomic devices-hydrogen masers and advanced rubidium frequency standards utilize wall coatings to obtain very narrow hyperfine resonances. A Cs atomic beam is hyperfine or spin polarized by optical pumping techniques using a single mode AlGaAs diode laser. The ground state distribution is probed before and after scattering from coated surfaces using laser induced fluorescence spectroscopy. The coatings under investigations are paraffin and organosilanes and these are known to be very weakly relaxing surfaces for polarized alkali atoms. The spin relaxation properties of paraffin and organosilane coatings have been studied in glass cell-vapor environment. In our experiments using polarized atomic beams, our goal is to examine in detail the hyperfine and spin relaxation properties of these coatings in a carefully controlled environment which is not possible in the gas cell environment. We measure the spin relaxation probability per wall collision as a function of temperature of the surface. Results of our studies will be presented.
Relaxation of optically pumped Rb atoms on paraffin-coated walls has been studied using Franzen's sequence (relaxation in the dark) for observables
〈Sz〉 (mean electronic longitudinal polarization), and <S\ifmmode\cdot\else\textperiodcentered\fi{}I> (population difference between the two hfs levels). The physical meaning of optical signals under different conditions is analyzed in some detail, and it is pointed out that different observables relax differently. In the interpretation of our results, extensive use has been made of the theoretical analysis of the relaxation of a spin S (coupled to a spin I in the Rb atom) caused by a weak interaction of the type $_{\ensuremath{\gamma}s}H(t)\ifmmode\cdot\else\textperiodcentered\fi{}\mathbf{S}$,
H(t) being a random magnetic field acting on S during the dwell time of a Rb atom on the wall. Experimental results are in excellent agreement with this analysis, if one assumes the existence of two uncorrelated interactions of the above type. The first is the dipole-dipole interaction between S and the nuclear spins K of the protons (or deuterons) of the coating. This interaction has a long correlation time ${\ensuremath{\tau}}_{c1}\ensuremath{\approx}4\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}10}$ sec and dominates the relaxation of
〈Sz〉 in low fields. The second interaction which is independent of spins K, has a short correlation time ${\ensuremath{\tau}}_{c2}\ensuremath{\approx}{10}^{\ensuremath{-}12}$ sec, and dominates the relaxation of <S\ifmmode\cdot\else\textperiodcentered\fi{}I> in low fields, and of
〈Sz〉 in large fields. The values of these correlation times and of the strengths of the two interactions have been measured, first in low fields by combining results on
〈Sz〉 and <S\ifmmode\cdot\else\textperiodcentered\fi{}I> for the two Rb isotopes and for two types of coatings [
(CH2)n and
(CD2)n], and second, by studying the variations of the "pseudo" relaxation time
T1 of
〈Sz〉 for magnetic-field values up to 5000 G. We arrive at a detailed picture of physical adsorption of Rb on paraffin-coated walls, and find 0.1 eV for the adsorption energy. These results are compatible with those obtained for the relaxation of oriented Rb atoms in collisions with buffer-gas molecules.
A theory is derived to predict the density matrices describing two atoms after a spin-exchange collision from the density matrices before the collision and the scattering amplitude for binary collisions. This theory is then applied to a system of quasifree electrons interacting with optically pumped rubidium atoms. For calculating the change in the electron density matrix, the
Rb85 and
Rb87 are replaced by a fictitious rubidium isotope with no nuclear spin. Expressions are derived for the change in the light transmission when a radiofrequency field is present at the electron frequency. In addition to the linewidth for the electron signal, the spin-exchange theory predicts a frequency shift the magnitude of which depends upon the two-body scattering amplitude, the rubidium polarization and the rubidium density. Experiments performed to test various aspects of the theory are then reported. The measurements were made on a system of quasifree electrons interacting with rubidium atoms. Measurements of the electron linewidth as a function of temperature indicated that spin-exchange collisions dominated the electron relaxation. The predicted frequency shift was measured by observing the electron resonance frequency first with left circularly polarized light and then with right circularly polarized light. For electrons colliding with rubidium atoms the shift is negative when the rubidium polarization is positive and the ratio of the shift to the linewidth is $\frac{\ensuremath{\delta}{\ensuremath{\nu}}_{0}}{\ensuremath{\Delta}\ensuremath{\nu}}=\ensuremath{-}0.025\ifmmode\pm\else\textpm\fi{}0.005$. From the measured values of the shift and the linewidth, a value is derived for the electron-rubidium spin-flip cross section. In one Appendix the replacement of the
Rb85 and
Rb87 by the fictitious rubidium isotope with no nuclear spin is justified. In a second Appendix the calculations for the simple electron-rubidium system are generalized and applied to more complicated systems. Results are reported for the change in the density matrix of hydrogen atoms when they collide with polarized electrons, the change in the density matrix of
Rb87 atoms when they collide with polarized electrons, and the change in the density matrix of hydrogen atoms when they collide with hydrogen atoms.