In the optical excitation of atoms with polarized light, producing excited atoms, only some of the Zeeman sublevels of the excited state are actually reached, so that large differences of population can be built up between Zeeman sublevels or between hyperfine structure (hfs) levels. This property can be used to detect radio-frequency resonance in optically excited atomic states. These resonances produce a characteristic change in intensity or in the degree of polarization of the light re-emitted. Zeeman intervals, Stark effects, and hfs intervals can be measured in this manner. (The Stark constant of the 63P1 level of Hg and the electric quadrupole moments of the alkali atoms have been obtained in this way.)The technique of “optical pumping” gives a way to concentrate atoms in some of the Zeeman sublevels of one of the hfs levels of the ground state.Atomic orientation has been obtained with the Na atom, in an atomic beam and in the vapor in equilibrium with the metal. The orientation effects have been studied by detection of radio-frequency resonance signals in the ground state. Orientation can be increased many times by adding a variable pressure of a foreign gas to the pure Na vapor. Because of the coupling between nuclear spin and electron spin, nuclear orientation is produced at the same time as atomic orientation.
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 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
2001 of the wall area, with a thin film of tetracontane (
C40H82). 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/sec and 0.24
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, 3.7\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}22}$
cm2, 5.9\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}21}$
cm2, and 1.3\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}20}$
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.
Relaxation constants
T1 and
T2 have been computed for experiments involving optical pumping and optical detection in alkali metal vapor. The calculations have been performed for several possible spin relaxation mechanisms; namely, magnetic dipole, electric quadrupole, spin exchange, and the optical pumping process itself. For all of these mechanisms a reorientation experiment will approximately predict a spin resonance line width (equivalent to the statement ${T}_{1}\ensuremath{\approx}{T}_{2}$ for spin-\textonehalf{} particles.) However, a spin reorientation experiment of the type originally performed by Dehmelt, employing circularly polarized light, gives approximate results because of the nonexponential character of the reorientation. A more suitable experiment is one employing hyperfine population differences and unpolarized light.
A new method has been designed for obtaining the hyperfine optical pumping of Na vapor. The pumping lamp is placed in a magnetic field and the light emitted in the field direction is used for excitation after crossing a circular polarizer selecting one of the Zeeman lines. This method has two interesting features: (i) The atoms can be pumped either in the lower or in the upper hyperfine sublevel by simply rotating a polarizer by an angle of $\frac{1}{2}\ensuremath{\pi}$; (ii) the hyperfine pumping is obtained using both the
D1 and
D2 resonance lines without filtering losses. The pumping efficiency is good and it has been possible to measure the spin-exchange cross section between sodium atoms by studying the hyperfine relaxation rates as a function of the sodium density. The result is ${\ensuremath{\sigma}}_{\mathrm{ex}}=(1.109\ifmmode\pm\else\textpm\fi{}0.005)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}$
cm2.
The ground electronic state of even such simple atoms as those of alkali elements has the set of sublevels. These sublevels are hyperfine (HF) components and magnetic sublevels. The collisions with particles of nonmagnetic buffer gas or even with walls (when walls have proper coating) do not mix practically the populations of ground state HF sublevels, if the orbital moment of electrons in the ground state is equal to zero. Due to this reason these sublevels may be extremely long lived. Because of this, for instance, the so-called effects of optical orientation and optical pumping are apparent in atoms of alkali metals. The radiation can pump practically all the atoms (with which there is effective interaction) to a single HF component. In a situation in which optical pumping is a minor effect, the monochromatic absorption line consists of separate lines corresponding to intra-atomic transitions. The optical pumping is not significant, for example, if the radiation intensity is so low that now pumping between HF sublevels occurs in the time it takes the atom to traverse the light beam. Under the conditions of optical pumping and when other nonlinear effects are present, the absorption line profile can undergo considerable alteration. Many theoretical and experimental investigations have been done in the laser spectroscopy of resonant transitions of atoms (atoms of alkali metals) under the conditions of optical pumping within ground state HF structure. A characteristic feature of all such investigations is the velocity-selective excitation of absorbing atoms. Also, as a rule, the value of HF splitting is not very big in comparison to Doppler broadening in these experiments. Under such conditions, the absorption spectra consists of Doppler- broadened lines with nonlinear resonances, which emerge when two fields of different frequencies or different propagation directions are employed. When only one monochromatic traveling wave is employed, optical pumping leads to formation of a single smooth absorption line occupying a position between the resonant transitions frequencies associated with HF components. As HF splitting grows, the line profile remains smooth, its width is approximately equal to the size of the HF splitting. The strength of the optical pumping from one ground state HF component to another is greater for greater HF splitting in comparison to the Doppler width. In this regard, Cs and Rb are the most typical of the alkali atoms (the HF splitting exceeds the Doppler width by a factor close to 20). This is the qualitative picture of the absorption line profile (particularly for a monochromatic radiation) under the conditions of optical pumping between the HF sublevels of the electronic ground state, this qualitative picture had formed by now.
The relaxation and generation of multipole orientations in a heavy-alkali-metal vapor in the presence of a weak static magnetic field are theoretically studied both for populations and for Zeeman coherences by taking into account the effects on the evolution of the atomic density matrix of the relaxation processes (by alkali-atom--buffer-gas, alkali-atom--alkali-atom with spin exchange and alkali-atom--cell-wall collisions) and of the optical pumping with any light polarization and spectral distribution. The dependence of the stationary-state multipole orientations on the pumping characteristic parameters is numerically analyzed. The detection process of these orientations is also studied.