The polarization properties of excited alkali atoms having suffered half collisions with noble gas atoms following excitation by nonresonant photon absorption during a strong collision, are investigated. On the basis of a semiclassical perturbation treatment of the density matrix up to second order in the driving field a general expression for the polarization dependent intensity of the emitted alkali fluorescence is derived. Assuming quasistatic excitation of the collision complex and considering reorientation of the orbital and spin electronic angular momenta within a cut off radius, explicit results for the polarization degrees are presented and discussed, depending on the initial molecular excited state and coupling case.
The polarization properties of excited alkali atoms having suffered half collisions with noble gas atoms following excitation by nonresonant photon absorption during a strong collision, are investigated. On the basis of a semiclassical perturbation treatment of the density matrix up to second order in the driving field a general expression for the polarization dependent intensity of the emitted alkali fluorescence is derived. Assuming quasistatic excitation of the collision complex and considering reorientation of the orbital and spin electronic angular momenta within a cut off radius, explicit results for the polarization degrees are presented and discussed, depending on the initial molecular excited state and coupling case.
The cross sections for disorientation of 32P1/2 sodium atoms, induced in collisions with noble gas atoms, have been determined by following the depolarization of Na–D1 resonance fluorescence in relation to noble gas pressure. Sodium vapor at low density, mixed with a noble gas in a fluorescence cell, was irradiated with circularly polarized D1 resonance radiation and the resulting D1 resonance fluorescence, observed in an approximately backward direction, was analyzed with respect to circular polarization. The variation of the degree of polarization with gas pressure was interpreted on the basis of a 'J randomization' model for the collisions, and yielded the following disorientation cross sections which are appropriately corrected for effects due to nuclear spin. Na–He: 28.1 ± 4.0 Å2; Na–Ne: 27.8 ± 4.0 Å2; Na–Ar: 57.0 ± 8.0 Å2; Na–Kr: 78.0 ± 10 Å2; Na–Xe: 87.0 ± 13 Å2.
Energy transfer and coherence transfer between two atoms of different species are studied theoretically. The electric dipole-dipole interaction is the mechanism considered for the excitation transfer. A generalized perturbation method for a damping system is used. A general formula is derived for the polarization of the sensitized fluorescence resulting from the excitation transfer. This polarization is shown to be dependent on the angular momenta of the two atoms, and to be independent of their relative velocity as well as of their difference in the energy of excitation. The polarizations are found to be nonzero in many cases which demonstrate the transfer of coherence through collision processes. A general and compact formula is also derived for the polarization of pure fluorescence where excitation exchange has not taken place. The polarization of the sensitized fluorescence is in general smaller than that of the pure fluorescence. This means that the coherence is transferred only partially. Finally, the magnetic field effect has been included. This field depolarization depends on the gj values and the lifetimes of the excited states of both atoms. The general feature of the field dependence also differs considerably from that of the Hanle effect for resonance fluorescence.
The cross sections for disorientation of 42P1/2 potassium atoms, induced in collisions with noble gas atoms, have been determined in zero magnetic field by studying the depolarization of K(7699 Å) resonance fluorescence in relation to noble gas pressures. Potassium vapor at low density, mixed with a noble gas in a fluorescence vessel, was irradiated with circularly polarized 7699 Å potassium resonance radiation and the resulting resonance fluorescence, observed in an approximately backward direction, was analyzed with respect to circular polarization. The variation of the degree of polarization with gas pressure was interpreted on the basis of a 'J randomization' model for the collisions and yielded the following disorientation cross sections which are appropriately corrected for the effect of nuclear spin: K–He, 24 ± 4 Å2; K–Ne, 21 ± 3 Å2; K–Ar, 37 ± 5 Å2; K–Kr, 51 ± 7 Å2; K–Xe, 69 ± 9 Å2. The cross sections are significantly smaller than values obtained previously in kilogauss fields.
The theory of spin exchange between optically pumped alkali-metal atoms and noble-gas nuclei is presented. Spin exchange with heavy noble gases is dominated by interactions in long-lived van der Waals molecules. The main spin interactions are assumed to be the spin-rotation interactions $\ensuremath{\gamma}\stackrel{\ensuremath{\rightarrow}}{\mathrm{N}}\ifmmode\cdot\else\textperiodcentered\fi{}\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$ between the rotational angular momentum $\stackrel{\ensuremath{\rightarrow}}{\mathrm{N}}$ of the alkali-metal---noble-gas pair and the electron spin $\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$ of the alkali-metal atom, and the contact hyperfine interaction $\ensuremath{\alpha}\stackrel{\ensuremath{\rightarrow}}{\mathrm{K}}\ifmmode\cdot\else\textperiodcentered\fi{}\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$ between the nuclear spin $\stackrel{\ensuremath{\rightarrow}}{\mathrm{K}}$ of the noble-gas atom and the electron spin $\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$. Arbitrary values for K and for the nuclear spin I of the alkali-metal atom are assumed. Precise formal expressions for spin transfer coefficients are given along with convenient approximations based on a perturbation expansion in powers of ${(\frac{\ensuremath{\alpha}}{\ensuremath{\gamma}N})}^{2}$, a quantity which has been shown to be small by experiment.
Polarization phenomena in collisions between one-electron (alkali-like) atoms are calculated with density-matrix techniques. The kinetic energies for which this treatment is valid are limited from above by the use of the Born-Oppenheimer approximation, and from below by the assumed degeneracy of the hyperfine states. The basic mechanism for polarization changes is the electron-exchange effect, as suggested by Purcell and Field and by Wittke and Dicke. The special situation of unpolarized targets is treated in some detail. In this case, there are two numbers which characterize the scattering through any angle: the absolute values of certain direct and exchange scattering amplitudes, Fd and Fx. All cross sections must be expressible in terms of ∣Fd∣ and ∣Fx∣, and this is explicitly carried out in two cases of special interest. One refers to the case in which only the electron-spin polarization is measured, and the other to measurements of the polarization of the hyperfine states of the scattered atom. Effects of the identity of the atoms are also studied in detail.
The polarization of the resonance fluorescence of interacting atoms and the transfer of coherence, due to the exchange of excitation, are studied theoretically. The treatment is for the general case where both the excited and the ground states can have arbitrary angular momenta, except that they can be connected to each other by an allowed transition. Electrostatic dipole–dipole interaction and electromagnetic radiative interaction are considered simultaneously as the perturbations on the system. Heitler and Ma's generalized time-dependent perturbation method is used. The system is quantized with respect to the space-fixed z axis and a static magnetic field along the z axis may be present, so that the magnetic sublevels (m, m′, etc., for the excited state J, and α, β, etc., for the ground state J′) are not necessarily degenerate. The intensity of the scattered light of a given polarization, in a given direction, is expressed as a function of kR (where ℏck is the energy of excitation and R is the internuclear distance), and of the orientation of R with respect to z axis. The matrix elements (ℏ / 2)γmβ,αm′ and Vmβ,αm′, which cause resonant transfer of excitation between two atoms through radiative and electrostatic interaction, respectively, are also expressed as a function of kR, and of the orientation of R. For randomly oriented atoms, the polarization after being averaged over the random orientation of R becomes a function of kR. Numerical calculations have been carried out for S01 → 1P1 transition. The coherence is shown to be conserved upon resonant transfer of excitation when R is parallel to the quantization axis.