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Journal of Physics B Atomic and Molecular Physics

Magnetic resonance in sensitized fluorescence due to collisional transfer of orientation and alignment

E L Lewis, C S Wheeler

Published Mar 11, 1976• 2 citations
Publisher

Abstract

The resonance functions observed in sensitized fluorescence are derived for the magnetic resonance of an oriented or aligned atomic system. The functions are seen to be modified forms of those observed in direct fluorescence, but with an apparent anisotropy in the relaxation processes, even in an isotropic environment.
DOI
10.1088/0022-3700/9/4/008

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Theoretical study is made of the transfer between orientation and alignment of excited-state atoms by anisotropic collisions with ground-state atoms. The anisotropy considered is due to the anisotropic velocity distribution of atoms excited by a single-mode laser beam. The transfer rate and relaxation rates for each multipole moment are calculated for the excited state with J=1J=1J=1 as a function of detuning of the laser frequency from the center of an absorption line and mass of perturbing ground-state atoms. Experiments to observe the transfer from alignment to orientation and from orientation to alignment in a weak magnetic field are considered, and corresponding signals are analyzed in terms of the transfer and relaxation rates.
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{g}_{j}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 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.
Following (i) a sharp step or (ii) a pulse of applied magnetic field, the resonance fluorescence of an atomic vapour exposed to steady linearly polarized resonance radiation undergoes transient behaviour until a new steady state is reached; the form of the transient will be (i) modulation of the intensity with an exponential envelope, or (ii) simple exponential decay. From the modulation period the gJ value of the excited state is obtained. From the exponential decay the lifetime for the relaxation of atomic alignment is obtained directly. The technique, applied to the 63P1 state of mercury, gives 117.4+or-1.0 ns for the natural mean life.