Depolarization of Resonance Fluorescence from Interacting Atoms
Lue‐Yung Chow Chiu
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.
The Journal of Chemical Physics•Jan 1, 1970•4 citations