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Optics and Spectroscopy

Radiative quenching and excitation of metastable states upon differential scattering of atoms: I. Uniform quasi-classical theory

Alexander Z. Devdariani, E. A. Chesnokov

Published Dec 1, 2005• 2 citations
Publisher

Abstract

A theory of radiative-collisional transitions between the ground and metastable 1 S states of a colliding atom is proposed. The theory uses the uniform quasi-classical approximation generalized to the case of spherically asymmetric interactions. The theory takes into account the angular momentum of an emitted (absorbed) photon and allows one to calculate the total and differential scattering cross sections in a wide range of radiation frequencies including both wings and the center of the line of a forbidden atomic transition. The range of admissible collision energies and intensities of an external radiation field is restricted by the use of the adiabatic approximation, as well as the approximation of a weak coupling between the ground and excited states of a quasi-molecule, the potentials of which are assumed to be monotonically repulsive.

DOI
10.1134/1.2149408

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A theory of radiative-collisional transitions between the ground and metastable 1 S states of a colliding atom is proposed. The theory uses the uniform quasi-classical approximation generalized to the case of spherically asymmetric interactions. The theory takes into account the angular momentum of an emitted (absorbed) photon and allows one to calculate the total and differential scattering cross sections in a wide range of radiation frequencies including both wings and the center of the line of a forbidden atomic transition. The range of admissible collision energies and intensities of an external radiation field is restricted by the use of the adiabatic approximation, as well as the approximation of a weak coupling between the ground and excited states of a quasi-molecule, the potentials of which are assumed to be monotonically repulsive.
We calculate the total and differential cross sections for radiative-collisional excitation of the metastable 2 1 S state of He atoms at collisions with Ne atoms in external radiation fields of various frequencies and polarizations. The calculations are performed for a thermal collision energy of E = 10 −3 atomic units and light intensity of I = 1 MW cm −2 , which corresponds to a single photon absorption by a quasi-molecule during the collision. Both the differential and total cross sections are shown to depend strongly on the relative orientation of the radiation polarization vector and the initial relative velocity vector of the colliding atoms. We analyze the azimuthal scattering asymmetry related to the orientation of the angular momentum of the absorbed photon.
The scattering of radiation in the presence of collisions can be described quantum-mechanically in terms of essentially two processes. The first may be thought of as an absorption to the excited state followed subsequently (after propagating in the excited state) by emission. This gives rise to radiation redistributed about the transition frequency. The effects of m-degeneracy are particularly interesting for this first process. As an example a case is considered in which the incident frequency is in the quasi-static line wing, while the scattered frequency is close to the line center. It is found that under these circumstances the dominant contribution from this process in the scattered spectrum is obtained for an absorption of the incident frequency taking place during a strong (close) collision and reemission of the scattered frequency when the atom is essentially unperturbed
The collision-induced absorption and emission coefficients for electric-dipole forbidden atomic transitions are calculated for weak radiation fields. The approximations used are valid for $\ensuremath{\hbar}\ensuremath{\omega}$ near $\ensuremath{\hbar}{\ensuremath{\omega}}_{0}$, the atomic energy differences. The example case of $S\ensuremath{-}D$ transitions induced by a spherically symmetric perturber (e.g., a noble-gas atom) is treated in detail and compared to measurements. The case of "radiative collisions," in which both colliding atoms change their state, is included in the theory and is also compared to experiment.
The molecular expansion method within the framework of the semiclassical approximation is applied to quenching of low-lying excited states of Rydberg atoms colliding with ground-state He at thermal energies. Interactions between the colliding atoms are accounted for in terms of pseudopotentials, and their relative motion is described by a classical linear trajectory. A fairly large basis set of Slater-type orbitals is used to obtain molecular eigenstates, and subsequently a 14-state close-coupling calculation is performed to evaluate the total quenching cross sections and the contributions of individual transitions. The energy dependence of the calculated cross sections is investigated, and possible mechanisms responsible for individual transitions are explained. Finally, the collision rates are calculated and compared with experimental results.
The close-coupled theory of atomic collisions in the presence of a radiation field may be used to calculate the distribution of final atomic states which results from absorption of polarized light during a collision. The theory applies equally well to optical collisions (line broadening) and to radiative collisions (laser-induced collisional energy transfer). For an optical collision the detuning $\ensuremath{\omega}\ensuremath{-}{\ensuremath{\omega}}_{\ensuremath{\infty}}$ is restricted to be larger than either the Rabi frequency or the widths due to natural, Doppler, or pressure broadening. The radiation field is assumed to be weak enough that the transition probabilities are linear in field intensity. The molecular picture is emphasized in which the wave function is expanded in a basis of field-free molecular states and the Hamiltonian is blocked in accordance with molecular quantum numbers. The quantities needed to predict experimental observables are reduced radiative scattering SSS-matrix elements ${s}_{\ensuremath{\omega}}$ in the asymptotic Hund's case-(e) representation. The theory of product orientation and alignment is equivalent to that which has been developed for molecular photodissociation. It requires coherent sums of ${s}_{\ensuremath{\omega}}$ matrix elements from different transition branches, that is, for PPP-, QQQ-, and RRR-type transitions corresponding to changes of -1, 0, and +1 in total molecular angular momentum. On the other hand, the total absorption coefficient and the branching ratio to different final fine-structure states irrespective of orientation or alignment depend on incoherent sums of the same matrix elements.
A theory of inelastic n,l-changing and quasielastic l-mixing collisions of Rydberg atoms with the heavy rare-gas atoms is developed. It is based on the semiclassical impact-parameter approach combined with the normalized perturbation theory. Semiclassical formulas for scaled transition probabilities and cross sections as functions of the inelasticity parameter and the collision strength are analyzed. This approach gives a general description of collisional nl\ensuremath{\rightarrow}${\mathit{n}}^{\ensuremath{'}}$ transitions independently of the specific values of the principal quantum number, the relative velocity, and the type of colliding atoms. The energy and angular dependence of the electron-atom scattering amplitude is included in the theory by incorporating the impulse-approximation results in the weak-coupling limit. The Ramsauer-Townsend effect affects significantly the values of the cross sections, especially for the inelastic transitions with large energy transfer. The results obtained are used in calculations of the quenching cross sections for the Rb(nS,nD,nF) atoms in collisions with Ar, Kr, and Xe. Comparison of theory and experiment is made in a wide range of the principal quantum numbers and transition energy defects. \textcopyright{} 1996 The American Physical Society.