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Journal of Physics B Atomic Molecular and Optical Physics

Laser-induced fluorescence and polarized light in the collision regime: the ) case

S. De Benedictis, Giorgio Dilecce, Vito Luigi Lepore

Published Dec 14, 1997• 1 citation
Publisher

Abstract

Laser-induced fluorescence experiments carried out using linearly polarized photons from a pulsed laser on a excitation - detection scheme in electrical discharges at 0.04 - 0.6 Torr, show that light emitted during the interaction and in the subsequent decay manifests anisotropy in its angular distribution and polarization. A rate equation approach is used to discuss the general features of the interaction between polarized light and atoms observed experimentally. The incident electromagnetic field is decomposed into multipolar components that may interact with the atom through an appropriate coupling. Defining the Einstein coefficients for each coupling, it is possible to introduce the equations for the dynamics of the atomic populations. For each direction and polarization, the temporal profile of the intensity during the transition is calculated. The theoretical prediction explains the outcome of the He experiment satisfactorily, providing that the role of the quenching and of the collision mixing within the manifold of the state is duly taken into account. Fitting of the model calculations to the experimental data then allows one to deduce the value of the `thermally averaged' cross section for collision-induced transitions between fine-structure and degenerate components of the sublevel, , for each J,M in the manifold.

DOI
10.1088/0953-4075/30/23/006

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Laser-induced fluorescence experiments carried out using linearly polarized photons from a pulsed laser on a excitation - detection scheme in electrical discharges at 0.04 - 0.6 Torr, show that light emitted during the interaction and in the subsequent decay manifests anisotropy in its angular distribution and polarization. A rate equation approach is used to discuss the general features of the interaction between polarized light and atoms observed experimentally. The incident electromagnetic field is decomposed into multipolar components that may interact with the atom through an appropriate coupling. Defining the Einstein coefficients for each coupling, it is possible to introduce the equations for the dynamics of the atomic populations. For each direction and polarization, the temporal profile of the intensity during the transition is calculated. The theoretical prediction explains the outcome of the He experiment satisfactorily, providing that the role of the quenching and of the collision mixing within the manifold of the state is duly taken into account. Fitting of the model calculations to the experimental data then allows one to deduce the value of the `thermally averaged' cross section for collision-induced transitions between fine-structure and degenerate components of the sublevel, , for each J,M in the manifold.
The fluorescent light from two atomic levels is studied assuming that the atoms are subjected to a gas discharge, to a static magnetic field, and, simultaneously, to a laser beam having the transition frequency between the atomic levels. Calculations are developed in the formalism of irreducible tensor operators. One takes into account the existence of isotropic relaxations and cascade effects due to spontaneous emission between the upper and the lower levels. Following Lamb, the laser beam is described classically by its electric field, and its effects are calculated by perturbation theory. It is predicted that the σ component of fluorescent light exhibits the Hanle effect, which allows one to measure the relaxation rates\Gamma(0)and\Gamma(2)of the population and of the alignment of the emitting level, respectively. Experimental agreement with the theoretical analysis has been found for the3s_{2}, 2s_{2}, and2P_{4}levels of Ne. Among the experimental results obtained by this method are the natural widths and the collision cross sections for population (quenching collision) and for alignment. Several transition probabilities are also derived. Furthermore, the theory of coherent imprisonment of the fluorescent line has been found valid even if laser pumping light is used.
Measurements of collisional depolarization cross sections play an important role in gaining valuable information about the interaction between inert and rare-gas atoms.A key element in understanding collisional dynamics is the detailed analysis of the polarization of the emitted photons.In order to investigate the collisional cross section of the excited J=1/2 cesium atoms, by collisions with the ground level argon atoms, experimental measurements were made studying circular polarization spectra.Orientation in the J=1/2 level was optically induced by circularly polarized light with a positive helicity.A two-photon double-resonance (6s 2 S 1/2 →6p 2 P 1/2 → 10s 2 S 1/2 ) condition was achieved using nanosecond pulsed dye lasers, and the intensity of the cascade fluorescence was monitored in the presence of argon atoms ranging from 10 -4 torr to 100 torr.
Redistribution and depolarisation of light scattered by atoms undergoing collisions outside the impact region of the line profile has been studied experimentally and theoretically. In a cell experiment intensity and linear degree of polarisation of the fluorescence components 32S1/2 to or from 32P1/2,3/2 of Na atoms induced by collisions with Ar buffer gas atoms were measured as functions of the laser frequency omega L. The decrease of polarisation of the D2 component observed when omega L is shifted away from the D2 toward D1 resonance disagrees with calculations on the basis of the factorisation approximation of the theory of redistribution. Using Baylis (1975) potentials for the Na/Ar system, the effect is interpreted in terms of adiabatic coupling of the 32P3/2 electronic angular momentum to the collision axis during 'strong' collisions, giving rise to a greater than average depolarisation.
The dependence of the circular polarization of the fluorescence of alkali atoms on the intensity and spectral composition of the σ+-polarized exciting D1 line has been investigated by considering the stationary solutions of rate equations for populations of the Zeeman sublevels. The calculations were performed for pumping-light intensities corresponding to those of classical light sources, e.g., radio frequency or microwave discharge lamps, and commonly accepted values of cross sections for collisional relaxation of ground-state and excited atoms. The systematic errors of cross sections for collisional disorientation of 2P1/2 alkali atoms due to the neglect of intensity and spectral composition of the exciting light are estimated.
Merging two subfields, collisions and spectroscopy, this book presents the latest research proposals, innovative experiments and fresh ideas. Topics considered include radiative collision induced electron continuum-continuum scattering; models of laser-induced chemical reactions; experimental studies of laser-induced ionizing collisions; laser photodissociation of Na/sub 2/ + ions produced by laser resonant ionization of Na vapor; steady-state electron-atom collision in a laser field; conditions for the observation of the predicted splitting of the laser assisted electron impact of the differential cross section of atoms; transitions between resonances; some proposals for experiments; above-threshold multiphoton ionization; observability of optical collisions in the frequency and the time domain; laser switched collisions - a diagrammatical approach; polarization of atomic fluorescence excited by molecular photodissociation; multiphoton selective excitation; on the role of chaotic dynamics with many basins of attraction; predissociation in a strong electromagnetic field; theory of double resonance; and coherent excitation of polyatomic molecules up to highly excited vibrational states by laser light.
The effects of laser-induced anisotropy on the generation of the short-pulse laser-induced polarization spectroscopy (LIPS) signal is investigated by direct numerical integration (DNI) of the time-dependent density matrix equations. The calculations are performed in the short-pulse regime (laser pulse width τL less than characteristic collision time τC) to reduce the influence of collisions on the generation of medium anisotropies. The Zeeman-state structure of the upper and lower energy levels is included in the multistate formulation of the density matrix equations. For a P-branch transition when the isotropic ground-level population is pumped by a circularly polarized light, oriented anisotropy is mainly responsible for the LIPS signal generation; whereas, when the resonance is pumped by a linearly polarized light, aligned anisotropy is mainly responsible. For a Q-branch transition that is pumped by a circularly polarized light, the contributions to the LIPS signal from orientation and alignment are comparable. The effects of saturation on the induced anisotropy is also investigated. The magnitude of the LIPS signal increases by more than a factor of 14 for an initial right circularly polarized-oriented anisotropic distribution in the ground Zeeman states as opposed to an isotropic distribution. An understanding of the effects of anisotropy on the LIPS signal will aid the modeling of the LIPS signal-generation processes and the interpretation of experimental LIPS signals.