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Reviews of Modern Physics

Impact Excitation and Polarization of the Emitted Light

U. Fano, J. H. Macek

Published Oct 1, 1973• 949 citations
Publisher

Abstract

A new formulation is presented for the angular distribution and the polarization of light excited by atomic and electronic collisions and modulated in time by the action of internal and external fields. The formulation disentangles geometrical and dynamical effects and stresses the extraction of data on the alignment and orientation of radiating atoms from observations of the emitted light. The treatment is set in the context of recent experimental and theoretical literature and points to new avenues of research.

DOI
10.1103/revmodphys.45.553

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On the excitation of polarised light by electron impact. II.—Mercury

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Abstract In a number of recent papers descriptions have been given of how the light from atoms excited by a directed stream of electrons is polarised, in the absence of any external field of force. In particular we may refer to the paper by one of the present writers (Paper I), where some of the characteristics of the effect in mercury were discussed. It was found that the different lines of the spectrum were differently polarised, both in magnitude and direction. The behaviour of the polarisation when a magnetic field is applied to the mercury atoms was found to be identical with the effect produced by a similar field on the polarisa­tion when the light is excited by the absorption of plane polarised light, the electric vector of which is parallel to the direction of the stream of electrons. In this way, the polarisation of the light excited by electron impact was shown to be closely related to the polarisation of resonance radiation, which had been investigated by Wood and Ellett and others. In the paper referred to, the measurement of the polarisation of the spectral lines was, except in an individual instance, only qualitative. Since its appearance two papers have appeared in which polarisation measurements of the mercury lines excited by electron impact have appeared. Eldridge and Olsen gave qualitative results, and these confirmed those which we had given. Quarder gives quantitative measure­ments which are also for the most part in general accord. The aim of the present paper is to describe quantitative results, and, as will be seen, these are not in all cases in detailed agreement with those given by Quarder. The second aim is to determine the variation of the polarisation with the velocity of the electron stream, a point which has not been previously attempted. In Paper I it was shown that the magnitude of the polarisation is intimately connected with the dynamics of the collision process. By the electron impact, the atom is raised from its normal state into an upper quantum state, and by its return into the normal state, or into another state, light is emitted. The magnitude of the polarisation depends on both of these processes, but the second process, the actual emission of the light, is well understood. Polarisation measurements therefore give a powerful means of investigating the collision of an electron with an atom in the case when excitation of the atom takes place, and it is in this that their main interest lies.

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A new formulation is presented for the angular distribution and the polarization of light excited by atomic and electronic collisions and modulated in time by the action of internal and external fields. The formulation disentangles geometrical and dynamical effects and stresses the extraction of data on the alignment and orientation of radiating atoms from observations of the emitted light. The treatment is set in the context of recent experimental and theoretical literature and points to new avenues of research.
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.
A compact expression for the cross section of scattering of an arbitrarily polarized light by aligned atomic systems is obtained, in which the dependence on the geometric parameters and the Stokes parameters specifying the state of partial polarization of the incident radiation is represented in explicit form. The effect of atomic alignment and the processes of dissipation of the light energy on the polarization specific features and the angular distribution of the scattered light is investigated. In particular, it is shown that, if a dissipative channel is accessible, the angular distribution and the degree of linear polarization of scattered light depend on the degree of circular polarization of the incident radiation η 2 . Dissipative processes also induce the circular polarization of the light scattered by aligned atoms when η 2 =0.
Abstract In a number of recent papers descriptions have been given of how the light from atoms excited by a directed stream of electrons is polarised, in the absence of any external field of force. In particular we may refer to the paper by one of the present writers (Paper I), where some of the characteristics of the effect in mercury were discussed. It was found that the different lines of the spectrum were differently polarised, both in magnitude and direction. The behaviour of the polarisation when a magnetic field is applied to the mercury atoms was found to be identical with the effect produced by a similar field on the polarisa­tion when the light is excited by the absorption of plane polarised light, the electric vector of which is parallel to the direction of the stream of electrons. In this way, the polarisation of the light excited by electron impact was shown to be closely related to the polarisation of resonance radiation, which had been investigated by Wood and Ellett and others. In the paper referred to, the measurement of the polarisation of the spectral lines was, except in an individual instance, only qualitative. Since its appearance two papers have appeared in which polarisation measurements of the mercury lines excited by electron impact have appeared. Eldridge and Olsen gave qualitative results, and these confirmed those which we had given. Quarder gives quantitative measure­ments which are also for the most part in general accord. The aim of the present paper is to describe quantitative results, and, as will be seen, these are not in all cases in detailed agreement with those given by Quarder. The second aim is to determine the variation of the polarisation with the velocity of the electron stream, a point which has not been previously attempted. In Paper I it was shown that the magnitude of the polarisation is intimately connected with the dynamics of the collision process. By the electron impact, the atom is raised from its normal state into an upper quantum state, and by its return into the normal state, or into another state, light is emitted. The magnitude of the polarisation depends on both of these processes, but the second process, the actual emission of the light, is well understood. Polarisation measurements therefore give a powerful means of investigating the collision of an electron with an atom in the case when excitation of the atom takes place, and it is in this that their main interest lies.
Abstract The dipole radiation emitted by an atom excited by a unidirectional electron beam has a nonuniform angular distribution which is simply related to the percentage polarization P of the radiation emitted perpendicular to the beam. P was first calculated using the OppenheimerPenney (O.-P.) theory. In this theory the probability of excitation of an upper quantum state and the probability of subsequent emission of a polarized photon from such a state are considered independently. P is finally expressed in terms of the cross-sections QM for excitation of states of definite component of angular momentum along the direction of the electron beam. In general, P is dependent on detailed numerical calculations of QM j, but the selection rule A = 0 removes this dependence at threshold. In the O.-P. theory allowance may be made for fine structure and hyperfine structure, but the theory is ambiguous when the f.s. or h.f.s. separations are comparable with the line width. A theory is therefore developed which is based on the calculation of the probability of a polarized photon being emitted by the complete system of atom + electron. The ambiguity of the O.-P. theory is removed by integration over line profiles, but the expressions reduce to O.-P. expressions when the f.s. or h.f.s. separations are much smaller or much larger than the line width. The Lyot line of hydrogen is an intermediate case for which the line widths and the h.f.s. separations are comparable. Assuming the validity of the Born approximation, a simple expression is obtained which allows the QM to be calculated from the angular distribution of the scattered electrons. Theoretical predictions are compared with experimental results. For the Na£) lines the predicted polarization is small enough to escape experimental detection. Polarizations observed by - Skinner & Appleyard in 1927 for various Hg lines rise to maxima with decreasing electron energy, and then tend to values close to zero at threshold. These experimental results at low energies appear to be inexplicable in terms of the reactions considered, but if the polarization curve above the maximum is extrapolated to threshold, the theory and experiment are found to be in reasonable agreement. Further experimental work is thought to be desirable
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.
A density-matrix approach has been developed for the angular distribution and polarization of radiative emission during single-photon atomic transitions for a general set of steady-state excitation processes in an arbitrary arrangement of static (or quasistatic) electric and magnetic fields. Particular attention has been directed at spectroscopic observations in the intense fields of the high-power ion diodes on the Particle Beam Fusion Accelerator II (PBFA II) and SABRE devices at Sandia National Laboratories and at magnetic-field measurements in tokamak plasmas. The field-dependent atomic eigenstates are represented as expansions in a complete basis set of field-free bound and continuum eigenstates. Particular emphasis has been given to directed-electron collisional excitations, which may be produced by an anisotropic incident-electron velocity distribution. We have allowed for the possibility of the coherent excitation of the nearly degenerate field-dependent atomic substates, which can give rise to a complex spectral pattern of overlapping Stark-Zeeman components. Coherent excitations may be produced by a beam of electrons that are spin-polarized at an angle with respect to the propagation direction or by nonparallel electric and magnetic fields. Our main result is a general expression for the matrix elements of the photon-polarization density operator representing the total intensity, angular distribution, and polarization of the atomic radiative emission. For the observation of radiative emission in the direction of the magnetic field, the detection of linearly polarized emission, in addition to the usual circularly polarized radiation, can reveal the presence of a perpendicular electric field or a coherent excitation mechanism.