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Soviet Journal of Quantum Electronics

Optical processes in close atomic collisions

A. M. Bonch-Bruevich, Sergey G. Przhibel'skii, V. V. Khromov

Published Feb 28, 1978• 1 citation
Publisher

Abstract

An analysis is made of the general aspects of the physics of processes occurring in a system of colliding atoms in the presence of a radiation field. The attention is concentrated on the relationship between the spectral characteristics and various photon absorption (emission) processes in a system of interacting atoms (regarded as a quasimolecule). Nonlinear optical effects in the far wings of atomic lines are considered and the effects are interpreted. A relationship between these effects and the change in the atomic collision dynamics due to the presence of a radiation field is considered.

DOI
10.1070/qe1978v008n02abeh008544

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An analysis is made of the general aspects of the physics of processes occurring in a system of colliding atoms in the presence of a radiation field. The attention is concentrated on the relationship between the spectral characteristics and various photon absorption (emission) processes in a system of interacting atoms (regarded as a quasimolecule). Nonlinear optical effects in the far wings of atomic lines are considered and the effects are interpreted. A relationship between these effects and the change in the atomic collision dynamics due to the presence of a radiation field is considered.
A theory is given of radiative collisions, i.e., of elementary events in which the emission of a photon occurs in the course of a collision. Special attention is paid to radiative collisions stimulated by a laser field. Simple but clear approaches formulated in the forties or fifties are described briefly. This theory applies, in particular, to collisions in a strong electromagnetic field which affect the collision dynamics. Chemical radiative collisions, i.e., chemical reactions stimulated by photons absorbed in the course of a collision, are reviewed. An analysis is made of several recent experiments in which the theoretically predicted effects were observed: these include the radiative-collisional transfer of excitation from atom to atom, nonlinear effects due to the influence of the field on the collision dynamics, and photosubstitution of one of the atoms in a halogen molecule with an inert gas atom.
A study is made of the influence of photon absorption (emission) processes on the dynamics of collisions between two atoms. Under certain conditions the radiation field can transfer colliding atoms to a bound molecular state. The main contribution to these processes is made by atoms colliding with relative velocities and impact parameters which ensure that these atoms spend a long time near each other (quasifinite motion). The appearance of quasifinite states in the absorption spectra of Rb and Cs vapors is reported and a determination is described of the matrix elements of the transitions from these states to a bound molecular state.
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 close coupled theory of scattering in a radiation field may be used to describe absorption or emission processes occurring during a collision. Using a semi-classical description of the collision we study the evolution of the collisional complex. The case of atomic hydrogen perturbed by protons is particularly interesting since the exact solution of the dynamical problem is known for a large domain of internuclear distances. In the particular case of the Ly α line we determine the characteristic time of the absorption or the emission. The « impact » and « quasistatic » limits are then analysed.
An attempt is made to present a consistent detailed theory of optical phenomena, based on the suggestion recently made by the author in collaboration with Bohr and Kramers. This suggestion is that atoms are radiating or absorbing continuously, during their stationary states, and that transitions influence radiation only in terminating the radiation characteristic of the old state, and substituting that of the new. The atoms, on the other hand, are supposed not to change their energy while radiating, but to change it discontinuously on transition. This necessitates giving up the detailed application of the conservation of energy in interaction between atoms and radiation. In the present paper, an additional suggestion is made, namely that resonance radiation is to be identified with the radiation carried out by the spherical wavelets which, by their interference with the external field, also produce absorption. This is practically a return to the classical picture of resonance radiation. Statement of the theory consists formally of two parts: the description of the behavior of atoms, and of radiation, when the two interact. The first involves the statement of the probabilities of transition of atoms, and is taken without change from Einstein. The probability of interruption of coherent vibrations is also discussed. The second requires the specification of the fields emitted by atoms in any steady state under the influence of any external field. These consist of spherical wavelets of the frequencies of the various quantum lines which the atom can emit or absorb in the stationary state in which it is. For emission frequencies, wavelets are emitted even in the absence of an external field; for absorption frequencies, external fields induce wavelets, similar to the wavelets of linearly bound electrons in electron theory, which on the one hand interfere with the external field to produce the phenomena of dispersion, etc., and on the other carry out the resonance radiation in all directions. Detailed descriptions of these fields are given. In a discussion of the theory, it is first shown that the assumptions which have been made about the field satisfy the correspondence principle, in that for large quantum numbers the field aproaches that which would be emitted classically on account of the interaction of an external field and a multiply periodic atom. On the other hand, it is shown that the field has a character essentially like that of classical electron theory, which is known to be in general agreement with experiments. Next, the energy and momentum relations at interaction of atoms and light are investigated, and it is shown that, although these quantities are not precisely conserved, still the assumptions as to atomic and radiation processes have been so made that they are conserved on an average over a great number of atomic processes. Finally the spectral resolution of emitted and absorbed radiation is considered; the theory gives a minimum breadth for the lines, depending on the finite length of wave trains resulting from the finite life in stationary states, and it is shown that Kirchhoff's law is obeyed, the emission and absorption lines being of the same breadth. By way of illustration, specific application of the theory is made to the simple examples of emission of light by bombardment of electrons at the resonance potential, resonance radiation, its quenching by presence of foreign gases, absorption, scattering, and disperison.
Abstract : Work is summarized in areas of: Laser Assisted Collisions; Velocity Changing collisions in Atomic Vapors; Coherent Transients; Collision Induced Extra Resonances; Breakdown of the Optical Bloch Equations; Saturation Spectroscopy; Dynamics of Two-and Three-level Atoms Interacting with Radiation Fields; Pulse Propagation. Keywords: Laser spectroscopy, Optical collisions, Radiative collisions, Two-level atom, Atomic coherence, Degenerate four-wave mixing, Saturation spectroscopy, Laser propagation,, Dressed atom, Photon echo, Bloch equations, Collision kernal, Collisions, Optical noise.