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International Conference on Spectral Line Shapes (ICSLS)

Coherent transients as an effective technique to distinguish different collisional relaxational channels.

Н. Н. Рубцова, L. S. Vasilenko, Хворостов Евгений Борисович

Published Jan 1, 1999• 0 citations
Publisher

Abstract

Precise knowledge of collisional relaxation channels is in close relation with the research of both specific features of interaction potential and details of lineshape. When using nonlinear laser technique of spectral domain, it’s not so easy to distinguish between different channels of relaxation because of their integral contribution to the lineshape of rarefied gas. This report intends to demonstrate ability of coherent transient phenomena to overcome this difficulty. Comparative study of several photon echo modifications, performed in molecular gas SF6 has permitted to choose definite type of coherent transient phenomena, which is the most sensitive to peculiar channel of collisional relaxation. The data on relaxation rates of rotationally inelastic, elastic small angle scattering and depolarizing collisions in SF6 and its mixtures with buffer gases are examined.

DOI
10.1063/1.58321

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Precise knowledge of collisional relaxation channels is in close relation with the research of both specific features of interaction potential and details of lineshape. When using nonlinear laser technique of spectral domain, it’s not so easy to distinguish between different channels of relaxation because of their integral contribution to the lineshape of rarefied gas. This report intends to demonstrate ability of coherent transient phenomena to overcome this difficulty. Comparative study of several photon echo modifications, performed in molecular gas SF6 has permitted to choose definite type of coherent transient phenomena, which is the most sensitive to peculiar channel of collisional relaxation. The data on relaxation rates of rotationally inelastic, elastic small angle scattering and depolarizing collisions in SF6 and its mixtures with buffer gases are examined.
Collisional relaxation in SF6 gas and its mixtures with He and Xe is studied by photon echo and stimulated photon echo methods from the standpoint of the possibility of identifying the contributions of different types of collisions. The nonexponential nature of the kinetic curve of the photon echo is clearly observed for pure SF6, it is weaker in the mixture SF6+Xe, and it is virtually completely absent for high degrees of dilution of SF6 with helium. These features can be explained on the basis of estimates, made from experimental data, of the critical delay between the exciting pulses (for which the nonexponential behavior should be most strongly manifested). In pure SF6 it is possible to distinguish the contribution of the inelastic channel (rotational relaxation) and the contribution of weak collisions. To distinguish successfully the relaxation channels in mixtures with buffer gases a heavier buffer gas and a much better time resolution must be used. It is shown that data obtained on the orientation and alignment relaxation rates by the stimulated photon echo method can serve as an upper limit for the rates of inelastic processes which cannot be measured by the photon echo method. The combined use of photon echo and stimulated photon echo methods made it possible to obtain data on the cross sections for elastic and inelastic scattering of the collisional pairs SF6–SF6, SF6–Xe, and SF6–He.
A great variety of coherent transient processes in atomic and molecular gases is investigated. The degeneracy with respect to magnetic sublevels, which is typical of working levels of atomic and molecular transitions in gases, leads to new phenomena. In particular, the non-Faraday rotation of the coherent-response polarization vector at the 0 ↔ 1 transition is investigated in the presence of the longitudinal magnetic field in the 174 Yb vapor for both photon echo and stimulated photon echo. A specific relaxation channel that involves the depolarizing collisions emerges in a gas due to the degeneracy of working levels. Such collisions are especially important for atoms and are also observed in molecules. The anisotropy of the depolarizing collisions leads to a new phenomenon of the collision photon echo, which is experimentally demonstrated for the 0 ↔ 1 transition in the 174 Yb mixtures with atomic buffers. The velocity-dependent relaxation rates are observed for various coherent phenomena in molecular gases. The coherent control of a few coherent transient processes is implemented.
The method of a stimulated photon echo with specially selected linear polarizations of pumping pulses of a coherent resonant radiation is applied to a research of depolarizing collisions in molecular gas SF6 and its mixtures with buffer gases He and Xe. For the first time in one experiment the rates of a collisional decay of three lowest moments of polarization (population, orientation and alignment) are defined in an ensemble of gas particles. These rates of a relaxation are measured as functions on longitudinal velocities of resonant particles. In the frames of an experimental accuracy any noticeable dependence on velocities of particles was not detected both for orientation and alignment neither in pure resonant gas SF6 nor in mixtures. This result confirms the standard theoretical approach to depolarizing collisions. In pure SF6 decay rates of orientation and alignment have proved lesser than relaxation rate constant due to velocity changing (elastic) collisions. It means, that only the part of elastic collisions participates in destruction of multipole polarization moments of resonant levels. In comparison with our previous work the evidence is obtained that the relaxation of multipole moments seems to be j-dependent one in a medium of molecular gas SF6.
Method of stimulated photon echo with specially chosen linear polarizations of exciting pulses of coherent resonant radiation is applied for investigation of collisional decay of orientation and alignment in molecular gas SF6 and its mixtures with buffers He and Xe. These relaxation rates are measured as a function of longitudinal velocities. Within experiment accuracy, no remarkable velocity dependence of depolarizing collisions rates was detected. This result confirms conventional approach of depolarizing collisions theoretical treatment.
The method of stimulated photon echo with specially chosen linear polarizations of the pumping pulses of coherent resonant radiation is applied for the investigation of collisional decay of orientation and alignment in the molecular gas SF6 and its mixtures with buffers He and Xe. These relaxation rates are measured as a function of longitudinal velocities. Within the experiment accuracy, no remarkable velocity dependence of the depolarizing collisions rates was detected. This result confirms conventional approach of the depolarizing collisions theoretical treatment. In pure SF6 the rates of elastic depolarizing collisions for orientation and alignment proved smaller than the known rate of velocity changing collisions. It means that only part of the elastic collisions participates in destroying of the level multipole moments.
Stimulated photon echo technique with specially chosen linear polarizations of pumping pulses of exciting radiation is applied to investigation of depolarizing collisions in molecular gas SF6 and its mixtures with buffer gases He and Xe. For the first time, the collisional decay rates of population, orientation and alignment of SF6 levels are determined simultaneously. Translational velocity dependence of orientation and alignment collisional decay rates was under investigation. This velocity dependence proved to be negligible within the frames of experimental accuracy both in pure SF6 and in mixtures, which is in agreement with standard theoretical approach accepted for depolarizing collisions. Decay rates of orientation and alignment in pure SF6 have proved lower than velocity changing (elastic) collisions relaxation rate, which allows to conclude, that only some part of elastic collisions participates in destruction of multipole polarization moments of resonant levels. The evidence is obtained for j-dependence of multipole moments relaxation rates SF6.