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Journal of Physics B Atomic Molecular and Optical Physics

Observation of polarized 62P3/2thallium atoms produced in molecular photodissociation

A G Evseev, Oleg S. Vasyutinskii

Published Nov 14, 1991• 3 citations
Publisher

Abstract

The oriented and aligned metastable 6 2 P 3/2 thallium atoms produced in photodissociation of TlBr at 266 nm have been observed. The effect has been registered by a variable dichroism of the atomic vapours which is caused by a precession of the angular momenta in an external magnetic field. The application of the effect to study the dynamics of TlBr photodissociation has been discussed.

DOI
10.1088/0953-4075/24/21/002

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The Journal of Physical Chemistry A•Oct 1, 1997•66 citations
The oriented and aligned metastable 6 2 P 3/2 thallium atoms produced in photodissociation of TlBr at 266 nm have been observed. The effect has been registered by a variable dichroism of the atomic vapours which is caused by a precession of the angular momenta in an external magnetic field. The application of the effect to study the dynamics of TlBr photodissociation has been discussed.
A study has been made on the oriented ground state 5 2 S 1/2 Rb atoms produced in molecular photodissociation. Low-pressure RbI vapours have been photolysed by a beam of circularly polarized impulse laser radiation at 266 nm. The resulting Rb atoms were probed by a resonance atomic line at 794.8 nm from a discharge Rb lamp in two different experimental geometries. A free precession of the oriented atomic spins in an external magnetic field was detected by a dichroism of the atomic vapours. The initial degree of spin orientation was found to be P c = (20 +or- 2)%.
Decay rates of the 6 2P3/2 metastable and 6 2P1/2 ground state atomic thallium densities produced in UV photodissociation (at λ193, 222, 249, 308, and 353 nm) of TlI, TlBr, and TlCl molecular vapors have been measured for vapor densities from 1013 to 1017 cm−3. Dominant relaxation processes have been identified as (i) for the metastable state, collisional deexcitation by thallium halide molecules at high halide densities (≥1015 cm−3) and by free halogens and trace impurities at lower halide densities and (ii) for the ground state, diffusion in the ambient (argon/thallium halide) gas at high halide densities and volume reassociation under certain conditions at low halide densities. Cross sections and diffusion coefficients are evaluated.
The cross sections for production of 62P1/2 and 62P3/2 ground and metastable atomic thallium states via UV dissociation of the thallium halides TlCl, TlBr, and TlI have been measured at wavelengths 193, 222, 249, 308, and 353 nm using time-resolved atomic resonance absorption spectroscopy. The measured cross sections, which were independent of halide densities up to densities ∼1017 cm−3, were found to represent only 10% to 36% of the total UV absorption cross section at the appropriate wavelength.
The optical magnetic birefringence (Faraday) technique that can be used to study the anisotropy distributions of the angular momenta of photofragments produced in molecular photodissociation is compared theoretically and experimentally with the magnetic dichroism technique. The frame independent tensor form of the general expression describing the difference between an initial and a final polarization matrix of a probe light beam passing through the photofragment vapor is presented and analyzed. The procedure of detection of the photofragment electron orientation and alignment angular distributions by Doppler spectroscopy using each of the techniques is studied theoretically. The angular independent anisotropy orientation and alignment parameters describing photodissociation dynamics that can be determined from these studies are presented. It is shown that in principle each of the techniques can give the same information about the photodissociation dynamics; however, the birefringence technique has an undeniable advantage since it leads to an increase in accuracy of the experimental data. Both magnetic birefringence and magnetic dichroism techniques were used experimentally to study the spin orientation of ground state Rb atoms produced in photodissociation of RbI at 266 nm by circularly polarized laser light. The experiment was not of the Doppler spectroscopy type, but use of different 85 Rb and 87 Rb isotopes in the dissociation cell and in the probe light source allows detection of the oriented atomic photofragments separately by each of the techniques. Obtained experimental results are in agreement with the theoretical predictions. Contribution of the orientation of the Rb hyperfine structure energy states to the observed signals were also studied and treated theoretically. The initial degree of the electron spin orientation of the Rb atoms produced in the reaction was found to be P e = 0.11 ± 0.02.