In:
The Journal of Chemical Physics, AIP Publishing, Vol. 121, No. 14 ( 2004-10-08), p. 6835-6844
Abstract:
In this paper we propose and discuss the laser-induced circular dichroism (LICD) effect, which is expected to occur in linear molecules pumped by a strong circular resonant light beam. The effect is to be detected via the absorption of a weak circularly polarized probe beam on another transition. Analogous to the external magnetic field in magnetic circular dichroism the resonant circular polarized pumping optical field can induce the nonzero antisymmetric rotational polarizabilities of a linear molecule, and cause the LICD effect. LICD contains three distinct contributions from M-dependent splittings of the sublevels |JM〉 due to the ac Stark effect, from the differences of Boltzmann statistical distributions among the ground state sublevels |JM〉 due to the ac Stark splittings, and from the changes of occupation probability in rotational sublevels |JM〉 due to the pumping effect. The fundamental formulas for the above three terms of LICD have been deduced by the density matrix method. As an example, the LICD for CO molecules have been calculated. The results indicate that in comparison with the rotationally resolved magnetic vibrational circular dichroism experiment, LICD may be measurable and form a basis of a different kind of CD spectroscopy.
Type of Medium:
Online Resource
ISSN:
0021-9606
,
1089-7690
Language:
English
Publisher:
AIP Publishing
Publication Date:
2004
detail.hit.zdb_id:
3113-6
detail.hit.zdb_id:
1473050-9
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