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The Journal of Chemical Physics

Helicity of orientation parameters of photofragments in fluorescence-imaging experiments

Kuo-mei Chen, Cheng-chih Pei

Published Oct 22, 1998• 8 citations
Publisher

Abstract

A detection scheme in fluorescence-imaging experiments is presented for determining helicity of orientation parameters of photofragments prepared by circularly polarized photolysis lasers. In a framework of density matrix theory, explicit fluorescence intensity formulas are derived for detection of right- and left-circularly polarized fluorescence photons in various transition sequences. A pattern recognition from fluorescence images of photofragments in a state of definite helicity with respect to their recoil directions has been established, where differences between left- and right-circularly polarized fluorescence image patterns should be taken. Information on the coherence among various magnetic sublevels of an angular momentum state can be obtained by monitoring fluorescence images in a ΔJ=−1 transition (P branch in absorption).

DOI
10.1063/1.477316

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A detection scheme in fluorescence-imaging experiments is presented for determining helicity of orientation parameters of photofragments prepared by circularly polarized photolysis lasers. In a framework of density matrix theory, explicit fluorescence intensity formulas are derived for detection of right- and left-circularly polarized fluorescence photons in various transition sequences. A pattern recognition from fluorescence images of photofragments in a state of definite helicity with respect to their recoil directions has been established, where differences between left- and right-circularly polarized fluorescence image patterns should be taken. Information on the coherence among various magnetic sublevels of an angular momentum state can be obtained by monitoring fluorescence images in a ΔJ=−1 transition (P branch in absorption).
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Circular dichroism has been detected in the polarization of the fluorescence resulting from the decay of excited calcium ions. Synchrotron radiation was used to both ionize and excite calcium atoms from their ground state, and the photoejected electron was detected in coincidence with the polarized fluorescent photon. By introducing a degree of left, then right circularly polarized light into the incident photon beam the circular dichroism could be measured. The analysis of the results was carried out using recent developments of the statistical tensor method, and it was possible to determine the sign of the phase difference between the outgoing waves.
When a diatomic molecule is photodissociated on a singlet molecular potential energy surface to give two singlet atoms, one of which is electronically excited, the atoms are left in pure angular momentum states referred to the molecular quantization axis. Transformation of such pure states to a laboratory frame of reference gives atomic wave functions that are described as coherent superpositions of states. Application of an external magnetic field to an ensemble of excited atoms causes quantum beats, or, alternately, a Hanle effect to appear in the fluorescence emitted by the atoms. Calculations show that the interference effects are observed only for certain geometrical arrangements of the electric vector of the photodissociating radiation, the external field, and the polarization direction accepted by the fluorescence detector. The expressions for the fluorescence intensity show that the phase and modulation depth of the quantum beat can be used to determine the asymmetry parameter for recoil of the photofragments.