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Journal of Physics B Atomic and Molecular Physics

Observation of cascade quantum beats in atomic fluorescence

Bryan J. Dalton

Published Aug 14, 1982• 9 citations
Publisher

Abstract

Strong cascade Zeeman beats have been observed in the 3720 AA fluorescence from the z 5 F 5 0 level of Fe I following selective stepwise excitation of the higher e 5 D 4 level with linearly polarised light from two pulsed dye lasers.
DOI
10.1088/0022-3700/15/15/002

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For pt.I see ibid., vol.20, p.251 (1987). Theoretical expressions for cascade light intensity as a function of time have been evaluated for the case of cascade Zeeman beats produced by two-step excitation with broad-line laser pulses, and the results are compared with experimentally observed cascade Zeeman beats in Fe I. The beats were detected in time-resolved fluorescence from intermediate levels populated by cascades from highly excited levels of Fe I, using three different stepwise-excitation-cascade sequences. In the case of coincident laser pulses, good agreement between theory and experiment is obtained over a range of magnetic fields when allowance is made for Larmor precessions during the excitation period, for the width and shape of the exciting laser pulses and for the contribution of impurity processes. The effects of precession during the excitation period are especially important for the excitation sequence a 5 D 4 to z 5 F degrees 5 to e 5 F 5 , for which short-pulse theories predict no quantum beats for the experimental geometry used (parallel linear polarisations in the two excitation steps). For non-coincident pulses a predicted oscillation in the amplitude of the cascade beats with magnetic field has also been observed.

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For pt.I see ibid., vol.20, p.251 (1987). Theoretical expressions for cascade light intensity as a function of time have been evaluated for the case of cascade Zeeman beats produced by two-step excitation with broad-line laser pulses, and the results are compared with experimentally observed cascade Zeeman beats in Fe I. The beats were detected in time-resolved fluorescence from intermediate levels populated by cascades from highly excited levels of Fe I, using three different stepwise-excitation-cascade sequences. In the case of coincident laser pulses, good agreement between theory and experiment is obtained over a range of magnetic fields when allowance is made for Larmor precessions during the excitation period, for the width and shape of the exciting laser pulses and for the contribution of impurity processes. The effects of precession during the excitation period are especially important for the excitation sequence a 5 D 4 to z 5 F degrees 5 to e 5 F 5 , for which short-pulse theories predict no quantum beats for the experimental geometry used (parallel linear polarisations in the two excitation steps). For non-coincident pulses a predicted oscillation in the amplitude of the cascade beats with magnetic field has also been observed.
A theory of stepwise pulsed-laser excitation of cascade Zeeman quantum beats has been developed for a four-level system. The laser pulses are treated in the broad-line approximation and the full optical-pumping equations for the atomic-density matrix of each level have been obtained. These can be used to describe saturation and light shift effects. The weak-pumping theory solutions to the optical pumping equations have been used to obtain expressions for the cascade quantum-beat intensity versus time curves. Larmor precession, spontaneous-emission decay and the populating of the final cascade level during the excitation pulse are all allowed for. A Wiener-Levy phase diffusion model with slowly varying amplitudes is used for the laser pulses, and the final theoretical expressions for the quantum beats depend on the time-dependent intensities of the laser pulses as well as on their polarisations. Hyperfine effects have been ignored. The theory applies to both coincident pulses and to pulses with a time delay between them. An illustrative application to the case of two very short but coincident pulses (during which Larmor precession, spontaneous emission etc. can be ignored) is given. In an accompanying paper the theoretical expressions are further evaluated and successfully applied to the interpretation of cascade Zeeman quantum beat experiments in Fe I.