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Physical Review A

Light shifts in quantum-beat spectroscopy

DONG TAI-QIAN, Harold J. Metcalf

Published Jun 1, 1982• 1 citation
Publisher

Abstract

In ordinary quantum-beat spectroscopy the excitation mechanism (e.g., laser pulse) is not expected to affect the results because the measurements are made on a freely evolving atom in the dark (after pulse ends). In this paper we point out an example where this is not so. As an example, we show how light shifts can alter the results of time-delayed measurements.

DOI
10.1103/physreva.25.3435

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In ordinary quantum-beat spectroscopy the excitation mechanism (e.g., laser pulse) is not expected to affect the results because the measurements are made on a freely evolving atom in the dark (after pulse ends). In this paper we point out an example where this is not so. As an example, we show how light shifts can alter the results of time-delayed measurements.
The resolution of a quantum-beat experiment, which is basically limited by the atomic natural linewidth, has been improved by observing the fluorescence only from those atoms which have survived in excited states after some time delay. The resulting narrowing enables one to resolve previously overlapping lines in beam-foil quantum-beats experiments using $\mathrm{H}\ensuremath{\alpha}$ and 4He^{4}\mathrm{He}4He ii (4\ensuremath{\rightarrow}3) deexcitation.
Atomic mirrors and beam splitters based on adiabatic following by delayed laser pulses in a three-level Raman configuration are analyzed. We show that in a pure three-level system of two ground states and one excited state, laser pulses tuned precisely on resonance with the excited state do not produce any accumulated phase shifts due to ac Stark shifts even if the process is nonadiabatic. A numerical simulation suggests that multiple delayed laser pulses are attractive for precision interferometry since high transfer efficiencies (up to 98.7% per pulse for the cesium D1 line) and low ac Stark shifts are expected. A possible application to optical two-photon spectroscopy for an optical clock is discussed.
Within this work, electron dynamics inside argon atoms are observed by probing the autoionizing states of argon atoms, so-called window resonances, with both attosecond XUV and timed-delayed few-cycle femtosecond NIR laser pulses, using attosecond transient absorption spectroscopy. The window resonances in the energy region of 25 - 29.3 eV are first excited with the XUV pulse and then dressed by the NIR laser, where the natural decay process of the states is greatly affected by the strong-field of the NIR pulse. Preliminary results of the measurement are presented in this work, with a hypothetical description of some of the effects that are present. A comparison has been made with the experimental results from a paper publishing measurements of autoionizing states with attosecond transient absorption spectroscopy for the first time, where the same resonances were probed. The comparison is only partly possible due to different experimental parameters and conditions, where more pronounced and new effects have been observed in the here performed measurement.
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.