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Physical Review A

ac Stark splitting in doubly resonant three-photon ionization with nonmonochromatic fields

A. T. Georges, P. Lambropoulos

Published Aug 1, 1978• 104 citations
Publisher

Abstract

We present a theory of Stark splitting in doubly resonant three-photon ionization (three-level system) with nonmonochromatic fields. The asymmetry of the peaks of the resonance curve due to Stark splitting is shown to be reversed when the laser bandwidth is larger than the width of the atomic transitions of the resonant states. It is further shown that ionization as well as the probe field have a significant effect on the features of the splitting. Similar effects are found with monochromatic fields in the presence of an additional level near the initial level (four-level system). The results of the analysis are in general qualitative agreement with existing observations.

DOI
10.1103/physreva.18.587

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We present a theory of Stark splitting in doubly resonant three-photon ionization (three-level system) with nonmonochromatic fields. The asymmetry of the peaks of the resonance curve due to Stark splitting is shown to be reversed when the laser bandwidth is larger than the width of the atomic transitions of the resonant states. It is further shown that ionization as well as the probe field have a significant effect on the features of the splitting. Similar effects are found with monochromatic fields in the presence of an additional level near the initial level (four-level system). The results of the analysis are in general qualitative agreement with existing observations.
An intense laser and a probe laser in near resonance with the sodium $3{S}_{\frac{1}{2}}\ensuremath{\rightarrow}3{P}_{\frac{1}{2}}$ and $3{P}_{\frac{1}{2}}\ensuremath{\rightarrow}4{D}_{\frac{3}{2}}$ transitions, respectively, produce a three-photon ionization current used to study the broadening and Rabi splitting of the 3P123{P}_{\frac{1}{2}}3P21​​ intermediate state as a function of probe-laser tuning. We find a narrow, intense-laser detuning region where the peak-heights ratio of the Rabi-split 3P123{P}_{\frac{1}{2}}3P21​​ doublet is reversed from that predicted for a monochromatic laser field. This is attributed to the finite (\ensuremath{\sim} GHz) laser linewidth.
A detailed theoretical analysis of ac Stark splitting in double optical resonance and resonance fluorescence by a nonmonochromatic complex chaotic field is presented. It is shown that a one-photon transition undergoes Stark splitting, which is strongly affected by the intensity fluctuations of the chaotic light. On resonance, the lines in the doublet structure of double optical resonance and the sidebands of the triplet structure in resonance fluorescence are broadened by the intensity fluctuations and tend to copy the Rayleigh distribution of the field amplitude. Off resonance, the asymmetry of the doublet in double optical resonance is reversed and a sideband asymmetry appears in resonance fluorescence for finite bandwidth of the incident light. While on resonance the splitting is always reduced, off resonance the intensity fluctuations may lead to an enhancement of the splitting in comparison to phase-diffusing light.
In this paper we present a detailed treatment of the ac Stark effect of a three-level atom driven by two strong laser fields in a cascade scheme. We consider two situations where there is a weak laser field probing a new transition starting from one of the three levels to a fourth level. In one case the initial level of the probed transition is the ground state and in the other case the initial level is the intermediate state. For both situations we derive an analytical expression for the absorptive and dispersive responses of the weak probe field and present the spectrum obtained from numerical calculation. The general feature of the spectrum has a three-peak structure. The positions and relative intensities of the three spectral components are affected strongly by the driving field intensities and detunings. An account of the spectrum is given in terms of the dressed-state formalism.
An experimental study of doubly resonant multiphoton ionization of Na has been carried out. Coherence effects, such as AC - Stark splitting and population trapping, have been manifested in different coupling schemes, i.e. ladder, lambda, vee configurations. These effects have been investigated in terms of their dependence on the laser intensity and resonance detuning, as well as the state of the laser polarization. The experimental results are qualitatively interpreted in terms of a few level system.
Ac-Stark-broadened three-photon resonances in four-photon ionization of iodine atoms are investigated experimentally and analyzed theoretically, including the effect of laser intensity fluctuations and spatiotemporal distribution of average intensity. It is shown that the resonance maximum cannot be used in estimating the hyperpolarizabilities of atomic levels. By applying the properly designed procedure, the difference in hyperpolarizabilities of 5p(2P1/2) and nd(…)73/2 levels is found to be α12 = 20 ± 10 Å3.