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Physical Review A

Effect of inversion of polarization in laser-excited molecular beams

Wojciech Gawlik

Published Mar 1, 1987• 3 citations
Publisher

Abstract

In the paper by Weber, Bylicki, and Miksch [Phys. Rev. A 30, 270 (1984)] the ``inversion effect'' of the Hanle and rf double-resonance signals in ${\mathrm{NO}}_{2}$ molecules is explained with the questionable assumption of a ``light-induced stability of the optically prepared state.'' We give an alternative explanation of the ``inversion effect'' which is based on the nonstationarity of molecular perturbation by a laser and which is consistent with the present knowledge of interaction of laser light with matter.

DOI
10.1103/physreva.35.2744

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In the paper by Weber, Bylicki, and Miksch [Phys. Rev. A 30, 270 (1984)] the inversion effect'' of the Hanle and rf double-resonance signals in ${\mathrm{NO}}_{2}$ molecules is explained with the questionable assumption of a light-induced stability of the optically prepared state.'' We give an alternative explanation of the ``inversion effect'' which is based on the nonstationarity of molecular perturbation by a laser and which is consistent with the present knowledge of interaction of laser light with matter.
We report on a new effect which is observed when the small polyatomic molecule NO2{\mathrm{NO}}_{2}NO2​ is prepared under collision-free conditions into an electronically excited state. As the intensity of the exciting laser light is varied, the degree of polarization of the fluorescence light may undergo a change in sign. The analysis of the experimental results confronts us with an interesting problem concerning the time evolution of an isolated polyatomic system. In this paper we present the experimental results and a simple model which successfully describes these results. According to this model, the inversion of the polarization of the fluorescence light is a consequence of light-induced stability of the optically prepared state.
New studies of Na2{\mathrm{Na}}_{2}Na2​ hyperfine structure (hfs) by the laser-induced-fluorescence molecular-beam magnetic-resonance technique are described which show that state selection and detection by strong optical fields can produce rf-magnetic-resonance spectra which differ drastically from the Rabi shape, even though the optical and rf fields do not act simultaneously on the molecules. We suggest that in the case of optically unresolved ground-state sublevels these effects are due to the creation of ground-state coherence by absorption and stimulated-emission cycles in the laser field, and we present a model calculation which exhibits the essential features of the observed spectra. We also give a proof that no model based only upon populations can explain the negative signals we observe.
With use of a narrow-band laser, the free NO2{\mathrm{NO}}_{2}NO2​ molecule is prepared in a well-defined excited state under conditions that correspond to an optical-frequency--radiofrequency double-resonance experiment. We observe a resonant increase or decrease (dependent on the divergence of the light beam) of the total fluorescence intensity when the radiofrequency field is in resonance with the Zeeman splitting in the ground or excited state of the laser-induced transition. These resonances differ significantly from well-known optical-rf double-resonance signals and laser saturation effects. The resonances are, however, well described with use of a model which assumes an irreversible evolution in the free NO2{\mathrm{NO}}_{2}NO2​ molecule.
The polarization state of laser light is affected by the nonlinear processes in the matter it passes through. Wieman and Hancsh’ used this effect to investigate the spectra of molecular systems. Another example is the laser-based investigations of parity-breaking weak interactions,2 In this contribution we investigate polarization changes induced by a three-level cascade system when laser light is used to break the left-right symmetry of the atom. By causing the asymmetry externally we can manipulate the effect and observe its magnitude and signal shape. Works related to ours are those by Liao and Bjorklund.3,4