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Physics Letters A

Preparation and decay of an excited molecular state studied by optical-rf double resonance

F. Bylicki, H.G. Weber

Published Jan 1, 1984• 8 citations
Publisher
DOI
10.1016/0375-9601(84)90755-2

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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 NO2{\mathrm{NO}}_{2}NO2​ 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.
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.