Observation of infrared–optical double resonance in NO2

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Abstract
Several experiments are described in which infrared–optical double resonance is observed for the first time in NO2. A cw argon‐ion laser (4545–5145 Å) is used to excite molecules to the 2B2 and 2B1 states and a chopped cw CO2 laser (9.2–10.8 μ) is employed to induce an excited vibronic state transition; detection is through infrared laser‐induced amplitude modulation of the visible fluorescence. Double resonance is, in fact, observed at each visible–infrared wavelength pair employed. This effect is studied as a function of laser wavelengths, lateral separation of the two laser beams, and NO2 pressure, and the modulated fluorescence is spectrally analyzed. These results suggest that isoenergetic collisional transfer may contribute to the observations. In addition, evidence is obtained that the optically excited levels participating in the double resonance have very short zero‐pressure lifetimes, ∼0.6±0.2 μsec.

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