Abstract

We report what is to our knowledge the first generation of far-infrared laser radiation by stimulated Raman scattering resonantly enhanced by an overtone vibrational–rotational transition. Using a frequency-tunable high-pressure CO2 laser as the pump source, we obtained laser emission in the frequency range from 12 to 27 cm−1 by optical pumping of gaseous CH3I near resonant vibrational–rotational transitions of the 2ν3 overtone and the ν6 fundamental band. Overtone Raman transitions involving the nondegenerate ν3 vibration were found to show higher efficiency than Raman transitions within the fundamental band of the twofold-degenerated ν6 vibration. From the studies of the temporal behavior of the far-infrared laser emission, we estimate a bandwidth of approximately 200 MHz for the Raman gain regions for both the 2ν3 overtone and the ν6 fundamental transitions.

© 1992 Optical Society of America

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