The population of highly vibrationally excited molecular energy levels, which are not directly Franck-Condon accessible from thermally populated levels of the electronic ground state, is achieved by setting up a triple resonance excitation scheme using modulated gain spectroscopy1: A cw optically pumped molecular laser prepares a steady-state population in a selected vibronically highly excited ro-vibronic level of the electronic ground state. Excitation to the desired near-dissociation energy levels of the excited electronic state under study is finally achieved with a probe laser and detected by monitoring the change in the output of the molecular laser when the probe laser is tuned into resonance.

© 1984 Optical Society of America

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