Highly excited,normally inaccessible vibrational levels by sub-doppler modulated gain spectroscopy: The Na2 A1Σ+u state

Modulated gain spectroscopy is a sensitive, widely applicable, rovibronically state selective, sub-Doppler, triple resonance method for examining excited vibronic levels which are Franck—Condon inaccessible from thermally populated levels of the electronic ground state. A cw optically pumped molecular laser (OPL) prepares a steady-state population in a selected, vibrationally highly excited, rotation-vibration level of the electronic ground state (the lower level of the OPL transition). An intensity-modulated, single frequency dye laser excites part of this intracavity OPL-prepared population to the level of interest, thereby causing an increase in the OPL population inversion density, and, in turn, its output power. As the frequency of the dye laser is scanned, resonances are selectively detected by the appearance of modulation on the OPL output power; discrimination against dye laser excitations out of levels unconnected with the OPL is nearly perfect. Sub-Doppler (≈300 MHz FWHM) transitions are observed, thereby extending knowledge of the Na₂A¹Σ⁺_u state from v=44 to 62.