Cavity ringdown (CRD) spectroscopy, with its high sensitivity, provides a novel way to perform continuous-wave (cw) stimulated
Raman gain (SRG) spectroscopy, rather than by conventional optically detected coherent Raman techniques. Tunable cw laser
light at ∼1544 nm is used to probe ringdown decay from a rapidly-swept, high-finesse optical cavity containing a gas-phase
sample of interest and itself located inside the cavity of a cw single-longitudinal-mode Nd:YAG ring laser operating at ∼1064.4
nm. This approach is used to measure cw SRG spectra of the
ν
1 fundamental rovibrational Raman band of methane gas at ∼2916.5 cm
−1. The resulting SRG-CRD resonances have ringdown times longer than in the off-resonance case, in contrast to the usual shorter
ringdown times arising from absorption and other loss processes. Previously reported noise-equivalent sensitivities have been
substantially improved, by using a second ringdown cavity to facilitate subtraction of infrared-absorption background signals.
Moreover, by employing a ringdown cavity in the form of a ring, the SRG-pump and CRD-detected Stokes beams can co-propagate
uni-directionally, which significantly reduces Doppler broadening.
PACS 42.62.Fi - 42.65.Dr - 82.53.Kp