Lamb-dip saturated-absorption cavity ring-down rovibrational molecular spectroscopy in the near-infrared

The high-detection-sensitivity saturated-absorption cavity ring-down (SCAR) technique is extended to Lamb-dip spectroscopy of rovibrational molecular transitions in the near-infrared region. Frequency-comb-referenced sub-Doppler saturation measurements, performed on the acetylene (nu(1) + nu(3) + nu(4) <- nu(4)) R(14)e line at 6562 cm(-1), are analyzed by a SCAR global line profile fitting routine, based on a specially developed theoretical model. Compared to a conventional cavity ring-down evaluation, our approach yields dip profiles with a linewidth freed from saturation broadening effects, reduced by 40%, and a signal-to-noise ratio increased by 90%. Ultimately, an overall (statistical and systematic) fractional uncertainty as low as 7 x 10(-12) is achieved for the absolute line-center frequency. At the same time, our method is also able to accurately infer the linear (non-saturated) behavior of the gas absorption, providing Lamb-dip-based line strength measurements with a relative uncertainty of 0.5%. (C) 2022 Chinese Laser Press