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Modulation transfer spectroscopy is used to demonstrate absolute frequency stabilization of an 8.6-µm-wavelength quantum cascade laser against a sub-Doppler absorption of the C H F 3 molecule. The obtained spectral emission properties are thoroughly characterized through a self-referenced optical frequency comb, stabilized against either a GPS-disciplined Rb clock or a 1.54-µm Er-fiber laser locked to a high-finesse ultra-low-expansion optical cavity. Fractional long-term stability and accuracy at a level of 4×10 -12 (at 100 s) and 3×10 -10 , respectively, are demonstrated, along with an emission linewidth as narrow as 10 kHz for observation times of 0.1 s.

We report on absolute measurements of saturated-absorption line-center frequencies of room-temperature trifluoromethane using a quantum cascade laser at 8.6 μm and the frequency modulation spectroscopy method. Absolute calibration of the laser frequency is obtained by direct comparison with a mid-infrared optical frequency comb synthesizer referenced to a radio-frequency Rb standard. Several sub-Doppler transitions falling in the υ 5 vibrational band are investigated at around 1158.9  cm -1 with a fractional frequency precision of 8.6·10 -12 at 1-s integration time, limited by the Rb-clock stability. The demonstrated frequency uncertainty of 6.6·10 -11 is mainly limited by the reproducibility of the frequency measurements.

We report saturated-absorption spectra recorded by use of 5 muW of infrared radiation coupled into a build-up cavity. Single-pass generation of difference-frequency radiation tunable near 4.25 mum in a periodically poled LiNbO(3) crystal was used. Lamb dips of weak transitions of the fundamental rovibrational band of CO(2) were observed, for what is believed to be the first time, up to the J=82 level. Application of these results to the extension of frequency-comb-based metrology in the infrared is discussed.