Laser frequency combs emit a spectrum with hundreds of thousands of evenly spaced phase-coherent narrow lines. A comb-enabled instrument, the dual-comb interferometer, exploits interference between two frequency combs and attracts considerable interest in precision spectroscopy and sensing, distance metrology, tomography, telecommunications, etc. Mutual coherence between the two combs over the measurement time is a pre-requisite to interferometry, although it is instrumentally challenging. At best, the mutual coherence reaches about 1 s. Computer-based phase-correction techniques, which often lead to artifacts and worsened precision, must be implemented for longer averaging times. Here with feed-forward relative stabilization of the carrier-envelope offset frequencies, we experimentally realize a mutual coherence over times approaching 2000 s, more than three orders of magnitude longer than that of state-of-the-art dual-comb systems. An illustration is given with near-infrared Fourier transform molecular spectroscopy with two combs of slightly different repetition frequencies. Our technique without phase correction can be implemented with any frequency comb generator including microresonators or semiconductor lasers.
Mid-infrared high-resolution spectroscopy has proven an invaluable tool for the study of the structure and dynamics of molecules in the gas phase. The advent of frequency combs advances the frontiers of precise molecular spectroscopy. Here we demonstrate, in the important 3-µm spectral region of the fundamental CH stretch in molecules, dual-comb spectroscopy with experimental coherence times between the combs that exceed half an hour. Mid-infrared Fourier transform spectroscopy using two frequency combs with self-calibration of the frequency scale, negligible contribution of the instrumental line shape to the spectral profiles, high signal-to-noise ratio, and broad spectral bandwidth opens up opportunities for precision spectroscopy of small molecules. Highly multiplexed metrology of line shapes may be envisioned.
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