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We present a new method of optical frequency comb spectroscopy that combines cavity enhancement with frequency modulation to obtain immunity to laser frequency-to-amplitude noise conversion by the cavity modes and, thus, high absorption sensitivity over a broad spectral range. A frequency comb is locked to a cavity with a free spectral range (FSR) equal to 4/3 times the repetition rate of the laser, and phase-modulated at a frequency equal to the cavity FSR. The transmitted light is analyzed by a Fourier transform spectrometer with a high bandwidth detector. Phase-sensitive detection of the interferogram yields a noise-immune cavity-enhanced optical frequency comb spectroscopy (NICE-OFCS) signal. In the first demonstration, we record NICE-OFCS signals from the overtone CO2 band at 1575 nm with absorption sensitivity of 4.3×10(-10) cm(-1) Hz(-1/2) per spectral element, close to the shot noise limit.

We demonstrate detection of atmospheric species in air and combustion environment using near-infrared cavity-enhanced optical frequency comb spectroscopy based on an Er:fiber femtosecond laser and a fast-scanning Fourier transform spectrometer.

International audience; We present a robust, compact, and transportable instrument that measures the iodine monoxide atmospheric radical at extremely low concentration, down to 40 ppqv (parts per quadrillion by volume, 1:1015). As nitrogen dioxide is strongly absorbed in the same spectral region it could be simultaneously measured down to 4 pptv (parts per trillion by volume, 1:1012). Relying on ''mode locked cavity-enhanced absorption spectroscopy,'' the instrument makes use of a free-running commercial femtosecond Titane Saphir laser. We demonstrate that this multiplex detection scheme provides shot noise limited spectra for acquisition times as long as 5 min. Moreover, this instrument is very versatile as it can be potentially tuned from the infrared to the ultraviolet (1080-340 nm) to reach various molecular absorptions. It has been recently deployed at the Station Biologique de Roscoff on the North West Atlantic coast of France.

We demonstrate near-infrared cavity-enhanced optical frequency comb spectroscopy of water in a premixed methane/air flat flame. The detection system is based on an Er:fiber femtosecond laser, a high finesse optical cavity containing the flame, and a fast-scanning Fourier transform spectrometer (FTS). High absorption sensitivity is obtained by the combination of a high-bandwidth two-point comb-cavity lock and auto-balanced detection in the FTS. The system allows recording high-temperature water absorption spectra with a resolution of 1 GHz and a bandwidth of 50 nm in an acquisition time of 0.4 s, with absorption sensitivity of 4.2 × 10(-9) cm(-1) Hz(-1/2) per spectral element.