We utilize mid-infrared dual frequency comb spectroscopy for the detection of methane in ambient air. Two mid-infrared frequency comb sources based on femtosecond Er:fiber oscillators are produced through difference frequency generation with periodically poled MgO-doped lithium niobate crystals and stabilized at slightly different repetition rates at about 250 MHz. We performed dual frequency comb spectroscopy in the spectral range between 2900 cm −1 and 3150 cm −1 with 0.07 cm −1 resolution using a multipass cell of ~580 m path length, and achieved the sensitivity about 7.6 × 10 −7 cm −1 with 80 ms data acquisition time. We determined the methane concentration as ~1.5 ppmv in the ambient air of the laboratory, and the detection limit as ~60 ppbv for the current setup.

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Optical frequency combs have revolutionized the measurement of optical frequencies and improved the precision of spectroscopic experiments. Besides their importance as a frequency-measuring ruler, the frequency combs themselves can excite target transitions (direct frequency comb spectroscopy). The direct frequency comb spectroscopy may extend the optical frequency metrology into spectral regions unreachable by continuous wave lasers. In high precision spectroscopy, atoms/ions/molecules trapped in place have been often used as a target to minimize systematic effects. Here, we demonstrate direct frequency comb spectroscopy of single 25Mg ions confined in a Paul trap, at deep-UV wavelengths. Only one mode out of about 20,000 can be resonant at a time. Even then we can detect the induced fluorescence with a spatially resolving single photon camera, allowing us to determine the absolute transition frequency. The demonstration shows that the direct frequency comb spectroscopy is an important tool for frequency metrology for shorter wavelengths where continuous wave lasers are unavailable.

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