We report a photoacoustic spectroscopy setup with a high-power mid-infrared frequency comb as the light source. The setup is used in broadband spectroscopy of radiocarbon methane. Due to the high sensitivity of a cantilever-enhanced photoacoustic cell and the high power light source, we can reach a detection limit below 100 ppb in a broadband measurement with a sample volume of only a few milliliters. The first infrared spectrum of 14 CH 4 is reported and given a preliminary assignment. The results lay a foundation for the development of optical detection systems for radiocarbon methane.

We report a novel, to the best of our knowledge, photoacoustic spectrometer for trace gas sensing of benzene. A quantum cascade laser emitting at the wavelength 14.8 µm is used as the light source in the spectroscopic detection. This wavelength region contains the strongest vibrational band of benzene, which is free of spectral overlap from common trace gases, making it a strong candidate for sensitive benzene detection. Cantilever-enhanced photoacoustic spectroscopy is used for detection. This simple and robust measurement setup can reach a benzene detection limit below 1 ppb.

Abstract:A fully stabilized mid-infrared optical frequency comb spanning from 2.9 to 3.4 µm is described. The comb is based on half-harmonic generation in a femtosecond optical parametric oscillator, which transfers the high phase coherence of a fully stabilized nearinfrared Er-doped fiber laser comb to the mid-infrared region. The method is simple, as no phase-locked loops or reference lasers are needed. Precise locking of optical frequencies of the mid-infrared comb to the pump comb is experimentally verified at sub-20 mHz level, which corresponds to a fractional statistical uncertainty of 2×10 -16 at the center frequency of the midinfrared comb. The fully stabilized mid-infrared comb is an ideal tool for high-precision molecular spectroscopy, as well as for optical frequency metrology in the mid-infrared region, which is difficult to access with other stabilized frequency comb techniques.

We report a setup for high-resolution two-photon spectroscopy using a mid-infrared continuous wave optical parametric oscillator (CW-OPO) and a near-infrared diode laser as the excitation sources, both of which are locked to fully stabilized optical frequency combs. The diode laser is directly locked to a commercial near-infrared optical frequency comb using an optical phaselocked loop. The near-infrared frequency comb is also used to synchronously pump a degenerate femtosecond optical parametric oscillator to produce a fully stabilized mid-infrared frequency comb. The beat frequency between the mid-infrared comb and the CW-OPO is then stabilized through frequency locking. We used the setup to measure a double resonant twophoton transition to a symmetric vibrational state of acetylene with a sub-Doppler resolution and high signal-to-noise ratio.© 2017 Optical Society of America. One print or electronic copy may be made for personal use only. Systematic reproduction and distribution, duplication of any material in this paper for a fee or for commercial purposes, or modifications of the content of this paper are prohibited. Bartalini, and P. De Natale, "Subkilohertz linewidth room-temperature mid-infrared quantum cascade laser using a molecular sub-Doppler reference," Opt. Lett. 37(23), 4811-4813 (2012). 9.

A method of measuring double resonant two-photon signal and background from a single cavity ring-down decay is introduced. This is achieved by modulating the double resonance loss via one of the light sources exciting the transition. The noise performance of the method is characterized theoretically and experimentally. The addition of a new parameter to the fitting function introduces a minor noise increase due to parameter correlation. However, the concurrent recording of the background can extend the stable measurement time. Alternatively, the method allows a faster measurement speed, while still recording the background, which is often advantageous in double resonance measurements. Finally, the method is insensitive to changes in the cavity decay rate at short timescales and can lead to improved performance if they have significant contribution to the final noise level compared to the detector noise.