Gael Mouret

Atmospheric emissions from waste recovery centers are strictly regulated by industrial emission directives which stipulate that they should be continuously monitored. In this work, we demonstrate and evaluate the capacity of terahertz rotational spectroscopy for real-time diagnosis and monitoring of gases of environmental interest on industrial sites. A spectrometer based on the use of a frequency multiplication chain operating at 530–620 GHz has been constructed, enabling the detection of most of the regulated compounds in waste incineration. The detection limits obtained are compatible with regulatory emission limit values. The installation of the instrument at the waste recovery center in Dunkirk demonstrated its ability to perform real-time quantitative multi-component in situ monitoring in an industrial environment. Continuous measurements of SO ₂ and CO over more than 24 h are compared with the measurements performed by two certified infrared instruments. The agreement between the three sets of measurements is excellent, demonstrating that high-resolution terahertz spectroscopy is relevant for real-time in situ monitoring of regulated industrial emissions gases, constituting an interesting alternative to other techniques thanks to a higher degree of selectivity.

We demonstrate the advantages of THz frequency combs for high-resolution spectroscopy. This benefits from wide spectral coverage and the exact knowledge of the frequency position of each comb component. Heterodyne detection combined with a fast Fourier spectrometer enables rapid and simultaneous measurement of more than 80 frequency comb modes covering a 7.5 GHz bandwidth. A spectrum is obtained in under 20 minutes yielding a uniform resolution of 70 kHz. This new setup has been validated by recording more than 150 lines of methanol around 723 GHz, and represents a new solution to exploit THz frequency combs for high-resolution spectroscopy.

A novel high finesse cavity allowing THz CRDS has enabled accurate quantification of CF₄. Yielding spectral parameters with unprecedented precision, these finding are critical to monitor and understand CF₄'s contribution to global radiative forcing.

The correct interpretation of infrared (IR) observations of planetary atmospheres requires an accurate knowledge of temperature and partial and global pressures. Precise laboratory measurements of absorption intensities and line profiles, in the 200–350 K temperature range, are, therefore, critical. However, for gases only existing in complex chemical equilibria, such as nitrous or hypobromous acids, it is not possible to rely on absolute pressure measurements to measure absolute integrated optical absorption cross sections or IR line intensities. To overcome this difficulty, a novel dual-beam terahertz (THz)/mid-IR experimental setup has been developed, relying on the simultaneous use of two instruments. The setup involves a newly constructed temperature-controlled (200–350 K) cross-shaped absorption cell made of inert materials. The cell is traversed by the mid-IR beam from a high-resolution Fourier transform spectrometer using along a White-cell optical configuration providing absorption path lengths from 2.8 to 42 m and by a THz radiation beam (82.5 GHz to 1.1 THz), probing simultaneously the same gaseous sample. The THz channel records pure rotational lines of molecules for which the dipole moment was previously measured with high precision using Stark spectroscopy. This allows for a determination of the partial pressure in the gaseous mixture and enables absolute line intensities to be retrieved for the mid-IR range. This new instrument opens a new possibility for the retrieval of spectroscopic parameters for unstable molecules of atmospheric interest. The design and performance of the equipment are presented and illustrated by an example of simultaneous THz and mid-IR measurement on nitrous acid (HONO) equilibrium.

Synchrotron radiation (SR) has proven to be an invaluable contributor to the field of molecular spectroscopy, particularly in the terahertz region (1-10 THz) where its bright and broadband properties are currently unmatched by laboratory sources. However, measurements using SR are currently limited to a resolution of around 30 MHz, due to the limits of Fourier-transform infrared spectroscopy. To push the resolution limit further, we have developed a spectrometer based on heterodyne mixing of SR with a newly available THz molecular laser, which can operate at frequencies ranging from 1 to 5.5 THz. This spectrometer can record at a resolution of 80 kHz, with 5 GHz of bandwidth around each molecular laser frequency, making it the first SR-based instrument capable of sub-MHz, Doppler-limited spectroscopy across this wide range. This allows closely spaced spectral features, such as the effects of internal dynamics and fine angular momentum couplings, to be observed. Furthermore, mixing of the molecular laser with a THz comb is demonstrated, which will enable extremely precise determinations of molecular transition frequencies.