Isotope analysis of water by means of near-infrared dual-wavelength diode laser spectroscopy

A novel diode laser spectrometer was developed using dual-wavelength multiplexing, ensuring ideal conditions for high-precision and simultaneous measurements of the 2H/1H, 17O/16O, and 18O/16O isotope ratios in water. A 1.4-µm diode laser probed a H16OH/HO2H line pair near 7198 cm-1, while a similar laser observed H16OH, H17OH, and H18OH ro-vibrational lines around 7183 cm-1, or a H16OH/H18OH line pair near 7200 cm–1. The 1-σ standard deviation is 0.2‰ for 18O/16O, and 0.5‰ for the 2H/1H and 17O/16O isotope ratios. Preliminary experiments with repeated injections of a natural abundance sample point to an accuracy of about 1‰ for all three isotope ratios in natural samples.

Observing the intrinsic linewidth of a quantum-cascade laser: beyond the Schawlow-Townes limit

A comprehensive investigation of the frequency-noise spectral density of a free-running mid-infrared quantum-cascade laser is presented for the first time. It provides direct evidence of the leveling of this noise down to a white noise plateau, corresponding to an intrinsic linewidth of a few hundred Hz. The experiment is in agreement with the most recent theory on the fundamental mechanism of line broadening in quantum-cascade lasers, which provides a new insight into the Schawlow-Townes formula and predicts a narrowing beyond the limit set by the radiative lifetime of the upper level.Comment: 4 pages, 4 figure

Primary gas thermometry by means of laser-absorption spectroscopy: Determination of the Boltzmann constant

We report on a new optical implementation of primary gas thermometry based on laser absorption spectrometry in the near infrared. The method consists in retrieving the Doppler broadening from highly accurate observations of the line shape of the R(12) $\nu_{1} + 2 \nu_{2}^{\phantom{1}0} + \nu_{3}$ transition in CO$_{2}$ gas at thermodynamic equilibrium. Doppler width measurements as a function of gas temperature, ranging between the triple point of water and the gallium melting point, allowed for a spectroscopic determination of the Boltzmann constant with a relative accuracy of $\sim1.6\times10^{-4}$.Comment: Submitted to Physical Review Letter

Novel laser-based techniques for monitoring of volcanoes

An overview of novel laser techniques suitable for volcanic monitoring, based on different kinds of infrared laser sources, is presented. Their main advantages and drawbacks are discussed focusing on the achievable sensitivity and precision levels in analysis of gaseous species. Some of the most recent experimental results obtained in laboratory development as well as in field tests of home-built laser spectrometers are reported. New perspectives in optical devices aimed at geochemical and geophysical applications are also considered

Comb-assisted spectroscopy of CO2 absorption profiles in the near- and mid-infrared regions

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Absorption line shape recovery beyond the detection bandwidth limit: application to the precision spectroscopic measurement of the Boltzmann constant

22 pagesInternational audienceA theoretical model of the influence of detection bandwidth properties on observed line shapes in laser absorption spectroscopy is described. The model predicts artificial frequency shifts, extra broadenings and line asymmetries which must be taken into account in order to obtain accurate central frequencies and other spectroscopic parameters. This reveals sources of systematic effects most probably underestimated so far potentially affecting spectroscopic measurements. This may impact many fields of research, from atmospheric and interstellar physics to precision spectroscopic measurements devoted to metrological applications, tests of quantum electrodynamics or other fundamental laws of nature. Our theoretical model is validated by linear absorption experiments performed on H2O and NH3 molecular lines recorded by precision laser spectroscopy in two distinct spectral regions, near- and mid-infrared. Possible means of recovering original line shape parameters or experimental conditions under which the detection bandwidth has a negligible impact, given a targeted accuracy, are proposed. Particular emphasis is put on the detection bandwidth adjustments required to use such high-quality molecular spectra for a spectroscopic determination of the Boltzmann constant at the 1 ppm level of accuracy

Versatile mid-infrared frequency-comb referenced sub-Doppler spectrometer

We present a mid-IR high-precision spectrometer capable of performing accurate Doppler-free measurements with absolute calibration of the optical axis and high signal-to-noise ratio. The system is based on a widely tunable mid-IR offset-free frequency comb and a Quantum-Cascade-Laser (QCL). The QCL emission frequency is offset locked to one of the comb teeth to provide absolute-frequency calibration, spectral-narrowing, and accurate fine frequency tuning. Both the comb repetition frequency and QCL-comb offset frequency can be modulated to provide, respectively, slow- and fast-frequency-calibrated scanning capabilities. The characterisation of the spectrometer is demonstrated by recording sub-Doppler saturated absorption features of the CHF3 molecule at around 8.6 μm with a maximum signal-to-noise ratio of ∼7 × 103 in 10 s integration time, frequency-resolution of 160 kHz, and accuracy of less than 10 kHz.We present a mid-IR high-precision spectrometer capable of performing accurate Doppler-free measurements with absolute calibration of the optical axis and high signal-to-noise ratio. The system is based on a widely tunable mid-IR offset-free frequency comb and a Quantum-Cascade-Laser (QCL). The QCL emission frequency is offset locked to one of the comb teeth to provide absolute-frequency calibration, spectral-narrowing, and accurate fine frequency tuning. Both the comb repetition frequency and QCL-comb offset frequency can be modulated to provide, respectively, slow- and fast-frequency-calibrated scanning capabilities. The characterisation of the spectrometer is demonstrated by recording sub-Doppler saturated absorption features of the CHF3 molecule at around 8.6 μm with a maximum signal-to-noise ratio of ∼7 × 103 in 10 s integration time, frequency-resolution of 160 kHz, and accuracy of less than 10 kHz