Infrared laser-absorption sensing for combustion gases

We demonstrate that a previously proposed model opens the route for the inclusion of refined non-Voigt profiles in spectroscopic databases and atmospheric radiative transfer codes. Indeed, this model fulfills many essential requirements: (i) it takes both velocity changes and the speed dependences of the pressure-broadening and -shifting coefficients into account. (ii) It leads to accurate descriptions of the line shapes of very different molecular systems. Tests made for pure H2, CO2 and O2 and for H2O diluted in N2 show that residuals are down to ≃ 0.2 % of the peak absorption, (except for the untypical system of H2 where a maximum residual of ±3% is reached), thus fulfilling the precision requirements of the most demanding remote sensing experiments. (iii) It is based on a limited set of parameters for each absorption line that have known dependences on pressure and can thus be stored in databases. (iv) Its calculation requires very reasonable computer costs, only a few times higher than that of a usual Voigt profile. Its inclusion in radiative transfer codes will thus induce bearable CPU time increases. (v) It can be extended in order to take line-mixing effects into account, at least within the so-called first-order approximation.

An isolated line-shape model to go beyond the Voigt profile in spectroscopic databases and radiative transfer codes

We review progress, since publication of the book ``Collisional effects on molecular spectra: Laboratory experiments and models, consequences for applications" (Elsevier, Amsterdam, 2008), on measuring, modeling and predicting the influence of pressure (ie of intermolecular collisions) on the spectra of gas molecules. We first introduce recently developed experimental techniques of high accuracy and sensitivity. We then complement the aforementioned book by presenting the theoretical approaches, results and data proposed (mostly) in the last decade on the topics of isolated line shapes, line-broadening and -shifting, line-mixing, the far wings and associated continua, and collision-induced absorption. Examples of recently demonstrated consequences of the progress in the description of spectral shapes for some practical applications (metrology, probing of gas media, climate predictions) are then given. Remaining issues and directions for future research are finally discussed.

/pdf/recent-advances-in-collisional-effects-on-spectra-of-1nv24iyx02.pdf

Recent advances in collisional effects on spectra of molecular gases and their practical consequences

Linestrengths and lineshapes for 7 H2O absorption transitions in the ν 1 + ν 3 combination band near 1.4 μm were measured at high resolution using tunable diode laser absorption. H2O- and N2-perturbed lineshapes were measured at 300–1300 K and 2–760 Torr and Voigt, Galatry, Rautian, and quadratic-speed-dependent-Voigt profiles were least-squares fit to measured spectra using a multi-spectrum fitting routine. Transitions with J ″ of 6–18 were studied to highlight the importance of collisional resonance and illustrate how the best-fit lineshape parameters varied with J ″ . The accuracy of the Voigt profile decreased as J ″ increased (especially for J = K c doublets). For transitions in N2, the collisional-broadening temperature exponents varied from ≈ 0.8 to −0.4 (for the Voigt profile) as J ″ increased and this behavior coincided with increasing speed-dependent collisional-broadening coefficients. The quadratic-speed-dependent Voigt profile was found to offer the best combination of accuracy and robust lineshape parameters; however, Rautian and Galatry profiles provided similar performance.

Diode-laser measurements of linestrength and temperature-dependent lineshape parameters for H2O transitions near 1.4 μm using Voigt, Rautian, Galatry, and speed-dependent Voigt profiles

Absorption lineshapes for two unresolved H2O doublets near 4029.52 and 4041.92 cm−1 were measured at high-resolution in a heated static cell using two distributed-feedback diode lasers. Measurements were acquired for H2O, CO2, and N2 perturbers over a temperature and pressure range of 650–1325 K and 2–760 Torr, respectively. Strong collisional narrowing effects were observed in CO2 and N2, but not in pure H2O. The Galatry profile was used to infer collisional-broadening and -narrowing coefficients and their respective temperature dependence for CO2 and N2 perturbers. The collisional-broadening and -narrowing coefficients for CO2 perturbers were found to decrease with increasing temperature in a similar manner. For N2 perturbers, the collisional-broadening coefficients increased with temperature while the collisional-narrowing coefficients decreased with increasing temperature. Self-broadening coefficients were inferred from Voigt profile fits and are compared with HITEMP 2010. The linestrengths of 17 H2O transitions are also reported.

Diode laser measurements of linestrength and temperature-dependent lineshape parameters of H2O-, CO2-, and N2-perturbed H2O transitions near 2474 and 2482 nm

The integrated intensities, self- and air-broadening coefficients of thirteen transitions of H216O in the 11980–12260 cm−1 region, belonging to the 2ν1+ν2+ν3 band, were measured. Using a tunable diode laser system, spectra were recorded at room temperature for a wide range of pressure (2–15 Torr for pure H2O and 50–760 Torr for H2O in air). Line parameters were adjusted from experiments using three line-shape models: the Voigt profile (VP), the (hard collision) Rautian profile (RP) and the speed dependent Voigt profile (SDVP). The results show that the RP and SDVP are in better agreement with measurements than the VP and that they lead to larger values of the line parameters (about 5% for the line broadening, and 0.8% for the line intensity). Comparisons of the present results with HITRAN 2008 [Rothman et al., JQSRT 2009, 110:533-72] show that the HITRAN intensities of the studied lines are overestimated by about 9.4%, suggesting a more complete study of the H2O line parameters in the considered region. The Dicke narrowing and speed dependence parameters deduced from this work are also presented and discussed, demonstrating the need for a more refined line-shape model.

Intensities and shapes of H2O lines in the near-infrared by tunable diode laser spectroscopy

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Intensities and shapes of H2O lines in the near-infrared by tunable diode laser spectroscopy