Validation of a rotational coherent anti-Stokes Raman spectroscopy model for carbon dioxide using high-resolution detection in the temperature range 294-1143 K.

Experiments were performed in the temperature range of 294-1143 K in pure CO(2) using high-resolution rotational coherent anti-Stokes Raman spectroscopy (CARS), in the dual-broadband approach. Experimental single-shot spectra were recorded with high spectral resolution using a single-mode Nd:YAG laser and a relay imaging lens system on the exit of a 1 m spectrometer. A theoretical rotational CARS model for CO(2) was developed for evaluation of the experimental spectra. The evaluated mean temperatures of the recorded single-shot dual-broadband rotational coherent anti-Stokes Raman spectroscopy (DB-RCARS) spectra using this model showed good agreement with thermocouple temperatures, and the relative standard deviation of evaluated single-shot temperatures was generally 2-3%. Simultaneous thermometry and relative CO(2)/N(2)-concentration measurements were demonstrated in the product gas of premixed laminar CO/air flames at atmospheric pressure. Although the model proved to be accurate for thermometry up to 1143 K, limitations were observed at flame temperatures where temperatures were overestimated and relative CO(2)/N(2) concentrations were underestimated. Potential sources for these discrepancies are discussed.

Improved temperature precision in rotational coherent anti-stokes raman spectroscopy with a modeless dye laser.

Single-shot thermometry with dual-broadband rotational coherent anti-Stokes Raman spectroscopy that employs amplified spontaneous emission from a broadband modeless dye laser has been examined. Evaluation of single-shot spectra of air, N2, and O2 showed an improved temperature precision at room temperature compared with the precision obtained with a conventional dye laser. A comparison was also made between the use of single-mode and multimode Nd:YAG lasers as sources for narrowband radiation, and in all cases the single-mode Nd:YAG laser resulted in higher precision. The experimental results are compared with theoretical predictions.

Pure rotational coherent anti-Stokes Raman spectroscopy in mixtures of CO and N2.

We present a model for quantitative measurements in binary mixtures of nitrogen and carbon monoxide by the use of dual-broadband rotational coherent anti-Stokes Raman spectroscopy. The model has been compared with experimental rotational coherent anti-Stokes Raman scattering spectra recorded within the temperature range of 294-702 K. Temperatures and concentrations were evaluated by spectral fits using libraries of theoretically calculated spectra. The relative error of the temperature measurements was 1-2%, and the absolute error of the CO concentration measurements was <0.5% for temperatures < or =600 K. For higher temperatures, the gas composition was not chemically stable, and we observed a conversion of CO to CO2. The influence of important spectroscopic parameters such as the anisotropic polarizability and Raman line-broadening coefficients are discussed in terms of concentration measurements. In particular, it is shown that the CO concentration measurement was more accurate if N2-CO and CO-N2 line-broadening coefficients were included in the calculation. The applicability of the model for quantitative flame measurements is demonstrated by measuring CO concentrations in ethylene/air flames.