Signal-enhanced Raman spectroscopy with a multi-pass cavity for quantitative measurements of formaldehyde, major species and temperature in a one-dimensional laminar DME-air flame

Abstract

While Raman spectroscopy provides opportunities for simultaneous detection and quantitative analysis of multiple species, it also suffers from certain limitations, such as low signal strength, which often makes it unsuitable for the study of minor species. The present work employs a high-repetition-rate and high-power laser and re-introduces an amplification technique to improve the detection limit, providing an up to 45-time signal enhancement. The amplification is achieved by employing a multi-pass cavity, and different modes were tested and optimized for the measurements. This multi-pass setup has enabled the detection of formaldehyde (CH2O), which is present in stoichiometric dimethyl ether (DME)-air flames on a sub-percent level, and, therefore, known to be challenging to study with Raman spectroscopy. Furthermore, Raman cross-sections of CH2O and DME, which have not been reported in the literature to the authors’ knowledge, are obtained ab initio using Raman scattering activities in the literature. The cross-sections are 6.63 and 22.43, respectively, for CH2O and DME, normalized by the Raman cross-section of nitrogen. The CH2O detection limit in flame with was estimated to 40 ppm with the present experimental settings. Mole fractions of CH2O, nitrogen (N2), water (H2O), carbon dioxide (CO2), oxygen (O2), DME (CH3OCH3), carbon monoxide (CO), and hydrogen (H2) measured in the flame show good agreement when compared with modeling results obtained using two chemical kinetic mechanisms. Flame temperatures were evaluated from the N2 Raman signals, and the steep temperature gradient is successfully resolved experimentally with the multi-pass setup and well predicted by the models.