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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

Kim, Haisol LU ; Zubairova, Alsu LU ; Aldén, Marcus LU and Brackmann, Christian LU (2022) In Combustion and Flame 244.
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... (More)

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.

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author
; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
DME flame, Formaldehyde, Laser-based diagnostics, Multi-pass, Raman Spectroscopy
in
Combustion and Flame
volume
244
article number
112221
publisher
Elsevier
external identifiers
  • scopus:85131811706
ISSN
0010-2180
DOI
10.1016/j.combustflame.2022.112221
language
English
LU publication?
yes
id
e48865d3-3c14-4d8a-b35a-e15c70118e71
date added to LUP
2022-09-05 14:35:17
date last changed
2023-11-06 21:31:42
@article{e48865d3-3c14-4d8a-b35a-e15c70118e71,
  abstract     = {{<p>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 (CH<sub>2</sub>O), 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 CH<sub>2</sub>O 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 CH<sub>2</sub>O and DME, normalized by the Raman cross-section of nitrogen. The CH<sub>2</sub>O detection limit in flame with was estimated to 40 ppm with the present experimental settings. Mole fractions of CH<sub>2</sub>O, nitrogen (N<sub>2</sub>), water (H<sub>2</sub>O), carbon dioxide (CO<sub>2</sub>), oxygen (O<sub>2</sub>), DME (CH<sub>3</sub>OCH<sub>3</sub>), carbon monoxide (CO), and hydrogen (H<sub>2</sub>) measured in the flame show good agreement when compared with modeling results obtained using two chemical kinetic mechanisms. Flame temperatures were evaluated from the N<sub>2</sub> Raman signals, and the steep temperature gradient is successfully resolved experimentally with the multi-pass setup and well predicted by the models.</p>}},
  author       = {{Kim, Haisol and Zubairova, Alsu and Aldén, Marcus and Brackmann, Christian}},
  issn         = {{0010-2180}},
  keywords     = {{DME flame; Formaldehyde; Laser-based diagnostics; Multi-pass; Raman Spectroscopy}},
  language     = {{eng}},
  publisher    = {{Elsevier}},
  series       = {{Combustion and Flame}},
  title        = {{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}},
  url          = {{http://dx.doi.org/10.1016/j.combustflame.2022.112221}},
  doi          = {{10.1016/j.combustflame.2022.112221}},
  volume       = {{244}},
  year         = {{2022}},
}