Concentration and pressure scaling of CH2O electronic-resonance-enhanced coherent anti-Stokes Raman scattering signals

Nanosecond electronic-resonance-enhanced coherent anti-Stokes Raman scattering (ERE-CARS) is evaluated for the measurement of formaldehyde ( C H 2 O ) concentrations in reacting and nonreacting conditions. The three-color scheme utilizes a 532 nm pump beam and a scanned Stokes beam near 624 nm for Raman excitation of the C-H symmetric stretch ( ν 1 ) vibrational mode; further, a 342 nm resonant probe is tuned to produce the outgoing CARS signal via the 101403 vibronic transition between the ground ( X ~ 1 A 1 ) and first excited ( A ~ 1 A 2 ) electronic states. This allows detection of C H 2 O at concentrations as low as 9×10 14 m o l e c u l e s / c m 3 (55 parts per million) in a calibration cell with C H 2 O and N 2 at 1 bar and 450 K with 3% uncertainty. The measurements show a quadratic dependence of the signal with C H 2 O number density. Pressure scaling experiments up to 11 bar in the calibration cell show an increase in signal up to 8 bar. We study pressure dependence up to 11 bar and further apply the technique to characterize the C H 2 O concentration in an atmospheric premixed dimethyl ether/air McKenna burner flame, with a maximum concentration uncertainty of 11%. This approach demonstrates the feasibility for spatially resolved measurements of minor species such as C H 2 O in reactive environments and shows promise for application in high-pressure combustors.