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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.

Broadband femtosecond (fs) two-photon laser-induced fluorescence (TP-LIF) of the B 1 Σ + ←X 1 Σ + , Hopfield-Birge system of carbon monoxide (CO) is believed to have two major advantages compared to narrowband nanosecond excitation. It should (i) minimize the effects of pressure-dependent absorption line broadening and shifting, and (ii) produce pressure-independent TP-LIF signals as the effect of increased quenching due to molecular collisions is offset by the increase in number density. However, there is an observed nonlinear drop in the CO TP-LIF signal with increasing pressure. In this work, we systematically investigate the relative impact of potential deexcitation mechanisms, including collisional quenching, forward lasing, attenuation of the source laser by the test cell windows or by the gas media, and a 2+1 photoionization process. As expected, line broadening and collisional quenching play minor roles in the pressure-scaling behavior, but the CO fs TP-LIF signals deviate from theory primarily because of two major reasons. First, attenuation of the excitation laser at high pressures significantly reduces the laser irradiance available at the probe volume. Second, a 2+1 photoionization process becomes significant as the number density increases with pressure and acts as a major deexcitation pathway. This work summarizes the phenomena and strategies that need to be considered for performing CO fs TP-LIF at high pressures.

Quantitative femtosecond two-photon laser-induced fluorescence of atomic oxygen was demonstrated in an H 2 /air flame at pressures up to 10 atm. Femtosecond excitation at 226.1 nm was used to pump the 3pP3 J ' =0,1,2 ←←2pP3 J '' =0,1,2 electronic transition of atomic oxygen. Contributions from multiphoton de-excitation, production of atomic oxygen, and photolytic interferences were investigated and minimized by limiting the laser irradiance to ∼10 11   W/cm 2 . Quantitative agreement was achieved with the theoretical equilibrium mole fraction of atomic oxygen over a wide range of fuel-air ratios and pressures in an H 2 /air laminar calibration burner.

Interference-free hybrid femtosecond/picosecond vibrational coherent anti-Stokes Raman scattering (CARS) of nitrogen is reported for temperature measurements of 1300-2300 K in high-pressure, laminar H 2 -air and CH 4 -air diffusion flames up to 10 bar. Following coherent Raman excitation by 100 fs duration pump and Stokes pulses, a time-asymmetric probe pulse is used for the detection of spectrally resolved N 2 CARS signals at probe delays as early as ∼200-300  fs. This allows for full rejection of nonresonant contributions while being independent of collisions for single-shot precision of ±2% at elevated pressures. The effects of collisions at longer probe-pulse delays are also investigated to determine the feasibility of varying the detection timing from 200 fs to 100 ps.

Quantitative, kiloherz-rate measurement of carbon monoxide mole fractions by femtosecond two-photon, laser-induced fluorescence (TP-LIF) was demonstrated in high-pressure, luminous flames over a range of fuel-air ratios. Femtosecond excitation at 230.1 nm was used to pump CO two-photon rovibrational X 1 Σ + →B 1 Σ + transitions in the Hopfield-Birge system and avoid photolytic interferences with excitation irradiance ∼1.7×10 10   W/cm 2 . The effects of excitation wavelength, detection scheme, and potential sources of de-excitation were also assessed to optimize the signal-to-background and signal-to-noise ratios and achieve excellent agreement with theoretically predicted CO mole fractions at low and high pressure.

A compact-footprint (0.18  m 2 ) flash-lamp-pumped, burst-mode Nd:YAG-based master-oscillator pulsed-amplifier laser is reported with a fundamental 1064 nm output of over 14 J per burst. A directly modulated diode laser seed source is used to generate 10 ms duration arbitrary sequences of 500 kHz doublet or MHz singlet pulses for flow-field velocity or species measurements, respectively. Flexible pulse widths are used to balance the energy distribution of pulse doublets and achieve second-harmonic conversion efficiencies up to 42%. Burst-mode laser performance characteristics, measurement accuracies in turbulent flows, and prospects for kHz-MHz flow-field diagnostics are discussed.