Femtosecond two-photon LIF imaging of atomic hydrogen in high-pressure methane-air flames

Abstract

Atomic hydrogen (H) imaging studies in combustion systems have been limited thus far to atmospheric- or low-pressure flames. The commonly used excitation scheme for two-photon laser-induced fluorescence (TPLIF) of H involves 205-nm deep-ultra-violet (DUV) laser pulses generated using nanosecond (ns), picosecond (ps), or femtosecond (fs) laser systems. Ultrashort pulse, fs excitation schemes are more attractive because of the efficient two-photon excitation and interference-free kHz-rate imaging capability. In this work, we implemented a home-built, direct fourth harmonic generation (FHG) laser system to generate high-energy fs pulses for H imaging in CH4/air flames at pressures up to 10 bar. The high-energy FHG output was capable of overcoming transmission losses of DUV laser pulses through thick optical windows of the pressure vessel. Signal interferences such as photoionization, photolytic production, amplified spontaneous emission, and background chemiluminescence were avoided or minimized during data acquisition and subsequent data processing steps. A quadratic dependence of the H TPLIF signal on the laser energy was observed. The increase in the pressure from 1 to 10 bar showed a rapid decay of the fs H TPLIF signal although it should scale linearly with increasing H number density with pressure ideally at equilibrium conditions. Besides a detailed quenching correction, laser absorption and fluorescence signal trapping remain major issues at elevated pressures. The measured fluorescence signals are compared with the equilibrium H number densities and local H concentrations calculated using the Cantera (0D) and UNICORN (2D) flame codes, respectively, for a range of equivalence ratios, and possible reasons for discrepancies are discussed. Experimentally obtained 1D and 2D spatial distributions of H are well predicted by the UNICORN flame model. Steps towards quantitative single-shot H TPLIF imaging measurements in high-pressure flames are also discussed. Overall, the fs TPLIF imaging technique coupled with a high-efficiency home-built FHG system is a promising diagnostic approach for H imaging in high-pressure flames.