Degenerate Four-Wave Mixing of S2 and OH in Fuel-Rich Propane/Air/ S02 Flames

Absolute concentration profiles of S 2 and OH in a premixed propane/air/SO 2 flame at atmospheric pressure are determined by DFWM and absorption spectroscopy in the wavelength range from 308.5 to 310.5 nm. The OH radical is monitored via the well known (0,0) band of the electronic A( 2 Σ + )-X( 2 Π) system. Upon addition of SO 2 to the fuel stream numerous transitions of sulfur containing species are observed in addition. Recent molecular parameters for the B( 3 Σ u - )-X( 3 Σ g - ) transition of S 2 are used to compute a synthetic spectrum of the molecule within the accuracy of the laser system (0.15 cm -1 ) that overlaps favorably with major features in the experimental spectra. In spite of the dense spectrum, isolated transitions are observed that are suitable for concentration measurements. Relative concentrations of OH and S 2 are mapped by taking advantage of the high sensitivity of the DFWM technique. Absorption spectroscopy, on the other hand, is used to obtain an absolute number density of OH at positions in the flame where a significant level of the radical occurs. These measurements are linked to the relative OH profile and yield the absolute concentration of the hydroxyl as a function of height above the burner surface. Furthermore, the relative S 2 profile obtained by DFWM is put on an absolute scale by quantitative comparison with the OH profile. The required Einstein B coefficients for the B-X transition of S 2 are obtained from a calculation of Honl-London factors and taking into account the Franck-Condon factors and the electronic transition moment from the literature. The measured profiles of S 2 and OH are in good qualitative agreement with a recent theoretical model of the sulfur chemistry in flames.

[1]  Skip Williams,et al.  Reduction of degenerate four-wave mixing spectra to relative populations II. Strong-field limit , 1994 .

[2]  J. Lindner,et al.  Laser Spectroscopy of the B3Σ−u−X3Σ−g Spectrum of S2 Produced by Photodissociation , 1994 .

[3]  R. Farrow,et al.  On the interpretation and rotational assignment of degenerate four‐wave mixing spectra: Four‐photon line strengths for crossover resonances in NO A 2Σ+–X 2Π , 1994 .

[4]  R. Lucht,et al.  The effects of collisional quenching on degenerate four-wave mixing , 1993 .

[5]  R. Lucht,et al.  Saturation effects in gas-phase degenerate four-wave mixing spectroscopy: nonperturbative calculations , 1993 .

[6]  M. Aldén,et al.  Two-photon degenerate four-wave mixing (DFWM) for the detection of ammonia: Applications to flames , 1993 .

[7]  M. Aldén,et al.  Detection of CO molecules using two-photon degenerate four-wave mixing (DFWM) , 1992 .

[8]  David S. Green,et al.  Detection of trace species in hostile environments using degenerate four-wave mixing: CH in an atmospheric-pressure flame , 1992 .

[9]  Thomas Dreier,et al.  Investigation of the dependence of degenerate four-wave mixing line intensities on transition dipole moment , 1992 .

[10]  Steven Zabarnick A Comparison of CH4/NO/02 and CH4/N20 Flames by LIF Diagnostics and Chemical Kinetic Modeling , 1992 .

[11]  D. Greenhalgh,et al.  Degenerate four-wave mixing in nitrogen dioxide: Application to combustion diagnostics , 1992 .

[12]  M. Winter,et al.  Nearly degenerate four-wave mixing using phase-conjugate pump beams. , 1992, Optics letters.

[13]  M. Winter,et al.  Double phase-conjugate four-wave mixing of oh in flames , 1992 .

[14]  M. Aldén,et al.  Detection of nitrogen atoms in flames using two-photon laser-induced fluorescence and investigations of photochemical effects. , 1991, Applied optics.

[15]  T. Dreier,et al.  Detection of NH radicals in flames using degenerate four-wave mixing , 1991 .

[16]  Thomas Dreier,et al.  Degenerate four-wave mixing diagnostics on OH and NH radicals in flames , 1990 .

[17]  T. Dreier,et al.  Measurement of OH rotational temperatures in a flame using degenerate four-wave mixing. , 1990, Optics letters.

[18]  J. Goldsmith,et al.  Doppler-free two-photon-excited fluorescence spectroscopy of OH in flames , 1988, International Laser Science Conference.

[19]  Robert J. Kee,et al.  A hybrid Newton/time-integration procedure for the solution of steady, laminar, one-dimensional, premixed flames , 1988 .

[20]  O. Smith,et al.  Experimental and numerical studies of sulfur chemistry in H2/O2/SO2 flames☆ , 1987 .

[21]  Ronald K. Hanson,et al.  Shock-tube study of pressure broadening of the A2∑+ - X2Π (0,0) band of OH by Ar and N2 , 1987 .

[22]  P Ewart,et al.  Detection of OH in a flame by degenerate four-wave mixing. , 1986, Optics letters.

[23]  D. Chandler,et al.  An experimental study of probe distortions to the structure of one-dimensional flames☆ , 1986 .

[24]  J. Wendt,et al.  Postflame behavior of nitrogenous species in the presence of fuel sulfur: II. Rich, CH4/He/O2 flames , 1984 .

[25]  O. Smith,et al.  Enhancement of Fuel-Nitrogen Oxidation by Fuel-Sulfur in Fuel Rich Flames , 1983 .

[26]  R. Lind,et al.  8 – Phase Conjugation and High-Resolution Spectroscopy by Resonant Degenerate Four-Wave Mixing , 1983 .

[27]  Robert C. Hilborn,et al.  Einstein coefficients, cross sections, f values, dipole moments, and all that , 1982, physics/0202029.

[28]  R. Cattolica OH radical nonequilibrium in methaneair flat flames , 1982 .

[29]  James A. Miller,et al.  ON THE USE OF ADAPTIVE GRIDS IN NUMERICALLY CALCULATING ADIABATIC FLAME SPEEDS , 1982 .

[30]  D. Puechberty,et al.  Use of laser-induced fluorescence of OH to study the perturbation of a flame by a probe , 1981 .

[31]  D. Crosley,et al.  Calculated rotational transition probabilities for the A−X system of OH , 1980 .

[32]  D. Crosley,et al.  Franck–Condon factors for the B–X system of S2 , 1979 .

[33]  K. German Direct measurement of the radiative lifetimes of the A2Σ+ (V′ = 0) states of OH and OD , 1975 .

[34]  D. Crosley,et al.  Franck‐Condon factors from selectively excited resonance fluorescence in the B‐X system of S2 , 1973 .

[35]  J. Watson,et al.  Rotational Line Strengths in 3~*-3~ * Transitions with Intermediate Coupling , 1971 .

[36]  R. Tischer Zum EPR-Spektrum des molekularen Sauerstoffs , 1967 .

[37]  S. Penner,et al.  Radiation from Isolated Spectral Lines with Combined Doppler and Lorentz Broadening , 1953 .