Martin Schenk

Simultaneous vibrational and pure rotational coherent anti-Stokes Raman spectroscopy for temperature and multispecies concentration measurements demonstrated in sooting flames

The potential of measuring temperature and multiple species concentrations (N2, O2, CO) by use of combined vibrational coherent anti-Stokes Raman spectroscopy (CARS) and pure rotational CARS has been investigated. This was achieved with only one Nd:YAG laser and one dye laser together with a single spectrograph and CCD camera. From measurements in premixed sooting C2H4-air flames it was possible to evaluate temperatures from both vibrational CARS and rotational CARS spectra, O2 concentration from the rotational CARS spectra, and CO concentration from the vibrational CARS spectra. Quantitative results from premixed sooting C2H4-air flames are presented, and the uncertainties in the results as well as the possibility of extending the combined CARS technique for probing of additional species are discussed.

SIMULTANEOUS TEMPERATURE AND RELATIVE NITROGEN-OXYGEN CONCENTRATION MEASUREMENTS IN AIR WITH PURE ROTATIONAL COHERENT ANTI-STOKES RAMAN SCATTERING FOR TEMPERATURES TO AS HIGH AS 2050 K

The accuracy of temperature and simultaneous relative N(2) -O(2) concentration measurements of accumulated as well as of single-pulse rotational coherent anti-Stokes Raman spectra has been investigated in air in the temperature range from 300 to 2050 K. The experimental spectra were taken in a high-temperature oven at atmospheric pressure for a constant oxygen concentration of 20.9% (air). The evaluation procedure is based on the energy-corrected sudden-power scaling law. The agreement of the thermocouple readings with the mean values of the evaluated coherent anti-Stokes Raman spectroscopy temperatures is higher than 50 K and independent of the temperature. The evaluated oxygen concentration is found to be in the range from 20.0 to 21.7% and is also independent of the temperature.

Pure rotational coherent anti-Stokes Raman scattering: comparison of evaluation techniques for determining single-shot simultaneous temperature and relative N 2 –O 2 concentration

The accuracy and precision of time-resolved simultaneous temperature and O(2)-concentration measurements in binary N(2)-O(2) mixtures by single-pulse dual-broadband pure rotational coherent anti-Stokes Raman scattering (CARS) have been investigated. We present a detailed comparison of the applicability of six evaluation procedures to measurements of air in a temperature range 300-2050 K. Special emphasis is put on the dependence of the results on experimental restrictions and distortions. This comparison includes the least-sum-of-squared-differences fit (LSF) in the frequency space obtained by use of three different kinds of weighting with respect to signal intensity and in Fourier space by use of the complex or the cosine Fourier transformation, both of which permit a great reduction in the number of data points necessary for multidimensional evaluation. Additionally, a cross-correlation technique is tested that, to the best of our knowledge, was not previously applied to pure rotational CARS. We also present the results of measurements directed to the determination of low O(2)-concentration levels that were performed for various binary mixtures (1.0-15.6% O(2)) and for natural air within a temperature range of 300-773 K. A comparison is given for the three evaluation techniques that have proved most promising for the high-temperature investigations, i.e., the constant and the inverse weighted LSF in frequency space and the Fourier analysis technique.

Simultaneous temperature and relative O 2 –N 2 concentration measurements by single-shot pure rotational coherent anti-Stokes Raman scattering for pressures as great as 5 MPa

Dual-broadband pure rotational coherent anti-Stokes Raman scattering is a valuable nonintrusive tool for gas diagnosis that provides simultaneous and time-resolved information about temperature and relative species concentration. A systematic investigation of single-shot precision and accuracy of simultaneous measurement of temperature and O(2)/N(2) concentration is presented. Various O(2) concentrations (1.0-15.6%) in binary mixtures with N(2) have been investigated in a temperature range from 300 to 773 K and for pressures of 1-50 bars (0.1-5 MPa). A comparison of two least-sum-squared differences fit evaluation procedures for the spectral shape, weighted constantly or inversely with respect to the relative signal intensity, is given. The results yielded good accuracy and precision for measuring temperature as well as concentration. The influence of temperature, O(2) concentration, pressure, and evaluation techniques on both accuracy and precision is discussed.

One-dimensional vibrational coherent anti-Stokes Raman-scattering thermometry.

Quantitative one-dimensional single-pulse temperature measurements by broadband N(2) vibrational coherent anti-Stokes Raman scattering (CARS) are presented. A planar BOXCARS phase-matching geometry was used to generate the CARS signal along a 6.16-mm path positioned perpendicularly to the beam propagation. Depending on the imaging optics used, a spatial resolution of 86 mm was achieved. The applicability of this technique for measuring temperature gradients is demonstrated in a premixed laminar CH(4) -air f lame.

Simultaneous and time-resolved temperature and relative CO2-N2 and O2-CO2-N2 concentration measurements with pure rotational coherent anti-Stokes Raman scattering for pressures as great as 5 MPa

Pure rotational coherent anti-Stokes Raman-scattering (CARS) measurements have been performed in binary CO2-N2 and ternary CO2-O2-N2 mixtures in a temperature range between 300 and 773 K and pressures from 0.1 to 5 MPa to prove its potential for simultaneous single-shot thermometry and multispecies concentration measurements. In pressurized systems the CO2 component has a strong spectral influence on the pure rotational CARS spectra. Because of this dominance, pure rotational CARS proves to be a sensitive tool to measure in high-pressure combustion systems and the relative CO2-N2 concentration in the lower temperature range simultaneously with the temperature and the relative O2-N2 concentration. The evaluation of the spectra utilized a least-sum-squared differences fit of the spectral shape, weighted either constantly or inversely with respect to the normalized signal intensity. The results of the simultaneous temperature and relative CO2-N2 and O2-CO2-N2 concentration measurements provided a good accuracy and precision both in temperature and in concentrations. Because of the strong increase in the relative spectral contribution of CO2 with rising pressure, the precision of the CO2 concentration determination is in general significantly improved toward higher pressures, thus also clearly enhancing the CO2 detectability. The influence of temperature, O2 and CO2 concentration, pressure, and the evaluation techniques employed on both the accuracy and the precision is explained as well as their cross dependencies. The influence and limitations of the approximations used to model the CO2 molecule are discussed.

Time-resolved CO2 thermometry for pressures as great as 5 MPa by use of pure rotational coherent anti-Stokes Raman scattering

Pure rotational coherent anti-Stokes Raman scattering measurements of pure CO2 have been performed in a temperature range from 300 to 773 K and for pressure from 0.1 to 5 MPa for the purpose of time-resolved CO2 thermometry. Particular emphasis was put on the comparison of several line-width approximations to model the experimental spectra. Generally good agreement of the temperature mean values with the thermocouple reference has been found for all models over almost the whole pressure and temperature range investigated. The standard deviations, which increased with temperature, were comparable with or better than the results gained for single-shot measurements of pure N2 or O2-N2 mixtures. Yet for high particle densities close to the critical point of CO2 the limitation of the models became obvious, owing to the strongly increased influence of motional narrowing effects. The characteristics of these effects have been demonstrated by measurements even closer to the critical conditions.

Accuracy and precision of single-pulse one-dimensional vibrational coherent anti-Stokes Raman-scattering temperature measurements

The accuracy and precision of time-resolved one-dimensional temperature measurements using single-pulse one-dimensional N(2) vibrational coherent anti-Stokes Raman scattering along a line have been investigated in air in the temperature range from 300 to 1500 K. For this, the experimental spectra were taken in a high-temperature oven at atmospheric pressure. A planar BOXCARS phase-matching geometry was employed to generate the signal along a 6.16-mm line directed perpendicular to the beam propagation. With the used imaging optics, in this direction a spatial resolution of 86 mum was achieved. Depending on the set temperature, the agreement between the thermocouple readings and the mean values of the evalutated coherent anti-Stokes Raman-scattering temperatures is better than 40 K. The applicability of this new technique for the time-resolved measurement of temperature gradients is demonstrated along a line that crosses the flame front in a premixed laminar CH(4)-air flame.

Quantitative In-Cylinder NO-LIF Imaging in a Direct-Injected Gasoline Engine with Exhaust Gas Recirculation

The influence of exhaust gas recirculation (EGR) on the formation of nitric oxide (NO) was studied experimentally in a transparent gasoline direct injection engine by quantitative laser-induced fluorescence imaging. Spectral properties of the excited transition within the NO A2S+-X2P(0,2) band are well known from previous studies. The excitation scheme allows quantitative NO concentration measurements without detailed knowledge of the gas phase temperature. Good agreement was found with exhaust gas NOx chemiluminescence (CLD) measurements. The experiments were carried out in an optically accessible gasoline engine featuring a direct injection cylinder head (BMW) and a Bosch injection system, based on a serial inline six-cylinder engine with an enlarged crankcase. The measurements were performed in the pent-roof section of the combustion chamber. Various concentrations (0, 10 and 16%) and compositions (pure nitrogen, nitrogen / carbon dioxide and nitrogen / carbon dioxide / water) of synthetic exhaust gas were investigated. NO formation could be significantly reduced by EGR, from an average of about 1200 ppm (without EGR) to about 200 ppm (16% EGR-rate). The NO formation decreased steadily with increasing heat capacity of the inert gases present, independent of their chemical composition. In the temporal evolution of the NO formation, a retarded onset of up to 5° CA was found with 16% EGR. The two-dimensional NO concentration fields appeared to be very homogeneous when adding 16% EGR, whereas without EGR, strong inhomogeneities with local NO peak concentrations of up to 3400 ppm were detected.

Near-resonance enhanced O2 detection for dual-broadband pure rotational coherent anti-Stokes Raman scattering with an ultraviolet-visible setup at 266 nm.

Broadband and dual-broadband coherent anti-Stokes Raman scattering (CARS) are widely established tools for nonintrusive gas diagnostics. Up to now the investigations have been mainly performed for electronic nonresonant conditions of the gas species of interest. We report on the enhancement of the O2-N2 detection limit of dual-broadband pure rotational CARS by shifting the wavelength of the narrowband pump laser from the commonly used 532-266 nm. This enhancement is caused when the Schumann-Runge absorption band is approached near 176 nm. The principal concept of this experiment, i.e., covering the Raman resonance with a single- or dual-broadband combination of lasers in the visible range and moving only the narrowband probe laser near or directly into electronic resonant conditions in the UV range, should also be applicable to broadband CARS experiments to directly exploit electronic resonance effects for the purpose of single-shot concentration measurements of minority species. To quantify the enhancement in O2 sensitivity, comparative measurements at both a 266 and a 532 nm narrowband pump laser wavelength are presented, employing a 4-dicyanomethylene-2-methyl-6-(p-dimethylaminostyryl)-4H-pyram (DCM) dye laser as a broadband laser source at 635 nm. An increase of approximately equal to 13% in the ratio of the rotational CARS cross sections of O2 and N2 was obtained. The broad spectral width of the CARS excitation profile was approximately equal for both setups. Further enhancement should be achievable by shifting the narrowband pump laser closer toward 176 nm, for example, with a frequency-doubled optical parametric oscillator or an excimer laser. The principal concept of this experiment should also be applicable to broadband CARS experiments to directly exploit electronic resonance effects of the narrowband pump laser with electronic transitions of minority species for the purpose of single-shot concentration measurements of those species.