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Thermodynamic measurements in a high pressure hydrogen-oxygen flame using Raman scattering from a broadband excimer laser

Raman scattering is an inelastic molecular scattering process in which incident radiation is reemitted at a fixed change in frequency. Raman spectroscopy can be used to measure the number density and temperature of the irradiated species. The strength of the Raman signal is inversely proportional to the wavelength raised to the fourth power. Consequently, high signal to noise ratios are obtained by using ultraviolet (UV) excitation sources. Using UV sources for Raman Spectroscopy in flames is complicated by the fact that some of the primary constituents in hydrogen-oxygen combustion absorb and reemit light in the UV and these fluorescence processes interfere with the Raman signals. This problem has been handled in atmospheric pressure flames in some instances by using a narrowband tunable excimer laser as a source. This allows for detuning from absorption transitions and the elimination of interfering fluorescence signals at the Raman wavelengths. This approach works well in the atmospheric pressure flame; however, it has two important disadvantages. First, injection-locked narrowband tunable excimer lasers are very expensive. More importantly, however, is the fact that at the high pressures characteristic of rocket engine combustion chambers, the absorption transitions are broadened making it difficult to tune to a spectral location at which substantial absorption would not occur. The approach taken in this work is to separate the Raman signal from the fluorescence background by taking advantage of the fact that Raman signal has nonisotropic polarization characteristics while the fluorescence signals are unpolarized. Specifically, for scattering at right angles to the excitation beam path, the Raman signal is completely polarized. The Raman signal is separated from the fluorescence background by collecting both horizontally and vertically polarized signals separately. One of the polarizations has both the Raman signal and the fluorescence background while the other has only the fluorescence signal. The Raman scatter is the difference between the signals. By choosing an appropriate optical setup, both signals can be obtained simultaneously with the same monochromator; hence, time resolved measurements are possible using this approach.

Hartfield, Roy, Jr.

Electride Mediated Surface Enhanced Raman Scattering (SERS)

An electride may provide surface enhanced Raman scattering (SERS). The electride, a compound where the electrons serve as anions, may be a ceramic electride, such as a conductive ceramic derived from mayenite, or an organic electride, for example. The textured electride surface or electride particles may strongly enhance the Raman scattering of organic or other Raman active analytes. This may also provide a sensitive method for monitoring the chemistry and electronic environment at the electride surface. The results are evidence of a new class of polariton (i.e., a surface electride-polariton resonance mechanism) that is analogous to the surface plasmon-polariton resonance that mediates conventional SERS.

Anderson, Mark S.

Raman scattering applied to hypersonic air flow

The Raman scattering technique was applied to measure the local static temperature and gas number density over a sharp-edge flat-plate model in a Mach 5 nozzle of the Langley nozzle test chamber with air as the test gas. The angle of attack varied from -5 to 15 deg, and the stagnation temperature varied from 317 to 442 K, with stagnation pressures ranging from 170 kN to 2.8 MN/sq m. The measured values of static temperature and density ranged from 60 to 100 K and from 0.03 to 0.8 kg/cu m, respectively. A comparison with calculated values based on static pressure measurements along the model shows that the Raman scattering technique is a viable measurement method in applications to high-speed three-dimensional flows.

Hillard, M. E., Jr.

Experimental investigation of transient stimulated Raman scattering in a linearly dispersionless medium.

The results of numerical calculations of the transient stimulated Raman scattering reported previously have been verified experimentally under conditions where both linear dispersion and self-focusing effects were negligible. The existence of a delay between maxima of the laser and Stokes pulses is experimentally demonstrated for the first time, while the pulse shortening in time via Raman scattering is established more firmly than in previous work. The incident-laser-pulse duration, generated-Stokes-pulse duration, and delay between intensity maxima for the laser and Stokes pulses were measured with the two-photon absorption-fluorescence technique. The effective phonon-dephasing time is determined via spontaneous Raman scattering. By using these measured quantities, inferences are made as to the magnitude of the transient gain and the shape of the exciting picosecond laser pulse.

Carman, R. L.

AROTEL Temperature Retrievals Within PSC's Using Raman Scattering

NASA Goddard Space Flight Center's Airborne Raman Ozone Temperature Lidar (AROTEL) made temperature retrievals within Polar Stratospheric Clouds (PSCs) on several flights during the SAGE III Ozone Loss and Validation Experiment (SOLVE) campaign. The location of the PSCs was confirmed using simultaneously acquired data from the NASA Langley Aerosol lidar. Retrievals were made on flight dates 991207, 991210 and 000127 from just above the aircraft to 25 kilometers geometric altitude. Raman temperature retrievals are, to first order, insensitive to Mie interference because the Raman signals are red shifted by 2331 cm(exp -1) from the initial laser wavelength. Backscattering from clouds and aerosols is consequently not observed by the detector; however, extinction does impact the measurement and limits retrievals to optically thin clouds. Comparisons between retrievals employing Rayleigh and Raman scattering show the Raman temperatures to be significantly warmer than those employing Rayleigh scattering. Uncertainties are a function of altitude: at 25 km they were approximately 3 K. Temperature profiles could not be retrieved for optically thick clouds.

Burris, John

Spontaneous Raman Scattering (SRS) System for Calibrating High-Pressure Flames Became Operational

A high-performance spontaneous Raman scattering (SRS) system for measuring quantitative species concentration and temperature in high-pressure flames is now operational. The system is located in Glenn s Engine Research Building. Raman scattering is perhaps the only optical diagnostic technique that permits the simultaneous (single-shot) measurement of all major species (N2, O2, CO2, H2O, CO, H2, and CH4) as well as temperature in combustion systems. The preliminary data acquired with this new system in a 20-atm hydrogen-air (H2-air) flame show excellent spectral coverage, good resolution, and a signal-to-noise ratio high enough for the data to serve as a calibration standard. This new SRS diagnostic system is used in conjunction with the newly developed High- Pressure Gaseous Burner facility (ref. 1). The main purpose of this diagnostic system and the High-Pressure Gaseous Burner facility is to acquire and establish a comprehensive Raman-scattering spectral database calibration standard for the combustion diagnostic community. A secondary purpose of the system is to provide actual measurements in standardized flames to validate computational combustion models. The High-Pressure Gaseous Burner facility and its associated SRS system will provide researchers throughout the world with new insights into flame conditions that simulate the environment inside the ultra-high-pressure-ratio combustion chambers of tomorrow s advanced aircraft engines.

Nguyen, Quang-Viet

Temperature Measurements in Hypersonic Wind Tunnels via Femtosecond Coherent Anti-Stokes Raman Scattering

A femtosecond coherent anti-Stokes Raman scattering (fs CARS) instrument is developed to perform gas-phase thermometry in cold-flow hypersonic wind tunnels. Measurements are reported for Mach 8 and 14 pure-nitrogen flows. The fs CARS instrument includes a 100 fs pump/Stokes pulse and a spectrally narrow probe pulse from a second harmonic bandwidth compressor. Important experimental considerations such as limits on the pump/Stokes pulse energy are discussed. The fs CARS focusing and collimating optics are mounted on a two-axis translation stage system to scan the measurement location during a 30 second wind tunnel run. Single-laser-shot rotational CARS spectra are recorded at the laser repetition rate of 1 kHz in the wind tunnel freestream and near simple cone models. Spectral fitting is used to determine quantitative gas temperatures. Freestream temperatures at Mach 8 and 14 spanned ranges of 40–75 and 35–50 K, respectively, depending on tunnel operating conditions. Temperature variations across the central 100 mm span of the wind tunnel were quantified. Measured temperature jumps across conical bow shocks from various models varied by less than 1% from predicted values. Hypersonic boundary layer measurements were demonstrated. In conclusion, these measurements illustrate the utility and robustness of this instrument for the study of complex fluid flow phenomena in challenging ground test facilities.

Aerodynamics

Effects of Raman scattering on the water-leaving radiance

The contribution of Raman scattering to the water-leaving radiance is examined using Monte Carlo simulations. Exit angle information is retained, allowing a comparison of different satellite viewing directions. Chlorophyll values of 0.0, 0.01, 0.1, and 1.0 mg Chl/cu m are simulated. Little directional variability is found, with the exception of the direct solar backscatter direction. The wavelength variability is greatest for low chlorophyll concentrations and is negligible for 1.0 mg Chl/cu m. At 550 nm the Raman contribution ranges from approximately 18% of the total water-leaving radiance for pure water to 3% for 1.0 mg Chl/cu m. At 440 nm the range is from 6% to 2%, indicating that Raman scattering will impact radiance ratios for ocean color satellite algorithms.

Waters, Kirk J.

Raman scattering as a probe of planetary atmospheres

The observable effects of Raman scattering on the spectra of the giant planets may provide new information on the composition and structure of these atmospheres. Satellite observations have already shown the influence of Raman scattering on the UV continuum albedo. A cross correlation technique is presented for detecting rotational and vibrational transitions of the Raman active gases in the atmosphere. This technique has been applied to ground-based visible spectra of Venus, Jupiter, Saturn and Uranus. Extension of this method into the UV would improve the detectability of the Raman lines because the ratio of Raman to Rayleigh cross section increases with decreasing wavelength. The technology currently exists to efficiently obtain high-signal-to-noise ratio UV spectra through the use of silicon diode array detectors. Application of the cross-correlation technique to UV spectra obtained from space vehicles would give a new important probe of the structure and composition of planetary atmospheres by enabling the use of the UV spectra of a planet to observe what would normally be an infrared molecular transition.

Cochran, W. D.

Stimulated Raman scattering and the extreme high-velocity H2O maser features in W49

Stimulated Raman scattering of the intense 22.2-GHz water-vapor maser radiation within W49 is examined as a possible explanation of the extremely broad spectrum of W49 extending to + or - 200 km/sec apparent Doppler velocity. Under the most favorable conditions, Raman scattering from ammonia molecules is calculated to be observable. It is unlikely that the Raman process contributes appreciably in the case of W49, as it fails to predict the observed spatial and spectral distribution of the radiation.

Boyd, R. W.

Spontaneous Raman Scattering Diagnostics for High-pressure Gaseous Flames

A high-pressure (up to 60 atm) gaseous burner facility with optical access that provides steady, reproducible flames with high precision, and the ability to use multiple fuel/oxidizer combinations has been developed. In addition, a high-performance spontaneous Raman scattering system for use in the above facility has also been developed. Together, the two systems will be used to acquire and establish a comprehensive Raman scattering spectral database for use as a quantitative high-pressure calibration of single-shot Raman scattering measurements in high-pressure combustion systems. Using these facilities, the Raman spectra of H2-Air flames were successfully measured at pressures up to 20 atm. The spectra demonstrated clear rotational and ro-vibrational Raman features of H2, N2, and H2O. theoretical Raman spectra of pure rotational H2, vibrational H2, and vibrational N2 were calculated using a classical harmonic-oscillator model with pressure broadening effects and fitted to the data. At a gas temperature of 1889 K for a phi = 1.34 H2-Air flame, the model and the data showed good agreement, confirming a ro-vibrational equilibrium temperature.

Kojima, Jun

Analysis of Raman scattered Ly-alpha emissions from the atmosphere of Uranus

A line at 1280 A, due to Raman scattering of solar Lyman alpha (Ly-alpha) in the atmosphere of Uranus, has been detected by the Voyager Ultraviolet Spectrometer. The measured intensity of 40 + or - 20 R implies that 200 R to 500 R of the measured 1500 R Ly-alpha intensity at the subsolar point is due to Rayleigh scattering of the solar line. The presence of Rayleigh and Raman scattering at 1216 A suggests that the Uranian atmosphere is largely devoid of absorbing hydrocarbons above the 0.5 mbar level. The most natural explanation of this depletion is very weak vertical mixing equivalent to an eddy coefficient on the order of 200 sq cm/sec between 0.5 mbar and 100 mbar.

Yelle, R. V.

Raman scattering cross section for N2O4.

Measurement of the Raman scattering cross section for N2O4 at a Raman shift of 7.3 micron, using a Q-switched ruby laser as an excitation source. The cross section for N2 at a Raman shift of 4.3 micron was also measured and compared with the value given by Leonard (1970).

Chen, C. J.

Raman scattering from rapid thermally annealed tungsten silicide

Raman scattering as a technique for studying the formation of tungsten silicide is presented. The tungsten silicide films have been formed by rapid thermal annealing of thin tungsten films sputter deposited on silicon substrates. The Raman data are interpreted by using data from resistivity measurements, Auger and Rutherford backscattering measurements, and scanning electron microscopy.

Kumar, Sandeep

A study of transient stimulated Raman scattering and self-focusing in the picosecond time regime

Two third order processes, stimulated Raman scattering and self-focusing, with picosecond pulses are studied. In the case of transient stimulated scattering, the gain is reduced from the steady state value, and qualitatively new features, such as shortening and delay of the Stokes pulse relative to the laser pulse, appear. These predictions are extended to realistic laser pulses, and experiments confirm all of the theoretical predictions. The self-focusing and frequency broadening of picosecond pulses is studied in the absence of stimulated Raman scattering in several materials with large orientational Kerr constants. Measurements of the relaxation time indicate that the orientational Kerr effect is important in the self-focusing of picosecond pulses. Self-focused filaments are observed to propagate with constant diameters over a distance greater than 10 cm, but disappear before the end of a 20 cm cell. The filaments radiate light continuously along their path and the spectrum of the light shows that the frequency content extends symmetrically for several hundred wave numbers on either side of the laser frequency.

Reintjes, J. F.