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At least 109 records · Page 6

Measurement and Simulation of Spontaneous Raman Scattering Spectra in High-Pressure, Fuel-Rich H2-Air Flames

Rotational vibrational spontaneous Raman spectra (SRS) of H2, N2, and H2O have been measured in H2-air flames at pressures up to 30 atm as a first stem towards establishing a comprehensive Raman spectral database for temperatures and species in high-pressure combustion. A newly developed high-pressure burner facility provides steady, reproducible flames with a high degree of flow precision. We have obtained an initial set of measurements that indicate the spectra are of sufficient quality in terms of spectral resolution, wavelength coverage, and signal-to-noise ratio for use in future reference standards. The fully resolved Stokes and anti-Stokes shifted SRS spectra were collected in the visible wavelength range (400-700 nm) using pulse-stretched 532 nm excitation and a non-intensified CCD spectrograph with a high-speed shutter. Reasonable temperatures were determined via the intensity distribution of rotational H2 lines at stoichiometry and fuel-rich conditions. Theoretical Raman spectra of H2 were computed using a semi-classical harmonic-oscillator model with recent pressure broadening data and were compared with experimental results. The data and simulation indicated that high-J rotational lines of H2 might interfere with the N2 vibrational Q-branch lines, and this could lead to errors in N2-Raman thermometry based on the line-fitting method. From a comparison of N2 Q-branch spectra in lean H2 low-pressure (1.2 atm) and high-pressure (30 atm) flames, we found no significant line-narrowing or -broadening effects at the current spectrometer resolution of 0.04 nm.

Kojima, Jun↗

Lidar Observations of Raman Scattering from S02 in a Power Plant Stack Plume

LIDAR techniques have been successfully applied to the detection of the Raman backscatter from S02 in the plume of a 200 megawatt coal-burning electrical- generating plant from a distance of 210 meters. The LIDAR system used consists of a 61-centimeter-diameter, f /4 Newtonian telescope and a 1.0-1.5-joules per pulse, 1-pulse-per-second ruby laser. Narrow band interference filters are used to select the 7546-angstrom v (sub 1) vibrational line of S02. The signal from a photomultiplier tube was sequentially applied to each 254-nanosecond-wide channel of a 15-cihannel photon counting system, resulting in a direct correlation between channel number and range increment. Photon counts were accumulated from the backscatter of a number of laser pulses (typically 50 or 100), and the accumulated counts per channel printed on paper tape. One sequence of measurements was made during a two-hour period while the plant electrical output was being reduced by approximately 50 percent. Although the Raman system had not been quantitatively calibrated, the LIDAR data correlated well with the varying plant electrical output. N2 scattering observations were also made and an approximate quantitative S02 concentration obtained by ratioing the S02 data to N2 data. This ratio compared well to the in-situ measurements made during the same period by Environmental Protection Agency sampling instruments.

Brumfield, M. L.↗

A tunable line filter polychromator for gas temperature measurements using laser Raman scattering

A proprietary laser line filter spectrograph (LLFS) was modified to test for improved remote measurement of atmospheric temperature by Raman spectroscopy of the rotational bands of N2 and O2. Both grating scan measurements with fixed PMT and polychromator image plane PMT scans with fixed grating setting were made using HeNe and Ar(+) lasers. The LLFS was found to have a laser line rejection ratio at 6A from the laser line and provides resolved rotational Raman spectral display at the polychromator exit plane. Spectral resolution is adequate to measure and correct for background in the Stokes spectrum. It is anticipated that this system should allow measurement of gas or atmospheric temperature to + or - 1 C.

Grossman, J. J.↗

Theoretical studies of Resonance Enhanced Stimulated Raman Scattering (RESRS) of frequency-doubled Alexandrite laser wavelength in cesium vapor

The solutions for the imaginary susceptibility of the Raman field transition with arbitrary relaxation rates and field strengths are examined for three different sets of relaxation rates. These rates correspond to: (1) Far Infrared (FIR) Raman lasers in the diabatic collision regime without consideration of coupled population decay in a closed system, (2) Raman FIR lasers in the diabatic collision regime with coupled population conserving decay, and (3) IR Raman gain in cesium vapor. The model is further expanded to include Doppler broadening and used to predict the peak gain as a function of detuning for a frequency doubled Alexandrite laser-pumped cesium vapor gain cell.

Lawandy, Nabil M.↗

Coherent Anti-Stokes Raman Scattering (CARS) as a Probe for Supersonic Hydrogen-Fuel/Air Mixing

The dual-pump coherent anti-Stokes Raman spectroscopy (CARS) method was used to measure temperature and the absolute mole fractions of N2, O2 and H2 in a supersonic non-reacting fuel-air mixing experiment. Experiments were conducted in NASA Langley Research Center s Direct Connect Supersonic Combustion Test Facility. Under normal operation of this facility, hydrogen and air burn to increase the enthalpy of the test gas and O2 is added to simulate air. This gas is expanded through a Mach 2 nozzle and into a combustor model where fuel is then injected, mixes and burns. In the present experiment the O2 of the test gas is replaced by N2. The lack of oxidizer inhibited combustion of the injected H2 fuel jet allowing the fuel/air mixing process to be studied. CARS measurements were performed 427 mm downstream of the nozzle exit and 260 mm downstream of the fuel injector. Maps were obtained of the mean temperature, as well as the N2, O2 and H2 mean mole fraction fields. A map of mean H2O vapor mole fraction was also inferred from these measurements. Correlations between different measured parameters and their fluctuations are presented. The CARS measurements are compared with a preliminary computational prediction of the flow.

Danehy, P. M.↗

Raman Scattering from Atmospheric Nitrogen in the Stratosphere

The Mark II laser radar system at Kingston, Jamaica, has been used to make observations on the Raman shifted line from atmospheric nitrogen at 828.5 nm. The size of the system makes it possible to detect signals from heights of up to 40 kilometres. The effects of aerosol scattering observed using a single wavelength are almost eliminated, and a profile of nitrogen density may be obtained. Assuming a constant mixing ratio, this may be interpreted as a profile of atmospheric density whose accuracy is comparable to that obtained from routine meteorological soundings. In order to obtain an accurate profile several interfering effects have had to be examined and, where necessary, eliminated. These include: 1) Fluorescence in optical components 2) Leakage of signal at 694.3 nm. 3) Overload effects and non-linearities in the receiving and counting electronics. Most of these effects have been carefully examined and comparisons are being made between the observed atmospheric density profiles and local meteorological radio-sonde measurements. Good agreement has been obtained over the region of overlap (15 - 30 KID), discrepancies being of the same order as the experimental accuracy (1-10%), depending on height and length of period of observation.

Garvey, M. J.↗

Remote measurement of ocean temperature from depolarization in Raman scattering

Ocean temperatures may be mapped in three dimensions from an aircraft down to depths of 2 to 4 attenuation lengths by monitoring Raman radiation backscattered from a laser beam. This paper describes laboratory experiments on the temperature dependence of Raman spectra of saline solutions and calculations of the expected performance of a field system. The Raman technique is of greatest potential utility in coastal and estuarine waters where gradients are relatively high. It is estimated that seawater temperature may be measured to a statistical precision of 0.5 C at depths to four attenuation lengths in two meter water, using one Joule of transmitted laser energy.

Chang, C. H.↗

Coherent Anti-Stokes Raman scattering with reflective optics

Attention is given to the implementation of a novel reflective optics configuration in which the lens normally employed for focusing and crossing the input laser beams in Coherent Anti-Stokes Raman spectroscopy (CARS) is replaced by a spherical mirror, allowing large crossing angles to be obtained with a single focusing device and permitting the laser generation and collection equipment to be located on one side of the sample region. The experimental results obtained demonstrate the feasibility of mirror-based CARS in remote combustion diagnostics.

Antcliff, R. R.↗

Theoretical studies of Resonance Enhance Stimulated Raman Scattering (RESRS) of frequency doubled Alexandrite laser wavelengths in cesium vapor

It is well known that the presence of a real atomic level which is nearly resonant with the pump field can greatly enhance the Raman emission cross section. In order to accurately calculate the Raman gain in systems where resonance enhancement plays a dominant role, expressions for the pump and signal susceptibilities must be derived. These expressions should be valid for arbitrary field strengths in order to allow for pump and signal saturation. In addition, the theory should allow for arbitrary longitudinal and transverse relaxation rates. This latter point is extremely vital for three level atomic systems such as the alkali earth metals since they do not have population reservoirs and can have widely varying spontaneous lifetimes on the three pertinent transitions. Moreover, the dephasing rates are strong functions of electron states and are therefore also different for the three coupled pairs of levels. These considerations are not as important when molecular systems are concerned since the large reservoir of rotational states serve to produce essentially equal longitudinal recovery rates for the population of the three levels. The three level system with three arbitrary longitudinal and transverse relaxation rates was solved. There is no need for setting either pair of rates equal and the expressions are valid for arbitrarily strong fields.

Lawandy, N. M.↗

The use of the transmission windows of the Fabry-Perot interferometer in the detection of Raman scattered radiation from atmospheric gases.

Demonstration that the use of the Fabry-Perot interferometer as a filter with transmission windows occurring at regular intervals in wave numbers provides a highly sensitive method for detection of atmospheric gases using their rotational Raman spectra excited by a suitable laser. Some of the operating advantages include signal gains of several orders of magnitude, a simple direct interpretation of the results in terms of the density and types of the gaseous constituents, size and weight reductions from conventional apparatus, ease of operation, and relative freedom from interference from other molecules in the scattering volume. This method is compared with the techniques that have been discussed in the literature by other workers in the field.

Smith, W. H.↗

Raman scattering of InGaAs/InP grown by uniform radial flow epitaxy

Uniform radial flow epitaxy, a novel growth technique, has been used to grown InGaAs films on InP. Epitaxial layers above and below the critical thickness for the onset of slip were grown. Raman spectroscopy was used to characterize the quality of epitaxial layers, determine alloy composition, and measure the strain. Raman spectra from both pseudomorphic (strained) and relaxed (unstrained) InGaAs films were obtained at 300 and 80 K. The difference in the frequencies of their GaAs-like longitudinal optical phonons was used to calculate stress for the strained InGaAs/InP, leading to a direct formula for the evaluation of the layer stress.

Feng, Z. C.↗

Raman Scattering in a New Carbon Material

Samples of a new carbon material, Diamonite-B, were fabricated under high pressure from a commercial carbon black--identified as mixed fullerenes. The new material is neither graphite-like nor diamond-like, but exhibits electrical properties close to graphite and mechanical properties close to diamond. The use of Raman spectroscopy to investigate the vibrational dynamics of this new carbon material and to provide structural characterization of its short-, medium- and long-range order is reported. We also provide the results of investigations of these samples by high-resolution electron microscopy and X-ray diffraction. Hardness, electrical conductivity, thermal conductivity and other properties of this new material are compared with synthetic graphite-like and diamond-like materials, two other phases of synthetic bulk carbon.

Voronov, O. A.↗

Species and temperature measurement in H2/O2 rocket flow fields by means of Raman scattering diagnostics

Validation of CFD codes developed for prediction and evaluation of rocket performance is hampered by a lack of experimental data. Nonintrusive laser based diagnostics are needed to provide spatially and temporally resolved gas dynamic and fluid dynamic measurements. This paper reports the first nonintrusive temperature and species measurements in the plume of a 110 N gaseous hydrogen/oxygen thruster at and below ambient pressures, obtained with spontaneous Raman spectroscopy. Measurements at 10 mm downstream of the exit plane are compared with predictions from a numerical solution of the axisymmetric Navier-Stokes and species transport equations with chemical kinetics, which fully model the combustor-nozzle-plume flowfield. The experimentally determined oxygen number density at the centerline at 10 mm downstream of the exit plane is four times that predicted by the model. The experimental number density data fall between those numerically predicted for the exit and 10 mm downstream planes in both magnitude and radial gradient. The predicted temperature levels are within 10 to 15 percent of measured values.

De Groot, Wim A.↗

Picosecond coherent anti-Stokes Raman scattering (CARS) study of vibrational dephasing of carbon disulfide and benzene in solution

The vibrational dephasing of the 656/cm mode (nu1, a1g) of CS2 and the 991/cm mode (nu2, a1g) of benzene have been studied as a function of concentration in mixtures with a number of solvents using a ps time-resolved CARS technique. This technique employs two tunable synchronously-pumped mode-locked dye lasers in a stimulated Raman pump, coherent anti-Stokes Raman probe time-resolved experiment. Results are obtained for CS2 in carbon tetrachloride, benzene, nitrobenzene, and ethanol and for benzene nu2 in CS2. The dephasing rates of CS2 nu1 increase on dilution with the polar solvents and decrease or remain constant on dilution with the nonpolar solvents. The CS2/benzene solutions show a contrasting behavior, with the CS2 nu1 dephasing rate being nearly independent of concentration whereas the benzene nu2 dephasing rate decreases on dilution. These results are compared to theoretical models for vibrational dephasing of polyatomic molecules in solution.

Perry, Joseph W.↗

Species and temperature measurement in H2/O2 rocket flow fields by means of Raman scattering diagnostics

Validation of Computational Fluid Dynamics (CFD) codes developed for prediction and evaluation of rocket performance is hampered by a lack of experimental data. Non-intrusive laser based diagnostics are needed to provide spatially and temporally resolved gas dynamic and fluid dynamic measurements. This paper reports the first non-intrusive temperature and species measurements in the plume of a 110 N gaseous hydrogen/oxygen thruster at and below ambient pressures, obtained with spontaneous Raman spectroscopy. Measurements at 10 mm downstream of the exit plane are compared with predictions from a numerical solution of the axisymmetric Navier-Stokes and species transport equations with chemical kinetics, which fully model the combustor-nozzle-plume flowfield. The experimentally determined oxygen number density at the centerline at 10 mm downstream of the exit plane is four times that predicted by the model. The experimental number density data fall between those numerically predicted for the exit and 10 mm downstream planes in both magnitude and radial gradient. The predicted temperature levels are within 10 to 15 percent of measured values. Some of the discrepancies between experimental data and predictions result from not modeling the three dimensional core flow injection mixing process, facility back pressure effects, and possible diffuser-thruster interactions.

Degroot, Wim A.↗

Theoretical studies of Resonance Enhanced Stimulated Raman Scattering (RESRS) of frequency doubled Alexandrite laser wavelength in cesium vapor

The third phase of research will focus on the propagation and energy extraction of the pump and SERS beams in a variety of configurations including oscillator structures. In order to address these questions a numerical code capable of allowing for saturation and full transverse beam evolution is required. The method proposed is based on a discretized propagation energy extraction model which uses a Kirchoff integral propagator coupled to the three level Raman model already developed. The model will have the resolution required by diffraction limits and will use the previous density matrix results in the adiabatic following limit. Owing to its large computational requirements, such a code must be implemented on a vector array processor. One code on the Cyber is being tested by using previously understood two-level laser models as guidelines for interpreting the results. Two tests were implemented: the evolution of modes in a passive resonator and the evolution of a stable state of the adiabatically eliminated laser equations. These results show mode shapes and diffraction losses for the first case and relaxation oscillations for the second one. Finally, in order to clarify the computing methodology used to exploit the speed of the Cyber's computational speed, the time it takes to perform both of the computations previously mentioned to run on the Cyber and VAX 730 must be measured. Also included is a short description of the current laser model (CAVITY.FOR) and a flow chart of the test computations.

Lawandy, Nabil M.↗

Theoretical studies of Resonance Enhanced Stimulated Raman Scattering (RESRS) of frequency doubled Alexandrite laser wavelengths in cesium vapor

This work focused on understanding the effects of arbitrary transverse and longitudinal relaxation rates on the susceptibilities of coherently driven three-level systems. The approximation of a single relaxation rate often made in previous work is strongly invalidated by the variation in the spontaneous emission lifetime between various atomic level pairs in systems such as cesium. It is of great importance to the problem of nonlinear infrared generation to determine the dependence of both real and imaginary susceptibility on relaxation rates. The imaginary susceptibility on the pump transition determines the absorption of pump photons and the imaginary susceptibility on the laser transition determines the spectral dependence of the gain. This is of particular importance for pure Raman emission (i.e., absorption at linecenter of the gain transition) as it determines the tunability characteristics we are aiming to predict. The real susceptibility is important when cavities are used at the signal field as this will determine the loaded resonance of the Raman oscillator. Researchers show that in some cases which result from having different relaxation rates mode splitting may result, allowing more than one frequency to have the same Raman wavelength, possibly resulting in a temporal instability.

Lawandy, N. M.↗

Spontaneous Raman Scattering Diagnostics: Applications in Practical Combustion Systems

In this chapter, the recent advancements and practical aspects of laser SRS diagnostics have been reviewed wi til regards to applications in practical combustion systems. Clearly, SRS represents a theoretically and experimentally mature diagnostic technology that has become an essential tool for multiscalar measurements in turbulent combustion at elevated pressures. Today, time-, space-, spectrally, and even polarization-resolved S RS diagnostics is at hand, with aid from recent innovations in theoretical and technological developments on electro-optical or electromechanical devices. Whilst a linear increase in SRS signals can be expected in high-pressure systems (this is perhaps one of the most important advantages for using SRS in high-pressure systems), there are practical (often severe) restrictions associated with pressurized vessels, due mainly to the limited degree of optical access. This narrows ti,e available choice of diagnostics that can be employed at any given time. Point-wise SRS diagnostics provides the highest accuracy on the chemical species and temperature measurements, and will continue to remain a vital approach for the study in such harsh environments. The practical design considerations and hands-on set-up guide for SRS diagnostics provided in this chapter are rarely presented elsewhere. Although the second-harmonic Nd:YAG pulsed laser (532 nm), combined with pulse-stretching optics or the recently introduced White Cell-based laser, seems to be the most favored excitation source of choice by the research community, UV excitation will undoubtedly continue to be used on many occasions, and especially in sooting flames. Detection methods may be divided into ICCD-based nanosecond-gate detection or a rotary-chopper electromechanical shutter-based CCD array detection, and the levels of background flame emission in individual cases would determine this critical design choice. Here, a process of Raman signal calibration based on ti,e crosstalk matrix formalism was explained step-by-step. As tI,is process may be very time-consuming and expensive, a well-planned experimental approach (01' building a transferable calibration database or library (at least with in a user's own facility over a series of different testing and runs) is vitally important. Hands on advice on the design and construction of flow control systems for high pressure burner facilities were also presented.

Kojima, Jun↗