Search NASA⌕ Search

SEARCH · Search NASA

Results for “collisional broadening”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 37 records · Page 2

Kinetic Temperature and Electron Density Measurement in an Inductively Coupled Plasma Torch using Degenerate Four-Wave Mixing

Laser wave mixing is presented as an effective technique for spatially resolved kinetic temperature measurements in an atmospheric-pressure radio-frequency inductively-coupled plasma. Measurements are performed in a 1 kW, 27 MHz RF plasma using a continuous-wave, tunable 811.5-nm diode laser to excite the 4s(sup 3)P2 approaches 4p(sup 3)D3 argon transition. Kinetic temperature measurements are made at five radial steps from the center of the torch and at four different torch heights. The kinetic temperature is determined by measuring simultaneously the line shape of the sub-Doppler backward phase-conjugate degenerate four-wave mixing and the Doppler-broadened forward-scattering degenerate four-wave mixing. The temperature measurements result in a range of 3,500 to 14,000 K+/-150 K. Electron densities measured range from 6.1 (+/-0.3) x 10(exp 15)/cu cm to 10.1 (+/-0.3) x 10(exp 15)/cu cm. The experimental spectra are analyzed using a perturbative treatment of the backward phase-conjugate and forward-geometry wave-mixing theory. Stark width is determined from the collisional broadening measured in the phase-conjugate geometry. Electron density measurements are made based on the Stark width. The kinetic temperature of the plasma was found to be more than halved by adding deionized water through the nebulizer.

Schafer, Julia↗

Ultraviolet spectroscopy of pressurized and supercritical carbon dioxide

Abstract Carbon dioxide (CO 2 ) is prevalent in planetary atmospheres and sees use in a variety of industrial applications. Despite its ubiquitous nature, its photochemistry remains poorly understood. In this work we explore the density dependence of pressurized and supercritical CO 2 electronic absorption spectra by vacuum ultraviolet spectroscopy over the wavelength range 1455-2000 Å. We show that the lowest absorption band transition energy is unaffected by a density increase up to and beyond the thermodynamic critical point (137 bar, 308 K). However, the diffuse vibrational structure inherent to the spectrum gradually decreases in magnitude. This effect cannot be explained solely by collisional broadening and/or dimerization. We suggest that at high densities close proximity of neighboring CO 2 molecules with a variety of orientations perturbs the multiple monomer electronic state potential energy surfaces, facilitating coupling between binding and dissociative states. We estimate a critical radius of ~4.1 Å necessary to cause such perturbations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Fully quantum calculations of O 2 –N 2 scattering using a new potential energy surface: Collisional perturbations of the oxygen 118 GHz fine structure line

A proper description of the collisional perturbation of the shapes of molecular resonances is important for remote spectroscopic studies of the terrestrial atmosphere. Of particular relevance are the collisions between the $\text{O}_2$ and $\text{N}_2$ molecules—the two most abundant atmospheric species. In this work, we report a new highly accurate $\text{O}_2(\text{X}^3Σ^–_g)–\text{N}_2(\text{X}^1Σ^+_g)$ potential energy surface and use it for performing the first quantum scattering calculations addressing line shapes for this system. We use it to model the shape of the 118 GHz fine structure line in $\text{O}_2$ perturbed by collisions with $\text{N}_2$ molecules, a benchmark system for testing our methodology in the case of an active molecule in a spin triplet state. The calculated collisional broadening of the line agrees well with the available experimental data over a wide temperature range relevant for the terrestrial atmosphere. This work constitutes a step toward populating the spectroscopic databases with ab initio line shape parameters for atmospherically relevant systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Amplified spontaneous emission in the extreme ultraviolet by expanding xenon clusters

Focused short-wavelength free-electron laser (FEL) pulses interacting with gas phase samples can induce by inner-shell ionization a short-lived population inversion, followed by coherent collective emission of directed, short, and strong radiation bursts. We extend our studies into the warm-dense matter (WDM) regime by investigating the nanoplasmas produced in an ensemble of nanometer-sized clusters by FEL irradiation. Here, additional pathways can also lead to strong, laserlike emission: Electron-ion collisions can yield a long-lived population inversion, and subsequent amplified spontaneous emission. We observe amplified spontaneous emission (ASE) in the extreme ultraviolet in xenon clusters excited by soft x-ray FEL pulses, we diagnose the generated nanoplasmas by fluorescence spectroscopy, and we study under various cluster and FEL parameters the directed ASE from the Xe 2+ 65 nm line. We show its exponential increase as a function of FEL irradiation power, and an accompanying collisional broadening of the emission spectra. These findings are corroborated by extensive numerical simulations based on theory, combining detailed hydrodynamic and kinetic simulations with time-dependent calculations of radiation transport, amplification, and collective emission in the WDM nanoplasma. Furthermore, our theoretical findings underline that population inversion is due to electron-ion collisions and that the observed decoherence processes can be empirically characterized by a phenomenological decoherence time in the range of 100–200 fs.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

High resolution absorption coefficients for Freon-12

The ultra high resolution absorption coefficients of the Q-branch of Freon-12 obtained with tunable diode laser spectroscopy are presented. Continuous spectra are presented from 1155/cm to 1163/cm, and absolute wavelength calibration was obtained using SO2 spectra as a standard and a 5 cm Ge etalon for relative calibration between SO2 lines. The Freon-12 data obtained at a pressure of 0.05 torr showed a rich and highly structured spectra, but with the exception of three isolated features, collisional broadening reduces the spectra to a structureless continuum for nitrogen pressures greater than 20 torr. The spectra at 1161/cm continue to exhibit structure at atmospheric pressure.

Hoell, J. M.↗

Photoexcitation of lasers and chemical reactions for NASA missions: A theoretical study

The possibility of obtaining CW laser oscillation by optical pumping in the infrared at an elevated gas pressure is reviewed. A specific example utilizing a mixture of CO and NO gases is included. The gas pressures considered are in excess of several atmospheres. Laser frequency tuning over a broad region becomes possible at such elevated gas pressures due to collisional broadening of the amplifying transitions. The prior-rate and surprisal analysis are applied to obtain detailed VV and VT rates for CO and NO molecules and the transfer rates in a CO-NO gas mixture. The analysis is capable of giving temperature dependence of the rate constants. Computer estimates of the rates are presented for vibrational levels up to v = 50. The results show that in the high-lying vibrational states the VV transfer rates with Delta nu = 2 become appreciable.

Javan, A.↗

Investigation of laser-induced iodine fluorescence for the measurement of density in compressible flows

Laser induced fluorescence is an attractive nonintrusive approach for measuring molecular number density in compressible flows although this technique does not produce a signal that is directly related to the number density. Saturation and frequency detuned excitation are explored as means for minimizing the quenching effect using iodine as the molecular system because of its convenient absorption spectrum. Saturation experiments indicate that with available continuous wave laser sources of Gaussian transverse intensity distribution only partial saturation could be achieved in iodine at the pressures of interest in gas dynamics. Using a fluorescence lineshape theory, it is shown that for sufficiently large detuning of a narrow bandwidth laser from a molecular transition, the quenching can be cancelled by collisional broadening over a large range of pressures and temperatures. Experimental data obtained in a Mach 4.3 underexpanded jet of nitrogen seeded with iodine for various single mode argon laser detunings from a strong iodine transition at 5145 A are discussed.

Mcdaniel, J. C., Jr.↗

Raman-shifted dye laser for water vapor DIAL measurements

For improved DIAL measurements of water vapor in the upper troposphere or lower stratosphere, narrowband (about 0.03/cm) laser radiation at 720- and 940-nm wavelengths was generated by stimulated Raman scattering (SRS), using the narrow linewidth (about 0.02/cm) output of a Nd:YAG-pumped dye laser. For a hydrogen pressure of 350 psi, the first Stokes conversion efficiencies to 940 nm were 20 percent and 35 percent, when using a conventional and waveguide Raman cell, respectively. The linewidth of the first Stokes line at high cell pressures, and the inferred collisional broadening coefficients, agree well with those previously measured in spontaneous Raman scattering.

Grossmann, B. E.↗

Computer processing of tunable diode laser spectra

A computer-controlled tunable diode laser spectrometer and spectral analysis software are described. The three-channel system records simultaneously the transmission of a subject gas, a temperature-stabilized etalon, and a calibration gas. The software routines are applied to diode laser spectra of HNO3 and NO2 to illustrate the procedures adopted for conversion of raw spectral data to useful transmission and harmonic spectra. Extraction of line positions, absorption intensities, collisional broadening coefficients, and gas concentrations from recorded spectra is also described.

May, Randy D.↗

Simultaneous measurements of velocity, temperature, and pressure using rapid CW wavelength-modulation laser-induced fluorescence of OH

The beam from a rapid-tuning single-frequency laser was used to probe the R1(7) and R1(11) A2Sigma(+) - X2Pi(0,0) line pair of OH at a 45-deg incident angle in a combustion-driven, supersonic free jet. Absorption line shapes were recorded in spatially resolved, single-point fluorescence. The Doppler shift, intensity ratio, and collisional broadening of the measured line pair were used to determine velocity, temperature, and pressure. The repetition rate of the measurement was 3 kHz.

Chang, A. Y.↗

Continuous wave laser absorption techniques for gasdynamic measurements in supersonic flows

Line-of-sight measurements of velocity, temperature, pressure, density, and mass flux were performed in a transient shock tube flow using three laser absorption schemes. All methods employed an intracavity-doubled ring dye laser tuned to an OH transition at 306 nm. In the first scheme, the gas was labeled by 193.3-nm excimer photolysis of H2O, and the passage of the generated OH was detected downstream. In the second method, the laser was tuned at a rate of 3 kHz over the R1(7) and R1(11) line pair, and absorption was simultaneously monitored at 90 and 60 deg with respect to the flow. Velocity was determined from the Doppler shift of the profiles and the temperature from the intensity ratio of the lines. Pressure was determined from both the magnitude of absorption and the collisional broadening. In the third method, the laser wavelength was fixed at a single frequency, and a continuous measurement of velocity and pressure was obtained using the signals from the two beam paths. All methods gave results which compare favorably to calculated values.

Davidson, David F.↗

Rapid tuning CW laser technique for measurements of gas velocity, temperature, pressure, density, and mass flux using NO

An intracavity-doubled rapid-tuning CW ring dye laser was used to acquire fully resolved absorption profiles of NO line pairs in the A-X band at 225 nm at a rate of 4 kHz. These profiles were utilized for simultaneous measurements of flow parameters in the high-speed 1D flows generated in a shock tube. Velocity was determined from the Doppler shift, measured using a pair of profiles simultaneously acquired at different angles with respect to the flow direction. Temperature was determined from the intensity ratio of the adjacent lines. Pressure and density were found both from the collisional broadening and the fractional absorption. From this information the mass flux was determined. The results compare well to 1D shock calculations.

Chang, Albert Y.↗

Nonintrusive, multipoint velocity measurements in high-pressure combustion flows

A combined experimental and analytical effort was conducted to demonstrate the applicability of OH Doppler-shifted fluorescence imaging of velocity distributions in supersonic combustion gases. The experiments were conducted in the underexpanded exhaust flow from a 6.8 atm, 2400 K, H2-O2-N2 burner exhausting into the atmosphere. In order to quantify the effects of in-plane variations of the gas thermodynamic properties on the measurement accuracy, a set of detailed measurements of the OH (1,0) band collisional broadening and shifting in H2-air gases was produced. The effect of pulse-to-pulse variations in the dye laser bandshape was also examined in detail and a modification was developed which increased in the single pulse bandwidth, thereby increasing the intraimage velocity dynamic range as well as reducing the sensitivity of the velocity measurement to the gas property variations. Single point and imaging measurements of the velocity field in the exhaust flowfield were compared with 2D, finite-rate kinetics simulations of the flowfield. Relative velocity accuracies of +/- 50 m/s out of 1600 m/s were achieved in time-averaged imaging measurements of the flow over an order of magnitude variation in pressure and a factor of two variation in temperature.

Allen, M.↗

Instantaneous velocity field imaging instrument for supersonic reacting flows

The technical tasks conducted to develop and demonstrate a new gas velocity measurement technique for high enthalpy reacting flows is described. The technique is based on Doppler-shifted Planar Laser-induced Fluorescence (PLIF) imaging of the OH radical. The imaging approach permits, in principle, single-shot measurements of the 2-D distribution of a single velocity component in the measurement plane, and is thus a technique of choice for applications in high enthalpy transient flow facilities. In contrast to previous work in this area, the present program demonstrated an approach which modified the diagnostic technique to function under the constraints of practical flow conditions of engineering interest, rather than vice-versa. In order to accomplish the experimental demonstrations, the state-of-the-art in PLIF diagnostic techniques was advanced in several ways. Each of these tasks is described in detail and is intended to serve as a reference in supporting the transition of this new capability to the fielded PLIF instruments now installed at several national test facilities. Among the new results of general interest in LlF-based flow diagnostics, a detailed set of the first measurements of the collisional broadening and shifting behavior of OH (1,0) band transitions in H7-air combustion environments is included. Such measurements are critical in the design of a successful strategy for PLIF velocity imaging; they also relate to accurate concentration and temperature measurements, particularly in compressible flow regimes. Furthermore, the results shed new light on the fundamental relationship between broadening and energy transfer collisions in OH A(sup 2)Sigma(+)v(sup ') = 1. The first single-pulse, spectrally-resolved measurements of the output of common pulsed dye lasers were also produced during the course of this effort. As with the OH broadening measurements, these data are a significant aspect of a successful velocity imaging strategy, and also have potential implications for many other LIF measurement techniques. Our results indicated the need to modify the commercially available laser cavity in order to accommodate the constraints imposed by typical SCRAMJET combustion characteristics as well as to increase the instrument's velocity dynamic range to span an intra-image range in excess of 2 km/s. The various technical efforts were brought together in a series of experiments demonstrating the applicability of the technique in a high pressure, high temperature H2-air combustion system. The resultant images were compared with 2-D flow simulations in order to determine the accuracy of the instrument. Mean velocity imaging in flows with an axis of symmetry was demonstrated with an accuracy of +/- 50 m/s out of an intra-image dynamic range of 1600 m/s, including reversed flow. A more complex configuration amenable to single-shot imaging in flows without an axis of symmetry was also demonstrated. Limitations imposed by available equipment resulted in an accuracy of about +/- 200 m/s out of 1750 m/s in these demonstrations. Minor modifications to the present configuration were suggested to improve this performance. Each technical task is described in detail, along with significance of the results for the overall imaging velocimeter configuration. This report should allow the user community to integrate this new measurement capability in their existing instrumentation platforms.

Allen, M. G.↗

Measuring Rocket Engine Temperatures with Hydrogen Raman Spectroscopy

Laser-based combustion diagnostics, such as single-pulse UV Raman spectroscopy and visible Raman spectroscopy, have been successfully applied to optically-accessible rocket-like test articles. If an independent pressure measurement is available, Raman major species concentration measurements can also provide a temperature measurement. However it is desirable to obtain a Raman-derived temperature measurement without the need for simultaneous pressure measurement, especially when chamber pressure may vary spatially. This report describes Raman temperature measurements obtained by exploiting the variation in shape of the H2 Raman spectrum. Hydrogen is advantageous since it is ubiquitous in H2-O2 systems and its Raman spectrum is simpler than for other diatomics. However the influence of high pressure on the H2 Raman spectrum must be investigated. At moderate pressures, well below those of rocket engines, the Raman spectra of O2 and N2 are known to become featureless due to collisional broadening.

Joseph A Wehrmeyer↗

Quantitative Analysis of Spectral Interference of Spontaneous Raman Scattering in High-Pressure Fuel-Rich H2-Air Combustion

We present a theoretical study of the spectral interferences in the spontaneous Raman scattering spectra of major combustion products in 30-atm fuel-rich hydrogen-air flames. An effective methodology is introduced to choose an appropriate line-shape model for simulating Raman spectra in high-pressure combustion environments. The Voigt profile with the additive approximation assumption was found to provide a reasonable model of the spectral line shape for the present analysis. The rotational/vibrational Raman spectra of H2, N2, and H2O were calculated using an anharmonic-oscillator model using the latest collisional broadening coefficients. The calculated spectra were validated with data obtained in a 10-atm fuel-rich H2-air flame and showed excellent agreement. Our quantitative spectral analysis for equivalence ratios ranging from 1.5 to 5.0 revealed substantial amounts of spectral cross-talk between the rotational H2 lines and the N2 O-/Q-branch; and between the vibrational H2O(0,3) line and the vibrational H2O spectrum. We also address the temperature dependence of the spectral cross-talk and extend our analysis to include a cross-talk compensation technique that removes the nterference arising from the H2 Raman spectra onto the N2, or H2O spectra.

Kojima, Jun↗

Pressure Monitoring Using Hybrid fs/ps Rotational CARS

We investigate the feasibility of gas-phase pressure measurements at kHz-rates using fs/ps rotational CARS. Femtosecond pump and Stokes pulses impulsively prepare a rotational Raman coherence, which is then probed by a high-energy 6-ps pulse introduced at a time delay from the Raman preparation. Rotational CARS spectra were recorded in N2 contained in a room-temperature gas cell for pressures from 0.1 to 3 atm and probe delays ranging from 10-330 ps. Using published self-broadened collisional linewidth data for N2, both the spectrally integrated coherence decay rate and the spectrally resolved decay were investigated as means for detecting pressure. Shot-averaged and single-laser-shot spectra were interrogated for pressure and the accuracy and precision as a function of probe delay and cell pressure are discussed. Single-shot measurement accuracies were within 0.1 to 6.5% when compared to a transducer values, while the precision was generally between 1% and 6% of measured pressure for probe delays of 200 ps or more, and better than 2% as the delay approached 300 ps. A byproduct of the pressure measurement is an independent but simultaneous measurement of the gas temperature.

Kearney, Sean P.↗