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At least 145 records · Page 8

Low-Temperature Rate Coefficients of C2H with CH4 and CD4 from 154 to 359 K

Rate coefficients for the reaction C2H + CH4 yields C2H2 + CH3 and C2H + CD4 yields C2HD + CD3 are measured over the temperature range 154-359 K using transient infrared laser absorption spectroscopy. Ethynyl radicals are produced by pulsed laser photolysis of C2H2 in a variable temperature flow cell, and a tunable color center laser probes the transient removal of C2H (Chi(exp 2) Sigma(+) (0,0,0)) in absorption. The rate coefficients for the reactions of C2H with CH4 and CD4 both show a positive temperature dependence over the range 154-359 K, which can be expressed as k(sub CH4) = (1.2 +/- 0.1) x 10(exp -11) exp((-491 +/- 12)/T) and k(sub CD4) = (8.7 +/- 1.8) x 10(exp -12) exp((-650 +/- 61)/T) cm(exp 3) molecule(exp -1) s(exp -1), respectively. The reaction of C2H + CH4 exhibits a significant kinetic isotope effect at 300 K of k(sub CH4)/k(sub CD4) = 2.5 +/- 0.2. Temperature dependent rate constants for C2H + C2H2 were also remeasured over an increased temperature range from 143 to 359 K and found to show a slight negative temperature dependence, which can be expressed as k(sub C2H2) = 8.6 x 10(exp -16) T(exp 1.8) exp((474 +/- 90)/T) cm(exp 3) molecule(exp -1) s(exp -1).

Opansky, Brian J.↗

Rate Coefficients of C2H with C2H4, C2H6, and H2 from 150 to 359 K

Rate coefficients for the reactions C2H with C2H4, C2H6, and H2 are measured over the temperature range 150-359 K using transient infrared laser absorption spectroscopy. The ethynyl radical is formed by photolysis of C2H2 with a pulsed excimer laser at 193 nm, and its transient absorption is monitored with a color center laser on the Q(sub 11)(9) line of the A(sup 2) Pi-Chi(sup 2) Sigma transition at 3593.68 cm(exp -1). Over the experimental temperature range 150-359 K the rate constants of C2H with C2H4, C2H6, and H2 can be fitted to the Arrhenius expressions k(sub C2H4) = (7.8 +/- 0.6) x 10(exp -11) exp[(134 +/- 44)/T], k(sub C2H6) = (3.5 +/- 0.3) x 10(exp -11) exp[(2.9 +/- 16)/T], and k(sub H2) = (1.2 +/- 0.3) x 10(exp -11) exp[(-998 +/- 57)]/T cm(exp 3) molecule(exp -1) sec(exp -1). The data for C2H with C2H4 and C2H6 indicate a negligible activation energy to product formation shown by the mild negative temperature dependence of both reactions. When the H2 data are plotted together with the most recent high-temperature results from 295 to 854 K, a slight curvature is observed. The H2 data can be fit to the non-Arrhenius form k(sub H2) = 9.2 x 10(exp -18) T(sup 2.17 +/- 0.50) exp[(-478 +/- 165)/T] cm(exp 3) molecules(exp -1) sec(exp -1). The curvature in the Arrhenius plot is discussed in terms of both quantum mechanical tunneling of the H atom from H2 to the C2H radical and bending mode contributions to the partition function.

Opansky, Brian J.↗

Scramjet Performance Assessment Using Water Absorption Diagnostics (U)

Simultaneous multiple path measurements of temperature and H2O concentration will be presented for the AIMHYE test entries in the NASA Ames 16-Inch Shock Tunnel. Monitoring the progress of high temperature chemical reactions that define scramjet combustor efficiencies is a task uniquely suited to nonintrusive optical diagnostics. One application strategy to overcome the many challenges and limitations of nonintrusive measurements is to use laser absorption spectroscopy coupled with optical fibers. Absorption spectroscopic techniques with rapidly tunable lasers are capable of making simultaneous measurements of mole fraction, temperature, pressure, and velocity. The scramjet water absorption diagnostic was used to measure combustor efficiency and was compared to thrust measurements using a nozzle force balance and integrated nozzle pressures to develop a direct technique for evaluating integrated scramjet performance. Tests were initially performed with a diode laser tuning over a water absorption feature at 1391.7 nm. A second diode laser later became available at a wavelength near 1343.3 nm covering an additional water absorption feature and was incorporated in the system for a two-wavelength technique. Both temperature and mole fraction can be inferred from the lineshape analysis using this approach. Additional high temperature spectroscopy research was conducted to reduce uncertainties in the scramjet application. The lasers are optical fiber coupled to ports at the combustor exit and in the nozzle region. The output from the two diode lasers were combined in a single fiber, and the resultant two-wavelength beam was subsequently split into four legs. Each leg was directed through 60 meters of optical fiber to four combustor exit locations for measurement of beam intensity after absorption by the water within the flow. Absorption results will be compared to 1D combustor analysis using RJPA and nozzle CFD computations as well as to data from a nozzle metric balance measuring thrust and integrated pressure measurements along the length of the nozzle. Assessment of its value as a combustor performance evaluation tool will be conducted.

Cavolowsky, John A.↗

NASA participation in the 1980 Persistent Elevated Pollution Episode/Northeast Regional Oxidant Study (PEPE/NROS) Project: Operational aspects

A field experiment designed to further understand the formation and transport of visibility reducing aerosols and to characterize regional scale air masses and urban plumes is described. Measurements were made primarily in the Ohio River Valley region. The NASA participation included obtaining measurements for the determination of mixing layer height and ozone profiles by using airborne remote sensor systems such as the ultraviolet differential absorption lidar, the high spectral resolution lidar, and the laser absorption spectrometer. Other NASA systems included the microwave atmospheric remote sensor, tethered balloons, an in situ measurements aircraft, and several photometer/transmissiometer systems.

Maddrea, G. L., Jr.↗

Pseudorandom Noise Code-Based Technique for Thin Cloud Discrimination with CO2 and O2 Absorption Measurements

NASA Langley Research Center is working on a continuous wave (CW) laser based remote sensing scheme for the detection of CO2 and O2 from space based platforms suitable for ACTIVE SENSING OF CO2 EMISSIONS OVER NIGHTS, DAYS, AND SEASONS (ASCENDS) mission. ASCENDS is a future space-based mission to determine the global distribution of sources and sinks of atmospheric carbon dioxide (CO2). A unique, multi-frequency, intensity modulated CW (IMCW) laser absorption spectrometer (LAS) operating at 1.57 micron for CO2 sensing has been developed. Effective aerosol and cloud discrimination techniques are being investigated in order to determine concentration values with accuracies less than 0.3%. In this paper, we discuss the demonstration of a pseudo noise (PN) code based technique for cloud and aerosol discrimination applications. The possibility of using maximum length (ML)-sequences for range and absorption measurements is investigated. A simple model for accomplishing this objective is formulated, Proof-of-concept experiments carried out using SONAR based LIDAR simulator that was built using simple audio hardware provided promising results for extension into optical wavelengths.

Campbell, Joel F.↗

Laser Sounder for Measuring Atmospheric CO2 Concentrations: Progress Toward Ascends

The next generation of space-based, active remote sensing instruments for measurement of tropospheric CO2 promises a capability to quantify global carbon sources and sinks at regional scales. Active (laser) methods will extend CO2 measurement coverage in time, space, and perhaps precision such that the underlying mechanisms for carbon exchange at the surface can be understood with .sufficient detail to confidently project the future of carbon-climate interaction and the influence of remediative policy actions. The recent Decadal Survey for Earth Science by the US National Research Council has recommended such a mission called the Active Sensing of CO2 Emissions over Nights, Days, and Seasons (ASCENDS) for launch in 2013-2016. We have been developing a laser technique for measurement of tropospheric CO2 for a number of years. Our immediate goal is to develop and demonstrate the method and instrument technology that will permit measurements of the CO2 column abundance over a horizontal path and from aircraft at the few-ppmv level. Our longer-term goal is to demonstrate the required capabilities of the technique, develop a space mission approach, and design the instrument for an ASCENDS-type mission. Our approach is to use a dual channel laser absorption spectrometer (i.e., differential absorption in altimeter mode), which continuously measures from a near-polar circular orbit. We use several co-aligned tunable fiber laser transmitters allowing simultaneous measurement of the absorption from a CO2 line in the 1570 nm band, O2 extinction in the oxygen A-band (near 765 nm), and aerosol backscatter in the same measurement path. We measure the energy of the laser echoes at nadir reflected from land and water surfaces, day and night. The lasers have spectral widths much narrower than the gas absorption lines and are turned on and off the selected CO2 and O2 lines at kHz rates. The gas extinction and column densities for the CO2 and O2 gases are estimated from the ratio of the on and off-line singnals via the DIAL technique. We used pulsed laser signals, photon counting detectors, and time gating to isolate the laser returns from the surface, and to reject photons scattered from thin clouds and aerosols. High signal-to-noise ratios are required and the CO2 estimates can be sensitive to small drifts or other errors in the instrument, so the absorption estimates need to be quite stable for hours. We have constructed a breadboard version of the CO2 sensor that uses a low power fiber laser and a 20 cm diameter telescope. We have used it to make measurements of CO2 absorption in the laboratory and over 200-m to 2-km long open horizontal paths. These have been done in several sessions extending over multiple days, which allows us to assess the measurement stability and to compare absorption variations to readings from an external in situ CO2 sensor. We have also calculated characteristics of the technique for space including its expected measurement performance for different modulation types, and have performed an initial space mission accommodation study. We sill describe these results in the presentation.

Abshire, J. B.↗

Radiant energy absorption studies for laser propulsion

A study of the energy absorption mechanisms and fluid dynamic considerations for efficient conversion of high power laser radiation into a high velocity flow is presented. The objectives of the study are: (1) to determine the most effective absorption mechanisms for converting laser radiation into translational energy, and (2) to examine the requirements for transfer of the absorbed energy into a steady flow which is stable to disturbances in the absorption zone. A review of inverse Bremsstrahlung, molecular and particulate absorption mechanisms is considered and the steady flow and stability considerations for conversion of the laser power to a high velocity flow in a nozzle configuration is calculated. A quasi-one-dimensional flow through a nozzle was formulated under the assumptions of perfect gas.

Caledonia, G. E.↗

Internal optical losses in very thin CW heterojunction laser diodes

Theoretical calculations are presented showing the relationship between the internal laser absorption and structural parameters appropriate for CW room-temperature lasers. These diodes have submicron-thick recombination regions, and very small spacings between the heat sink and the recombination region to minimize the thermal resistance. The optical loss is shown to be strongly dependent on the degree of radiation confinement to the active region. In particular, absorption in the surface GaAs layer providing the ohmic contact becomes very significant when the intermediate (AlGa)As layer is reduced below about 1 micron. It is further shown that excessive penetration into the GaAs regions gives rise to anomalies in the far-field radiation profiles in the direction perpendicular to the junction plane.

Butler, J. K.↗

Pulsed Lidar for Measurement of C02 Concentrations for the ASCENDS Mission - Update

We have been developing a laser-based sounding technique for the remote measurement of the tropospheric CO2 concentrations from orbit for NASA is ASCENDS mission. The mission's goals are to provide measurements of tropospheric CO2 abundance with global-coverage, a few hundred km spatial and monthly temporal resolution. These are needed to better understand CO2 fluxes and the processes that regulate CO2 storage by the land and oceans. For the lIP, we are developing and demonstrating the lidar techniques and key lidar technology that will permit measurements of the CO2 column abundance in the lower troposphere from aircraft. Our final goal is to demonstrate the key capabilities needed for a space lidar and mission approach for the ASCENDS mission. We use a pulsed lidar technique, which is much less sensitive to errors from cloud and atmospheric scattering and to noise from solar background. It allows continuous measurements of CO2 mixing ratio in the lower troposphere during day and night. Our approach uses the 1570nm CO2 band and a two-wavelength laser absorption spectrometer, which continuously measures at nadir from a circular polar orbit. It directs the narrow co-aligned laser beams from the instrument's lasers toward nadir, and measures the energy of the laser echoes reflected from land and water surfaces. It uses a pair of tunable laser transmitters, which allowing measurement of the extinction from a single selected CO2 absorption line in the 1570 nm band and from a line pair in the Oxygen A-band near 765 nm. These regions have temperature insensitive absorption lines are free from interference from other gases. The lasers pulse at 10KHz, use tunable diode seed lasers followed by laser amplifiers, and have MHz spectral widths. During the measurement the lasers are stepped across the selected lines at a kHz rate. The receiver uses a 1-m class telescope and photon sensitive detectors and measures the background light and energies of the laser echoes from the surface. The extinction and column densities for the CO2 and O2 gases are estimated from the ratio of the on and off line echo pulse energies via the integrated path differential absorption (IPDA) technique. Our technique exploits the atmospheric pressure broadening of the lines to weight the measurement sensitivity to the atmospheric column below 5 km. Pulsed laser signals, time gated receiver are used to isolate the surface laser echo signals and to exclude photons scattered from clouds and aerosols. We have successfully demonstrated many key aspects of the approach and lidar technology in the laboratory. We have demonstrated CO2 column measurements in airborne flights during the summers of 2009 and 2010. These included measurements from 3-l3 km altitudes made over a variety of surfaces and through thin and broken clouds. We demonstrated initial airborne measurements of O2 column density to 10 km altitudes during the summer 2010 flights. More details approach, key technologies, and demonstration measurements will be given in the presentation.

Abshire, James↗

HO2 detection by near infrared absorption using tunable diode lasers

The strongest absorption lines are in the v sub 2 vibrational band around 1400/cm; several near-coincident line pairs in this region provide max linestrengths of 1.2 x 10 exp -20 sq. cm/(molecule*cm). High Frequency wavelength modulation coupled with sweep integration were used to minimize noise and maintain spectral discrimination. Reduced pressure sampling was performed using supersonic nozzle and an aerodynamic flow cell to minimize residence time and wall losses of radicals. The astigmatic mirror design provides pathlengths up to 200 m in volume of 3 liters with minimal optical interference fringes; longer pathlengths are possible. The detection limit depends on pathlength and minimum fractional absorptions.

Nelson, David↗

Remote measurements of ozone, water vapor and liquid water content, and vertical profiles of temperature in the lower troposphere

Several advanced atmospheric remote sensing systems developed at the Jet Propulsion Laboratory were demonstrated under various field conditions to determine how useful they would be for general use by the California Air Resources Board and local air quality districts. One of the instruments reported on is the Laser Absorption Spectrometer (LAS). It has a pair of carbon dioxide lasers with a transmitter and receiver and can be flown in an aircraft to measure the column abundance of such gases as ozone. From an aircraft, it can be used to rapidly survey a large region. The LAS is usually operated from an aircraft, although it can also be used at a fixed location on the ground. Some tests were performed with the LAS to measure ozone over a 2-km horizontal path. Another system reported on is the Microwave Atmospheric Remote Sensing System (MARS). It is tuned to microwave emissions from water vapor, liquid water, and oxygen molecules (for atmospheric temperature). It can measure water vapor and liquid water in the line-of-sight, and can measure the vertical temperature profile.

Grant, W. B.↗

Wavelength-selective, sequential Q-switching laser cavity

Single-frequency continuous output of laser is converted into series of high-power laser pulses at high repetition rates. Applications include pollutant detection by absorption, laser gain measurements at discrete wavelengths, laser propagation measurement, and laser plasma diagnostics.

Allario, F.↗

Measurements of Temperature and Enthalpy in NASA Ames 60-MW Arcjet using Atomic Oxygen and Atomic Nitrogen Absorption

We report on measurements of temperature and enthalpy in the 60-MW Interaction Heating Facility (IHF) Arcjet at the NASA Ames Research Center. These quantities were measured at sub-second temporal resolution using tunable diode laser absorption spectroscopy, employing four Distributed Feedback (DFB) lasers to simultaneously probe the arcjet flow. Optical access was achieved through a specially-designed optical disk mounted in series with the modules of the arc heater in the add-air plenum of the column, which is positioned between the downstream electrodes and the nozzle. Gas at this measurement location serves as the reservoir condition for the ensuing supersonic expansion. Conditions in the reservoir are extreme, with temperatures between 5000-8000 K and pressures between 1-9 atm. Absorption from the 5S state of atomic oxygen at 777.2 nm and the 4P state of atomic nitrogen at 868.0 nm, two electronically-excited quantum states, formed the basis of the flow characterization measurements. Fiber-coupled laser light was pitched through the IHF via 1/8" ports in the optical disks, permitting optical access with minimal intrusion to the flow. Data was collected at 3 nominal conditions, a Low condition (1600 A, 2000 V, 0.13 kg/s), a Medium condition (3500 A, 5700 V, 0.61 kg/s), and a High condition (5900 A, 6800 V, 0.84 kg/s). Measurements suggest agreement within 1-2% between excited oxygen and excited nitrogen thermometry, indicating approximate thermal and chemical equilibration of the arcjet reservoir state, a result in keeping with long-standing assumptions of CFD modelling. Spatial gradients are found in the flow due to enthalpy loss to the facility walls, but the measured spatial non-uniformities are consistent with axi-symmetry. Measurements of specific enthalpy in the reservoir are also made utilizing excited oxygen and excited nitrogen absorption under the assumption of chemical equilibration.

Peter M. Finch↗

Investigation of N2O Production from 266 and 532 nm Laser Flash Photolysis of O3/N2/O2 Mixtures

Tunable diode laser absorption spectroscopy has been employed to measure the amount of N2O produced from laser flash photolysis of O3/N2/O2 mixtures at 266 and 532 nm. In the 532 nm photolysis experiments very little N2O is observed, thus allowing an upper limit yield of 7 x 10(exp -8) to be established for the process O3 + N2 yield N2O + O2, where O3 is nascent O3 that is newly formed via O(3P(sub J)) + O2 recombination (with vibrational excitation near the dissociation energy of O3). The measured upper limit yield is a factor of approx. 600 smaller than a previous literature value and is approximately a factor of 10 below the threshold for atmospheric importance. In the 266 nm photolysis experiments, significant N2O production is observed and the N2O quantum yield is found to increase linearly with pressure over the range 100 - 900 Torr in air bath gas. The source of N2O in the 266 nm photolysis experiments is believed to be the addition reaction O(1D(sub 2)) + N2 + M yields (k(sub sigma)) N2O + M, although reaction of (very short-lived) electronically excited O3 with N2 cannot be ruled out by the available data. Assuming that all observed N2O comes from the O(1D(sub 2)) + N2 + M reaction, the following expression describes the temperature dependence of k(sub sigma) (in its third-order low-pressure limit) that is consistent with the N2O yield data: k(sub sigma) = (2.8 +/- 0.1) x 10(exp -36)(T/300)(sup -(0-88+0.36)) cm(sup 6) molecule(sup -2)/s, where the uncertainties are 2(sigma) and represent precision only. The accuracy of the reported rate coefficients at the 95% confidence level is estimated to be 30 - 40% depending on the temperature. Model calculations suggest that gas phase processes initiated by ozone absorption of a UV photon represent about 1.4% of the currently estimated global source strength of atmospheric N2O. However, these processes could account for a significant fraction of the oxygen mass-independent enrichment observed in atmospheric N2O, and they appear to be the first suggested photochemical mechanism that is capable of explaining the altitude dependence of the observed mass -independent isotopic signature.

Estupinan, E. G.↗

A microscopic description of sound absorption in the atmosphere

The various mechanisms which contribute to sound absorption in the atmosphere are identified and a technique for computing the contribution from each is presented. The similarities between sound absorption, laser fluorescence measurements, and the opto-acoustic effect are discussed. Finally, experimental sound absorption results are compared to predictions to test the microscopic energy transfer approach.

Bass, H. E.↗

Kinetics of the Reactions of F((sup 2)P) and Cl((sup 2)P) with HNO3

The kinetics of the reactions of HNO3 with fluorine (k(sub 1)) and Chlorine (k(sub 2)) atoms have been studied by using a time-resolved long-path laser absorption technique to monitor the appearance of product NO3 radicals following 351-nm pulsed laser photolysis of X2/HNO3/He mixtures (X = F,Cl). Absolute rate coefficients for the F((sup 2)P) + HNO reaction have been determined over the temperature range 260-373 K. Between 260 and 320 K, the data are adequately represented by the Arrhenius expression k(sub 1)(T) = (6.0 +/- 2.6) x 10(exp -12) exp[(40 +/- 120)/T]cu cm/(molecule.s). Between 335 and 373 K, the rate coefficient is found to be (2.0 +/- 0.3) x 10(exp -11)cu cm/(molecule.s) independent of temperature. The observed temperature dependence suggests that reaction proceeds via competing direct abstraction and complex pathways. No NO3 production was observed in the experiments with X equals Cl, thus establishing that k(sub 2)(298 K) is less than 2 x 10(exp -16) cu cm/(molecule.s). The Cl((sup 2)P) + HNO reaction was also investigated by using a pulsed laser photolysis-resonance fluorescence technique to monitor the decay of Cl((sup 2)P). Upper limit values for k(sub 2) obtained from these experiments, in units of 10(exp -16)cu cm/(molecule.s), are 13 at 298 K and 10 at 400 K.

Wine, P. H.↗

Quantitative measurement of oxygen in microgravity combustion

This research combines two innovations in an experimental system which should result in a new capability for quantitative, nonintrusive measurement of major combustion species. Using a newly available vertical cavity surface-emitting diode laser (VCSEL) and an improved spatial scanning method, we plan to measure the temporal and spatial profiles of the concentrations and temperatures of molecular oxygen in a candle flame and in a solid fuel (cellulose sheet) system. The required sensitivity for detecting oxygen is achieved by the use of high frequency wavelength modulation spectroscopy (WMS). Measurements will be performed in the NASA Lewis 2.2-second Drop Tower Facility. The objective of this research is twofold. First, we want to develop a better understanding of the relative roles of diffusion and reaction of oxygen in microgravity combustion. As the primary oxidizer species, oxygen plays a major role in controlling the observed properties of flames, including flame front speed (in solid or liquid flames), extinguishment characteristics, flame size, and flame temperature. The second objective is to develop better diagnostics based on diode laser absorption which can be of real value in microgravity combustion research. We will also demonstrate diode lasers' potential usefulness for compact, intrinsically-safe monitoring sensors aboard spacecraft. Such sensors could be used to monitor any of the major cabin gases as well as important pollutants.

Silver, Joel A.↗