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NASA NTRS2003

Retrieval and Analysis of Stratospheric NO2 from GOME

In this paper we describe the retrieval of stratospheric NO2 from the GOME (Global Ozone Monitoring Experiment) spectrometer. For this retrieval the Differential Optical Absorption Spectroscopy (DOAS) is used and we describe the influence of the instrument s characteristics on this measurement technique. This analysis led to an improved version of the DOAS algorithm resulting in results with lower systematic errors. Subsequently these results were used to separate the tropospheric and stratospheric fraction of the measured NO;! in the atmosphere. This paper is focusing on the annual variations of the stratospheric distribution of nitrogen oxides. For this examination the satellite data from beginning of 1996 to the end of 2001 was used and has been visualized in a plot zonal means versus time of the year, a visualization which proved to be very useful for Ozone. Additionally the so called "Noxon Cliff", a drop of NO2 column densities Noxon measured in 1975-77 while traveling northwards towards the pole in Canada, is shown. Also its southern equivalent could be discovered in the GOME data.

Wenig, M.↗
NASA NTRS2004

Evidence That Nitric Acid Increases Relative Humidity in Low-Temperature Cirrus Clouds

In situ measurements of the relative humidity with respect to ice (RH(sub(i)) and of nitric acid (HNO3) were made in both natural and contrail cirrus clouds in the upper troposphere. At temperatures lower than 202 kelvin, RH(sub i) values show a sharp increase to average values of over 130% in both cloud types. These enhanced RH(sub i) values are attributed to the presence of a new class of NHO3- containing ice particles (Delta-ice). We propose that surface HNO3 molecules prevent the ice/vapor system from reaching equilibrium by a mechanism similar to that of freezing point depression by antifreeze proteins. Delta-ice represents a new link between global climate and natural and anthropogenic nitrogen oxide emissions. Including Delta-ice in climate models will alter simulated cirrus properties and the distribution of upper tropospheric water vapor.

Gao, R. S.↗
NASA NTRS2003

Elevated Ozone in the Troposphere over the Atlantic and Pacific Oceans in the Northern Hemisphere

Tropospheric column ozone (TCO) is derived from differential measurements of total column ozone from Nimus-7 and Earth Probe TOMS, and stratospheric column ozone from the Microwave Limb Sounder instrument on the Upper Atmospheric Research Satellite. It is shown that TCO during summer months over the Atlantic and Pacific Oceans at northern mid-latitudes is about the same (50-60 Dobson Units) as over the continents of North America, Europe and Asia, where surface emissions of nitrogen oxides from industrial sources, biomass and biofuel burning and biogenic emissions are significantly larger. This nearly uniform zonal variation in TCO is modulated by surface topography of the Rocky and Himalayan mountains and Tibetan Plateau where TCO is reduced by 20-30 Dobson Units. The zonal characteristics of TCO derived from satellite measurements are well simulated by a global chemical transport model called MOZART-2 (Model of Ozone and Related Chemical Tracers, version 2). The model results are analyzed to delineate the relative importance of various processes contributing to observed zonal characteristics of TCO, and they are shown that the surface emission of NOx contributes about 50% of the TCO at northern mid-latitudes, especially over the continents of North America, Europe and Asia. The result of TCO derived from TOMS and the analysis from MOZART-2 indicate that TCO is a very useful tool to study tropospheric O3 pollution resulting from surface emissions of pollutants.

Chandra, S.↗
NASA NTRS2004

RQL Integrated Module Rig Test

This report documents the activities conducted under Work Breakdown Structure (WBS) 1.0.2.7 of the NASA Critical Components (CPC) Program to evaluate the low emissions potential of a Rich-Quench-Lean combustor capable of achieving the program goal of emissions of nitrogen oxides (NOxEI) less than 5 gm/Kg fuel at the supersonic light condition while maintaining combustion efficiencies in excess of 99.9 percent. The chosen combustor module would then be tested in the subscale annular rig test prior to testing in the subscale core engine demonstrator, if the RQL concept were to be chosen at the Combustor Downselect.

Koopman, Frederick S.↗
NASA NTRS2004

Product Module Rig Test

The low emissions potential of a Rich-Quench-Lean (RQL) combustor for use in the High Speed Civil Transport (HSCT) application was evaluated as part of Work Breakdown Structure (WBS) 1.0.2.7 of the NASA Critical Propulsion Components (CPC) Program under Contract NAS3-27235. Combustion testing was conducted in cell 1E of the Jet Burner Test Stand at United Technologies Research Center. Specifically, a Rich-Quench-Lean combustor, utilizing reduced scale quench technology implemented in a quench vane concept in a product-like configuration (Product Module Rig), demonstrated the capability of achieving an emissions index of nitrogen oxides (NOx EI) of 8.5 gm/Kg fuel at the supersonic flight condition (relative to the program goal of 5 gm/Kg fuel). Developmental parametric testing of various quench vane configurations in the more fundamental flametube, Single Module Rig Configuration, demonstrated NOx EI as low as 5.2. All configurations in both the Product Module Rig configuration and the Single Module Rig configuration demonstrated exceptional efficiencies, greater than 99.95 percent, relative to the program goal of 99.9 percent efficiency at supersonic cruise conditions. Sensitivity of emissions to quench orifice design parameters were determined during the parametric quench vane test series in support of the design of the Product Module Rig configuration. For the rectangular quench orifices investigated, an aspect ratio (length/width) of approximately 2 was found to be near optimum. An optimum for orifice spacing was found to exist at approximately 0.167 inches, resulting in 24 orifices per side of a quench vane, for the 0.435 inch quench zone channel height investigated in the Single Module Rig. Smaller quench zone channel heights appeared to be beneficial in reducing emissions. Measurements were also obtained in the Single Module Rig configuration on the sensitivity of emissions to the critical combustor parameters of fuel/air ratio, pressure drop, and residence time. Minimal sensitivity was observed for all of these parameters.

Holdeman, James D.↗
NASA NTRS2004

New Reduced Two-Time Step Method for Calculating Combustion and Emission Rates of Jet-A and Methane Fuel With and Without Water Injection

A simplified kinetic scheme for Jet-A, and methane fuels with water injection was developed to be used in numerical combustion codes, such as the National Combustor Code (NCC) or even simple FORTRAN codes that are being developed at Glenn. The two time step method is either an initial time averaged value (step one) or an instantaneous value (step two). The switch is based on the water concentration in moles/cc of 1x10(exp -20). The results presented here results in a correlation that gives the chemical kinetic time as two separate functions. This two step method is used as opposed to a one step time averaged method previously developed to determine the chemical kinetic time with increased accuracy. The first time averaged step is used at the initial times for smaller water concentrations. This gives the average chemical kinetic time as a function of initial overall fuel air ratio, initial water to fuel mass ratio, temperature, and pressure. The second instantaneous step, to be used with higher water concentrations, gives the chemical kinetic time as a function of instantaneous fuel and water mole concentration, pressure and temperature (T4). The simple correlations would then be compared to the turbulent mixing times to determine the limiting properties of the reaction. The NASA Glenn GLSENS kinetics code calculates the reaction rates and rate constants for each species in a kinetic scheme for finite kinetic rates. These reaction rates were then used to calculate the necessary chemical kinetic times. Chemical kinetic time equations for fuel, carbon monoxide and NOx were obtained for Jet-A fuel and methane with and without water injection to water mass loadings of 2/1 water to fuel. A similar correlation was also developed using data from NASA's Chemical Equilibrium Applications (CEA) code to determine the equilibrium concentrations of carbon monoxide and nitrogen oxide as functions of overall equivalence ratio, water to fuel mass ratio, pressure and temperature (T3). The temperature of the gas entering the turbine (T4) was also correlated as a function of the initial combustor temperature (T3), equivalence ratio, water to fuel mass ratio, and pressure.

Molnar, Melissa↗
NASA NTRS2003

Elevated Tropospheric Ozone over the Atlantic

Tropospheric column ozone (TCO) is derived from differential measurements of TOMS total column ozone and Microwave Limb Sounder stratospheric column ozone. It is shown that TCO during summer months over the Atlantic and Pacific Oceans in northern midlatitudes is about the same (50 to 60 Dobson Units) as over the continents of North America, Europe, and Asia, where surface emissions of nitrogen oxides from industrial sources, biomass and biofuel burning and biogenic emissions are significantly larger. This nearly uniform zonal variation in TCO is modulated by surface topography of the Rocky and Himalayan mountains, and Tibetan plateau where TCO is reduced by 20 to 30 Dobson Units. The zonal variation in TCO is well simulated by a global chemical transport model called MOZART-2 (Model of Ozone and Related Chemical Tracers, version 2). The model results are analyzed to delineate the relative importance of various processes contributing to observed zonal characteristics of TCO.

Chandra, S.↗
NASA NTRS2000

Quantifying the Intercontinental and Global Reach and Effects of Pollution

The Atmospheric Chemistry Modeling Group is participating in an international effort to explore the projected interactions of the atmosphere with biota, human activity, and the natural environment over the next three decades. The group uses computer simulations and statistical analyses to compare theory and observations of the composition of the lower atmosphere. This study of global habitability change is part of a more ambitious activity to understand global habitability. This broad planetary understanding is central to planetary habitability, biomarker detection, and similar aspects of Astrobiology. The group has made highly detailed studies of immense intercontinental plumes that affect the chemistry of the global atmosphere, especially the region below the ozone (O3) layer whose chemical composition defines the conditions for healthy humans and the biosphere. For some decades there has been concern about the pollution from cities and industrial burning and its possible effect in increasing smog ozone, not only in continental regions, but also in plumes that spread downwind. Recently, there has been new concern about another kind of pollution plume. Projections for a greatly expanded aircraft fleet imply that there will be plumes of nitrogen oxides (NO(x)) from jet exhaust in the Northern Hemisphere downwind of major air traffic routes. Both of these are tied to large-scale O3 in the troposphere, where it is toxic to humans and plant tissues.

Chatfield, Robert B.↗
NASA NTRS2003

The Stable Isotope Fractionation of Abiotic Reactions: A Benchmark in the Detection of Life

One very important tool in the analysis of biogenic, and potentially biogenic, samples is the study of their stable isotope distributions. The isotope distribution of a sample depends on the process(es) that created it. One important application of the analysis of C & N stable isotope ratios has been in the determination of whether organic matter in a sample is of biological origin or was produced abiotically. For example, the delta C-13 of organic material found embedded in phosphate grains was cited as a critical part of the evidence for life in 3.8 billion year old samples. The importance of such analysis in establishing biogenicity was highlighted again by the role this issue played in the recent debate over the validity of what had been accepted as the Earth s earliest microfossils. These kinds of analysis imply a comparison with the fractionation that one would have seen if the organic material had been produced by alternative, abiotic, pathways. Could abiotic reactions account for the same level of fractionation? Additionally, since the fractionation can vary between different abiotic reactions, understanding their fractionations can be important in distinguishing what reactions may have been significant in the formation of different abiological samples (such as extraterrestrial samples). There is however, a scarcity of data on the fractionation of carbon and nitrogen by abiotic reactions. In order to interpret properly what the stable isotope ratios of samples tell us about their biotic or abiotic nature, more needs to be known about how abiotic reactions fractionate C and N. Carbon isotope fractionations have been studied for a few abiotic processes. These studies presumed the presence of a reducing atmosphere, focusing on reactions involving spark discharge, W photolysis of reducing gas mixtures, and cyanide polymerization in the presence of ammonia. They did find that the initial products showed a depletion in I3C with values in the range of a few per mil to as low as -60 % (potentially comparable to that which accompanies the biosynthesis of organic matter). We need to understand what kind of fractionations are observed with reactions under the non-reducing or mildly reducing conditions now thought to be present on the early Earth. While nitrogen is receiving increased attention as a tool for these kinds of analyses, almost nothing is known about the isotope fractionation that one would expect for abiotic sources of fixed/reduced nitrogen. This project will measure the fixation from a series of abiotic reactions that may have been present on the early Earth (and other terrestrial planets) and produced organic material that could have ended up in the rock record. The work will look at a number of reactions, under a non- reducing, or mildly reducing, atmosphere, covering sources of prebiotic organic C & N from shock heating, to photochemistry, to hydrothermal reactions. Some reactions that we plan to study are; Shock heating of a non-reducing atmosphere to produce CO and NO (in collaboration with Chris McKay), formation of formaldehyde (and related compounds) from COY the formation of ammonia from nitrogen oxides (ultimately from NO) by ferrous iron reduction, and the hydrothermal synthesis of compounds including the hydrocarboxylation/hydrocarbonylation reaction (in collaboration with George Cody), reactions of oxalate to form hydrocarbons and other oxygenated compounds and the formation of lipids from oxalic/formic acid (in collaboration with Tom McCollom), and reactions of carbon monoxide & carbon dioxide with N2, ammonia or nitritehitrate to form hydrogen cyanide, nitriles, ammonia/amines and nitrous

Summers, David P.↗
NASA NTRS2004

Human Health Risk Assessment Simulations in a Distributed Environment for Shuttle Launch

During the launch of a rocket under prevailing weather conditions, commanders at Cape Canaveral Air Force station evaluate the possibility of whether wind blown toxic emissions might reach civilian and military personnel in the near by area. In our model, we focused mainly on Hydrogen chloride (HCL), Nitrogen oxides (NOx) and Nitric acid (HNO3), which are non-carcinogenic chemicals as per United States Environmental Protection Agency (USEPA) classification. We have used the hazard quotient model to estimate the number of people at risk. It is based on the number of people with exposure above a reference exposure level that is unlikely to cause adverse health effects. The risk to the exposed population is calculated by multiplying the individual risk and the number in exposed population. The risk values are compared against the acceptable risk values and GO or NO-go situation is decided based on risk values for the Shuttle launch. The entire model is simulated over the web and different scenaria can be generated which allows management to choose an optimum decision.

Thirumalainambi, Rajkumar↗
NASA NTRS2003

Asian Outflow and Trans-Pacific Transport of Carbon Monoxide and Ozone Pollution: An Integrated Satellite, Aircraft, and Model Perspective

Satellite observations of carbon monoxide (CO) from the Measurements of Pollution in the Troposphere (MOPITT) instrument are combined with measurements from the Transport and Chemical Evolution Over the Pacific (TRACE-P) aircraft mission over the northwest Pacific and with a global three-dimensional chemical transport model (GEOS-CHEM) to quantify Asian pollution outflow and its trans-Pacific transport during spring 2001. Global CO column distributions in MOPITT and GEOS-CHEM are highly correlated (R(exp 2) = 0.87), with no significant model bias. The largest regional bias is over Southeast Asia, where the model is 18% too high. A 60% decrease of regional biomass burning emissions in the model (to 39 Tg/yr) would correct the discrepancy; this result is consistent with TRACE-P observations. MOPITT and TRACE-P also give consistent constraints on the Chinese source of CO from fuel combustion (181 Tg CO/yr). Four major events of trans-Pacific transport of Asian pollution in spring 2001 were seen by MOPITT, in situ platforms, and GEOS-CHEM. One of them was sampled by TRACE-P (26-27 February) as a succession of pollution layers over the northeast Pacific. These layers all originated from one single event of Asian outflow that split into northern and southern plumes over the central Pacific. The northern plume (sampled at 6-8 km off California) had no ozone enhancement. The southern subsiding plume (sampled at 2-4 km west of Hawaii) contained a 8 - 17 ppbv ozone enhancement, driven by decomposition of peroxyacetylnitrate (PAN) to nitrogen oxides (NOx). This result suggests that PAN decomposition in trans-Pacific pollution plumes subsiding over the United States could lead to significant enhancements of surface ozone.

Heald, Colette L.↗
NASA NTRS2002

An Improved Retrieval of Tropospheric Nitrogen Dioxide from GOME

We present a retrieval of tropospheric nitrogen dioxide (NO2) columns from the Global Ozone Monitoring Experiment (GOME) satellite instrument that improves in several ways over previous retrievals, especially in the accounting of Rayleigh and cloud scattering. Slant columns, which are directly fitted without low-pass filtering or spectral smoothing, are corrected for an artificial offset likely induced by spectral structure on the diffuser plate of the GOME instrument. The stratospheric column is determined from NO2 columns over the remote Pacific Ocean to minimize contamination from tropospheric NO2. The air mass factor (AMF) used to convert slant columns to vertical columns is calculated from the integral of the relative vertical NO2 distribution from a global 3-D model of tropospheric chemistry driven by assimilated meteorological data (Global Earth Observing System (GEOS)-CHEM), weighted by altitude dependent scattering weights computed with a radiative transfer model (Linearized Discrete Ordinate Radiative Transfer), using local surface albedos determined from GOME observations at NO2 wavelengths. The AMF calculation accounts for cloud scattering using cloud fraction, cloud top pressure, and cloud optical thickness from a cloud retrieval algorithm (GOME Cloud Retrieval Algorithm). Over continental regions with high surface emissions, clouds decrease the AMT by 20- 30% relative to clear sky. GOME is almost twice as sensitive to tropospheric NO2 columns over ocean than over land. Comparison of the retrieved tropospheric NO2 columns for July 1996 with GEOS-CHEM values tests both the retrieval and the nitrogen oxide radical (NOx) emissions inventories used in GEOS-CHEM. Retrieved tropospheric NO2 columns over the United States, where NOx emissions are particularly well known, are within 18% of GEOS-CHEM columns and are strongly spatially correlated (r = 0.78, n = 288, p less than 0.005). Retrieved columns show more NO2 than GEOS-CHEM columns over the Transvaal region of South Africa and industrial regions of the northeast United States and Europe. They are lower over Houston, India, eastern Asia, and the biomass burning region of central Africa, possibly because of biases from absorbing aerosols.

Martin, Randall V.↗
NASA NTRS2004

Analysis of 1970-1995 Trends in Tropospheric Ozone at Northern Hemisphere Midlatitudes with the GEOS-CHEM Model

I ] The causes of trends in tropospheric ozone at Northern Hemisphere midlatitudes from 1970 to 1995 are investigated with the GEOS-CHEM model, a global three-dimensional model of the troposphere driven by assimilated meteorological observations from the Goddard Earth Observing System (GEOS). This model is used to investigate the sensitivity of tropospheric ozone with respect to (1) changes in the anthropogenic emission of nitrogen oxides and nonmethane hydrocarbons, (2) increases in methane concentrations, (3) variations in the stratospheric source of ozone, (4) changes in solar radiation resulting from stratospheric ozone depletion, and ( 5 ) increases in tropospheric temperatures. Model results indicate that local increases in NO, emissions have caused most of the increases seen in lower tropospheric ozone over Europe and Japan. Increases in methane are responsible for roughly one fifth of the anthropogenically induced increase in tropospheric ozone at northern midlatitudes. However, changes in ozone precursors do not adequately explain either the spatial differences in observed ozone trends across midlatitudes or the observed decreases in ozone over Canada throughout the troposphere. We argue that ozone depletion in the lowermost stratosphere is likely to have reduced the stratospheric source by as much as 30% from the early 1970s to the mid 1990s. Model simulations that account for such a reduction along with reported changes in anthropogenic emissions show steep declines of ozone in the upper troposphere and variable increases in the lower troposphere that are more consistent with observations. Differential temperature trends in summer between North America and Europe may account for at least some of the remaining spatial variation in tropospheric ozone trends. Increases in ultraviolet (UV) radiation due to stratospheric ozone depletion do not appear to significantly reduce tropospheric ozone, except at midlatitudes in the Southern Hemisphere following the breakup of the ozone hole.

Fusco, Andrew C.↗
NASA NTRS1988

The enzymes associated with denitrification

The enzymes involved in the reduction of nitrogenous oxides are thought to be intermediates in denitrification processes. This review examines the roles of nitrate reductase, nitrite reductases, nitric oxide reductase, mechanisms of N-N bond formation, and nitrous oxide reductases.

NASA Discipline Exobiology↗
NASA NTRS2004

Analysis of Satellite and Sub-Orbital Measurements

The objective of this project is to support the INTEX aircraft mission by developing experience in the integrated analysis of existing sub-orbital observations and satellite observations with numerical models. Specific tasks include providing guidance to INTEX by identifying discrepancies in satellite observations with (1) in situ measurements, (2) bottom-up emission inventories of nitrogen oxides and volatile organic compounds, and (3) model calculations of the export of pollution from North America to the global atmosphere. An important focus area is developing and improving bottom-up emission inventories by combining top-down and bottom-up information.

Gleason, James↗
NASA NTRS1995

Capabilities Enhanced for Researching the Reduction of Emissions in Future Aircraft

Aircraft future aircraft jet engines will run at higher pressures to obtain greater fuel efficiency and performance. This will require new combustor designs to keep the nitrogen oxide and carbon monoxide emissions at environmentally acceptable levels. The actual pressures and temperatures found in gas turbine combustors must be duplicated in a laboratory to verify the emissions characteristics of gas turbine engines. Recognizing this, the U.S. aircraft gas turbine industry identified a need for a national facility that could duplicate the severe inlet conditions of future combustors. Because of our expertise in combustion emissions reduction research and in the design and operation of high-pressure test facilities, the NASA Lewis Research Center was seen as the natural location for such a facility. As a national laboratory, Lewis could provide these facilities to all U.S. gas turbine engine manufacturers while protecting their proprietary interests. Called the Advanced Subsonic Combustion Rig, the facility will provide up to 60-atm pressures at inlet temperatures up to 1300 F and air flow rates up to 38 lb/sec. Furthermore, it will offer state-of-the-art diagnostic methods for characterizing advanced combustor concepts. Aeronautical combustion research at Lewis provided several significant accomplishments recently in support of both the High Speed Research (HSR) and Advanced Subsonic Technology (AST) programs. For example, in the High Speed Research Program, NO_x reductions of up to 90 percent were achieved in prototype combustor hardware. Advanced computational analysis, gas sampling, and laser diagnostic techniques were critical to this success. Working closely with the gas turbine industry, we have successfully transferred this low-emissions combustor technology into engine prototype hardware. This hardware is now being tested at the engine manufacturers facilities. Complementary tests in Lewis currently available 30-atm test facilities are also underway, taking advantage of Lewis unique diagnostic capabilities. By utilizing test facilities belonging to both NASA and its industry partners, we have tested multiple combustor concepts in a shorter period of time.

Source record↗
NASA NTRS2003

Emissions of Trace Gases and Particles from Two Ships in the Southern Atlantic Ocean

Measurements were made of the emissions of particles and gases from two diesel-powered ships in the southern Atlantic Ocean off the coast of Namibia. The measurements are used to derive emission factors from ships of three species not reported previously, namely, black carbon, accumulation-mode particles, and cloud condensation nuclei (CCN), as well as for carbon dioxide, carbon monoxide (CO), methane (CH4), non-methane hydrocarbons, sulfur dioxide (SO2), nitrogen oxides (NOx), and condensation nuclei. The effects of fuel grade and engine power on ship emissions are discussed. The emission factors are combined with fuel usage data to obtain estimates of global annual emissions of various particles and gases from ocean-going ships. Global emissions of black carbon, accumulation- mode particles, and CCN from ocean-going ships are estimated to be 19-26 Gg yr(sup -1), (4.4-6.1) x 10(exp 26) particles yr(sup -1), and (1.0-1.5) x l0(exp 26) particles yr(sup -1), respectively. Black carbon emissions from ocean-going ships are approximately 0.2% of total anthropogenic emissions. Emissions of NOx and SO2 from ocean-going ships are approximately 10-14% and approximately 3-4%, respectively, of the total emissions of these species from the burning of fossil fuels, and approximately 40% and approximately 70%, respectively, of the total emissions of these species from the burning of biomass. Global annual emissions of CO and CH4 from ocean-going ships are approximately 2% and approximately 2-5%, respectively, of natural oceanic emissions of these species.

Sinha, Parikhit↗
NASA NTRS2003

Emissions of Trace Gases and Particles from Savanna Fires in Southern Africa

Airborne measurements made on initial smoke from 10 savanna fires in southern Africa provide quantitative data on emissions of 50 gaseous and particulate species, including carbon dioxide, carbon monoxide, sulfur dioxide, nitrogen oxides, methane, ammonia, dimethyl sulfide, nonmethane organic compounds, halocarbons, gaseous organic acids, aerosol ionic components, carbonaceous aerosols, and condensation nuclei (CN). Measurements of several of the gaseous species by gas chromatography and Fourier transform infrared spectroscopy are compared. Emission ratios and emission factors are given for eight species that have not been reported previously for biomass burning of savanna in southern Africa (namely, dimethyl sulfide, methyl nitrate, five hydrocarbons, and particles with diameters from 0.1 to 3 microns). The emission factor that we measured for ammonia is lower by a factor of 4, and the emission factors for formaldehyde, hydrogen cyanide, and CN are greater by factors of about 3, 20, and 3 - 15, respectively, than previously reported values. The new emission factors are used to estimate annual emissions of these species from savanna fires in Africa and worldwide.

Sinha, Parikhit↗