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NASA NTRS1991

Organic matter in meteorites and comets - Possible origins

At least six extraterrestrial environments may have contributed organic compounds to meteorites and comets: solar nebula, giant-planet subnebulae, asteroid interiors containing liquid water, carbon star atmospheres, and diffuse or dark interstellar clouds. The record in meteorites is partly obscured by pervasive reheating that transformed much of the organic matter to kerogen; nonetheless, it seems that all six formation sites contributed. For comets, the large abundance of HCHO, HCN, and unsaturated hydrocarbons suggests an interstellar component of 50 percent or more, but the contributions of various interstellar processes, and of a solar-nebula component, are hard to quantify. A research program is outlined that may help reduce these uncertainties.

Anders, Edward↗
NASA NTRS1996

Interpretation of lidar and satellite data sets using a global photochemical model

The status in the beginning of the report period was that the existing General Circulation Model (GCM) was running with a chemistry module compiled for stratospheric simulation studies. The chemistry simulation was not working sufficiently in the troposphere and any tropospheric trace gas sources or dry deposition sinks were not yet incorporated. The current status concerning the chemistry module is that the chemistry simulation has been modified to also simulate the chemistry in the troposphere with resulting mixing ratios close to other model simulations as described in Olson et al. (1996). The mechanism to incorporate trace gas source and dry deposition sinks, testing for H202, CH300H, 03, HCHO, HN03, and N02, are incorporated and is currently being tested. Existing model and development versions include: the full GCM model, currently still running with the original stratospheric chemistry module; an off-line version of the GCM, i.e. wind and photolysis rates are pre-calculated and prescribed in read-in arrays; a box model version of the modified chemistry module for developments and first tests of new modifications; and a box model with the same chemistry simulated but flexible partitioning and integration methods for test purposes of those. The grantee's work focused mainly on three areas: trace gas sources and dry deposition; method to introduce a NO source instead of a NO(x) source; and investigating integration methods.

Chyba, Thomas↗
NASA NTRS2000

Science Requirements Document for OMI-EOS

A Dutch-Finnish scientific and industrial consortium is supplying the Ozone Monitoring Instrument (OMI) for Earth Observing System-Aura (EOS-Aura). EOS-Aura is the next NASA mission to study the Earth's atmosphere extensively, and successor to the highly successful UARS (Upper Atmospheric Research Satellite) mission. The 'Science Requirements Document for OMI-EOS' presents an overview of the Aura and OMI mission objectives. It describes how OMI fits into the Aura mission and it reviews the synergy with the other instruments onboard Aura to fulfill the mission. This evolves in the Scientific Requirements for OMI (Chapter 3), stating which trace gases have to be measured with what necessary accuracy, in order for OMI to meet Aura's objectives. The most important data product of OMI, the ozone vertical column, densities shall have a better accuracy and an improved global coverage than the predecessor instruments TOMS (Total Ozone Monitoring Spectrometer) and GOME (Global Ozone Monitoring Experiment), which is a.o. achieved by a better signal to noise ratio, improved calibration and a wide field-of-view. Moreover, in order to meet its role on Aura, OMI shall measure trace gases, such as NO2, OClO, BrO, HCHO and SO2, aerosols, cloud top height and cloud coverage. Improved accuracy, better coverage, and finer ground grid than has been done in the past are goals for OMI. After the scientific requirements are defined, three sets of subordinate requirements are derived. These are: the algorithm requirements, i.e. what do the algorithms need in order to meet the scientific requirements; the instrument and calibration requirements, i.e. what has to be measured and how accurately in order to provide the quality of data necessary for deriving the data products; and the validation requirements, i.e. a strategy of how the OMI program will assure that its data products are valid in the atmosphere, at least to the required accuracy.

Levelt, P. F.↗
NASA NTRS2003

Tropospheric Chemistry Studies using Observations from GOME and TOMS

Studies to quantitatively determine trace gas and aerosol amounts from the Global Ozone Monitoring Experiment (GOME) and the Total Ozone Monitoring Experiment (TOMS) and to perform chemical modeling studies which utilize these results are given. This includes: 1. Analysis of measurements from the GOME and TOMS instruments for troposphere distributions of O3 and HCHO; troposphere enhancements of SO2, NO2 and aerosols associated with major sources; and springtime events of elevated BrO in the lower Arctic troposphere. 2. Application of a global 3-dimensional model of troposphere chemistry to interpret the GOME observations in terms of the factors controlling the abundances of troposphere ozone and OH.

Chance, Kelly↗
NASA NTRS2003

SAO Participation in the GOME and SCIAMACHY Satellite Instrument Programs

This report summarizes the progress on our three-year program of research to refine the measurement capability for satellite-based instruments that monitor ozone and other trace species in the Earth's stratosphere and troposphere, to retrieve global distributions of these and other constituents from the GOME and SCIAMACHY satellite instruments, and to conduct scientific studies for the ILAS instruments. This continues our involvements as a U.S. participant in GOME and SCIAMACHY since their inception, and as a member of the ILAS-II Science Team. These programs have led to the launch of the first satellite instrument specifically designed to measure height-resolved ozone, including the tropospheric component (GOME), and the development of the first satellite instrument that will measure tropospheric ozone simultaneously with NO2, CO, HCHO, N2O, H2O, and CH4 (SCIAMACHY). The GOME program now includes the GOME-2 instruments, to be launched on the Eumetsat Metop satellites, providing long-term continuity in European measurements of global ozone that complement the measurements of the TOMS, SBW, OMI, OMPS instruments. The research primarily focuses on two areas: Data analysis, including algorithm development and validation studies that will improve the quality of retrieved data products, in support for future field campaigns (to complement in situ and airborne campaigns with satellite measurements), and scientific analyses to be interfaced to atmospheric modeling studies.

Chance, Kelly↗
NASA NTRS2003

EOS-Aura's Ozone Monitoring Instrument (OMI): Validation Requirements

OMI is an advanced hyperspectral instrument that measures backscattered radiation in the UV and visible. It will be flown as part of the EOS Aura mission and provide data on atmospheric chemistry that is highly synergistic with other Aura instruments HIRDLS, MLS, and TES. OMI is designed to measure total ozone, aerosols, cloud information, and UV irradiances, continuing the TOMS series of global mapped products but with higher spatial resolution. In addition its hyperspectral capability enables measurements of trace gases such as SO2, NO2, HCHO, BrO, and OClO. A plan for validation of the various OM1 products is now being formulated. Validation of the total column and UVB products will rely heavily on existing networks of instruments, like NDSC. NASA and its European partners are planning aircraft missions for the validation of Aura instruments. New instruments and techniques (DOAS systems for example) will need to be developed, both ground and aircraft based. Lidar systems are needed for validation of the vertical distributions of ozone, aerosols, NO2 and possibly SO2. The validation emphasis will be on the retrieval of these products under polluted conditions. This is challenging because they often depend on the tropospheric profiles of the product in question, and because of large spatial variations in the troposphere. Most existing ground stations are located in, and equipped for, pristine environments. This is also true for almost all NDSC stations. OMI validation will need ground based sites in polluted environments and specially developed instruments, complementing the existing instrumentation.

Brinksma, E. J.↗
NASA NTRS2004

US Team Member Participation in the Ozone Monitoring Experiment on EOS CHEM

Progress on OMI operational algorithms for BrO, OClO, and HCHO includes: A parameterization scheme for OMI instrument function lab measurements was developed for both UV and Visible instrument channels. The scheme was implemented for all three PGEs and extensively tested. PGEs now have the option of either using the parameterized lab measurements or fitting a symmetric or asymmetric Gaussian function on-line.

Chance, Kelly↗
NASA NTRS2004

US Team Member Participation in the Ozone Monitoring Experiment on EOS Chem

Progress on OMI operational algorithms for BrO, OClO, and HCHO includes: Implemented changes to PGE_Description.txt that were required to promote the PGEs to Integration. Studies were initiated for a parameterization of the laboratory measurements of the OMi instrument function for use in the PGEs. V0.9.27 of the PGEs were delivered to the DAAC.

Change, Kelly↗
NASA NTRS2003

Global 3-D Modeling Studies Of Tropospheric Ozone And Related Gases

Our research was targeted at three issues: (1) the factors controlling ozone in the tropical troposphere, (2) the Asian outflow of ozone and its precursors, and (3) the causes of decadal trends observed in ozone and CO. We have also used support from this ACMAP grant to (1) work with Kelly Chance on the retrieval and interpretation of HCHO and NO2 observations from GOME, and (2) develop GEOS-CHEM into a versatile model supporting the work of a large number of users including outside Harvard. ACMAP has provided the core support for GEOS-CHEM development. Applications of the GEOS-CHEM model with primary support from ACMAP are discussed below. A list of publications resulting from this grant is given at the end of the report.

Jacob, Daniel J.↗
NASA NTRS2004

SAO Participation in the GOME and SCIAMACHY Satellite Instrument Programs

This report summarizes the progress on our three-year program of research to refine the measurement capability for satellite-based instruments that monitor ozone and other trace species in the Earth's stratosphere and troposphere, to retrieve global distributions of these and other constituents h m the GOME and SCIAMACHY satellite instruments, and to conduct scientific studies for the ILAS instruments. This continues our involvements as a U.S. participant in GOME and SCIAMACHY since their inception, and as a member of the ILAS-II Science Team. These programs have led to the launch of the first satellite instrument specifically designed to measure height-resolved ozone, including the tropospheric component (GOME), and the development of the first satellite instrument that will measure tropospheric ozone simultaneously with NO2, CO, HCHO, N2O, H2O, and CH4 (SCIAMACHY). The GOME program now includes the GOME-2 instruments, to be launched on the Eumetsat Metop satellites, providing long-term continuity in European measurements of global ozone that complement the measurements of the TOMS, SBUV, OMI, OMPS instruments. The research primarily focuses on two areas: Data analysis, including algorithm development and validation studies that will improve the quality of retrieved data products, in support for future field campaigns (to complement in situ and airborne campaigns with satellite measurements), and scientific analyses to be interfaced to atmospheric modeling studies.

Hilsenrath, Ernest↗
NASA NTRS2005

Metabolic Reactions among Organic Sulfur Compounds

Sulfur is central to the metabolisms of many organisms that inhabit extreme environments. Numerous authors have addressed the energy available from a variety of inorganic sulfur redox pairs. Less attention has been paid, however, to the energy required or gained from metabolic reactions among organic sulfur compounds. Work in this area has focused on the oxidation of alkyl sulfide or disulfide to thiol and formaldehyde, e.g. (CH3)2S + H2O yields CH3SH + HCHO + H2, eventually resulting in the formation of CO2 and SO4(-2). It is also found that reactions among thiols and disulfides may help control redox disequilibria between the cytoplasm and the periplasm. Building on our earlier efforts for thiols, we have compiled and estimated thermodynamic properties for alkyl sulfides. We are investigating metabolic reactions among various sulfur compounds in a variety of extreme environments, ranging from sea floor hydrothermal systems to organic-rich sludge. Using thermodynamic data and the revised HKF equation of state, along with constraints imposed by the geochemical environments sulfur-metabolizing organisms inhabit, we are able to calculate the amount of energy available to these organisms.

Schulte, M.↗
NASA NTRS2005

Gases and Aerosols over North America and the Atlantic: First results from INTEX-A

Intercontinental Chemical Transport Experiment (INTEX; http://cloud1.arc.nasa.gov) is an ongoing two-phase integrated atmospheric field experiment being performed over North America (NA). Its first phase (INTEX-A) was performed in the summer of 2004 and the second phase (INTEX-B) is planned for the early spring of 2006. The main goal is to characterize the sources and distribution of gases and aerosols over NA and to understand their transport and transformation on transcontinental/intercontinental scales in order to assess their impact on air quality and climate. Central to achieving this goal is the need to relate space-based observations with those from airborne and surface platforms. During JNTEX-A, NASA s DC-8 was joined by some dozen other aircraft from a large number of European (U. K., France, and Germany) and North American partners to explore the composition of the troposphere over NA and the Atlantic in a coordinated manner. Global and regional models along with satellite observations were extensively used to plan, coordinate, and implement this field mission. Aircraft were instrumented to measure a comprehensive suite of gases and aerosols utilizing in-situ and remote sensors. The NASA DC-8 alone was equipped with some 20 instruments capable of measuring species at concentrations as low as 10(exp -15) v/v. Measurements included major atmospheric gaseous constituents (O3, NO(x), HNO3, HNO4, PANS, SO2, VOC/OVOC, CO, and CO2), free radicals and precursors (OH, HO2, H2O2, HCHO), aerosols and radiation (microphysics, composition, optical depth, radiative flux), as well as multiple tracers of pollution. Validation of instruments aboard Terra, Aqua, and Envisat satellites was given high priority. Some of the highest pollution levels were present in the upper troposphere due to widespread deep convection. Although unexpected, frequent instances of Asian pollution over NA were encountered during these summer months. The soil uptake of CO2 over NA was characterized over large regions of NA helping to understand the continents CO2-sink potential. DC-8 sampling of smoke from Alaskan fires and formaldehyde over forested regions, and simultaneous satellite observations of these provided excellent opportunities for the interplay of these platforms. Outflow of pollution from NA was sampled again over the Atlantic after several days to assess its evolution during transport. Models of chemistry and radiation are presently being employed to help in the interpretation of JNTEX-A data. The planning for INTEX-B (spring 2006) is currently underway. First results from INTEX-A and plans for INTEX-B will be discussed

Singh, Hanwant B.↗
NASA NTRS2007

Evaluation of the MOCAGE Chemistry Transport Model during the ICARTT/ITOP Experiment

We evaluate the Meteo-France global chemistry transport 3D model MOCAGE (MOdele de Chimie Atmospherique a Grande Echelle) using the important set of aircraft measurements collected during the ICARRT/ITOP experiment. This experiment took place between US and Europe during summer 2004 (July 15-August 15). Four aircraft were involved in this experiment providing a wealth of chemical data in a large area including the North East of US and western Europe. The model outputs are compared to the following species of which concentration is measured by the aircraft: OH, H2O2, CO, NO, NO2, PAN, HNO3, isoprene, ethane, HCHO and O3. Moreover, to complete this evaluation at larger scale, we used also satellite data such as SCIAMACHY NO2 and MOPITT CO. Interestingly, the comprehensive dataset allowed us to evaluate separately the model representation of emissions, transport and chemical processes. Using a daily emission source of biomass burning, we obtain a very good agreement for CO while the evaluation of NO2 points out incertainties resulting from inaccurate ratio of emission factors of NOx/CO. Moreover, the chemical behavior of O3 is satisfactory as discussed in the paper.

Bousserez, N.↗
NASA NTRS2010

Highlights from 40 Years of Satellite UV Measurements

This year we are celebrating the 40th anniversary of the launch of the Backscatter Ultraviolet (BUV) instrument on NASA's Nimbus-4 satellite. The purpose of this instrument was to demonstrate the capability to measure total column ozone and its vertical distribution from space. The success of this instrument led to about a dozen instruments of this type on various NASA and NOAA satellites. These instruments used a single photomultiplier tube (PMT) that restricted the measurements to 6-12 discrete wavelengths in the 250-380 nm range. With the availability of solid-state detector arrays in the past decade it has been possible to make similar measurements but with hyperspectral (contiguous in wavelength) sampling and enhanced spectral resolution. This has allowed global mapping of several weakly-absorbing trace gases including S0 2, NO2, BrO, HCHO, and CIIOCHO. Since these measurements are affected by clouds and aerosols, a great deal of effort has gone into understanding their effect on ultraviolet radiation- both upwelling and downwelling. The downwelling UV radiation is chemically and biologically active and has both negative (genetic damage, air pollution) and positive (production of vitamin D and OH radical) environmental effects. I will discuss how the interaction of Rayleigh-scattered UV radiation with clouds and aerosols produce a variety of interesting effects that are leading to new methods of remote sensing of their properties. The UV measurements can greatly enhance the information that one derives from more traditional methods that use infrared and visible part of the solar spectrum.

Bhartia, Pawan K.↗
NASA NTRS2012

The Cabauw Intercomparison Campaign for Nitrogen Dioxide Measuring Instruments (CINDI): Design, Execution, and Early Results

From June to July 2009 more than thirty different in-situ and remote sensing instruments from all over the world participated in the Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI). The campaign took place at KNMI's Cabauw Experimental Site for Atmospheric Research (CESAR) in the Netherlands. Its main objectives were to determine the accuracy of state-ofthe- art ground-based measurement techniques for the detection of atmospheric nitrogen dioxide (both in-situ and remote sensing), and to investigate their usability in satellite data validation. The expected outcomes are recommendations regarding the operation and calibration of such instruments, retrieval settings, and observation strategies for the use in ground-based networks for air quality monitoring and satellite data validation. Twenty-four optical spectrometers participated in the campaign, of which twenty-one had the capability to scan different elevation angles consecutively, the so-called Multi-axis DOAS systems, thereby collecting vertical profile information, in particular for nitrogen dioxide and aerosol. Various in-situ samplers and lidar instruments simultaneously characterized the variability of atmospheric trace gases and the physical properties of aerosol particles. A large data set of continuous measurements of these atmospheric constituents has been collected under various meteorological conditions and air pollution levels. Together with the permanent measurement capability at the CESAR site characterizing the meteorological state of the atmosphere, the CINDI campaign provided a comprehensive observational data set of atmospheric constituents in a highly polluted region of the world during summertime. First detailed comparisons performed with the CINDI data show that slant column measurements of NO2, O4 and HCHO with MAX-DOAS agree within 5 to 15%, vertical profiles of NO2 derived from several independent instruments agree within 25% of one another, and MAX-DOAS aerosol optical thickness agrees within 20-30% with AERONET data. For the in-situ NO2 instrument using a molybdenum converter, a bias was found as large as 5 ppbv during day time, when compared to the other in-situ instruments using photolytic converters.

Atmospheric composition↗
NASA NTRS2012

Typical Types and Formation Mechanisms of Haze in an Eastern Asia Megacity, Shanghai

An intensive aerosol and gases campaign was performed at Shanghai in the Yangtze River Delta region over Eastern China from late March to early June 2009. This study provided a complementary picture of typical haze types and the formation mechanisms in megacities over China by using a synergy of ground-based monitoring, satellite and lidar observations. During the whole study period, several extreme low visibility periods were observed with distinct characteristics, and three typical haze types were identified, i.e. secondary inorganic pollution, dust, and biomass burning. Sulfate, nitrate and ammonium accounted for a major part of PM2.5 mass during the secondary inorganic pollution, and the good correlation between SO2/NOx/CO and PM2.5 indicated that coal burning and vehicle emission were the major sources. Large-scale regions with high AOD (aerosol optical depths) and low Angstrom exponent were detected by remote-sensing observation during the dust pollution episode, and this episode corresponded to coarse particles rich in mineral components such as Al and Ca contributing 76.8% to TSP. The relatively low Ca/Al ratio of 0.75 along with the air mass backward trajectory analysis suggested the dust source was from Gobi Desert. Typical tracers for biomass burning from satellite observation (column CO and HCHO) and from ground measurement (CO, particulate K+, OC, and EC) were greatly enhanced during the biomass burning pollution episode. The exclusive linear correlation between CO and PM2.5 corroborated that organic aerosol dominated aerosol chemistry during biomass burning, and the high concentration and enrichment degree of arsenic (As) could be also partly derived from biomass burning. Aerosol optical profile observed by lidar demonstrated that aerosol was mainly constrained below the boundary layer and comprised of spheric aerosol (depolarization ratio <5%) during the secondary inorganic and biomass burning episodes, while thick dust layer distributed at altitudes from near surface to 1.4 km (average depolarization ratio = 0.122+/-0.023) with dust accounting for 44-55% of the total aerosol extinction coefficient during the dust episode. This study portrayed a good picture of the typical haze types and proposed that identification of the complicated emission sources is important for the air quality improvement in megacities in China.

haze↗
NASA NTRS2014

Wildfire Emissions and Their Interaction with Urban and Rural Pollution: Data and Simulations

In recent years NASA has conducted a series of airborne campaigns (e. g. SEAC4RS*, ARCTAS, INTEX-A/B) over North America using an instrumented DC-8 aircraft equipped to measure a very large number of gaseous and aerosol constituents including several unique tracers. In these campaigns wild fires were extensively sampled near source as well as downwind after aging. The data provided detailed information on the composition and chemistry of fire emissions under a variety of atmospheric conditions as well as their interactions with rural and urban air pollution. Major fires studied including the California Rim fire in 2013 (SEAC4RS), the 2008 California wildfires (ARCTAS), and the Alaskan fires downwind over eastern US (INTEX-A). Although some fire plumes contained virtually no O3 enhancement, others showed significant ozone formation. Over Los Angeles, the highest O3 mixing ratios were observed in fire influenced urban air masses. Attempts to simulate these interactions using state of the art models were only minimally successful and indicated several shortcomings in simulating fire emission influences on urban smog formation. A variety of secondary oxidation products (e. g. O3, PAN, HCHO) were substantially underestimated. We will discuss the data collected in fire influenced air masses and their potential air quality implications.

FIre Emissions↗
NASA NTRS2015

Spatial and Temporal Variability of Trace Gas Columns Derived from WRF/Chem Regional Model Output: Planning for Geostationary Observations of Atmospheric Composition

We quantify both the spatial and temporal variability of column integrated O3, NO2, CO, SO2, and HCHO over the Baltimore / Washington, DC area using output from the Weather Research and Forecasting model with on-line chemistry (WRF/Chem) for the entire month of July 2011, coinciding with the first deployment of the NASA Earth Venture program mission Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ). Using structure function analyses, we find that the model reproduces the spatial variability observed during the campaign reasonably well, especially for O3. The Tropospheric Emissions: Monitoring of Pollution (TEMPO) instrument will be the first NASA mission to make atmospheric composition observations from geostationary orbit and partially fulfills the goals of the Geostationary Coastal and Air Pollution Events (GEO-CAPE) mission. We relate the simulated variability to the precision requirements defined by the science traceability matrices of these space-borne missions. Results for O3 from 0- 2 km altitude indicate that the TEMPO instrument would be able to observe O3 air quality events over the Mid-Atlantic area, even on days when the violations of the air quality standard are not widespread. The results further indicated that horizontal gradients in CO from 0-2 km would be observable over moderate distances (≥ 20 km). The spatial and temporal results for tropospheric column NO2 indicate that TEMPO would be able to observe not only the large urban plumes at times of peak production, but also the weaker gradients between rush hours. This suggests that the proposed spatial and temporal resolutions for these satellites as well as their prospective precision requirements are sufficient to answer the science questions they are tasked to address.

TEMPO↗