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All sourcesNASA NTRSDOE OSTI
NASA NTRS2001

Satellite Observations of Tropospheric Chemistry

The troposphere is an essential component of the earth's life support system as well as the gateway for the exchange of chemicals between different geochemical reservoirs of the earth. The chemistry of the troposphere is sensitive to perturbation from a wide range of natural phenomena and human activities. The societal concern has been greatly enhanced in recent decades due to ever increasing pressures of population growth and industrialization. Chemical changes within the troposphere control a vast array of processes that impact human health, the biosphere, and climate. A main goal of tropospheric chemistry research is to measure and understand the response of atmospheric composition to natural and anthropogenic perturbations, and to develop the capability to predict future change. Atmospheric chemistry measurements are extremely challenging due to the low concentrations of critical species and the vast scales over which the observations must be made. Available tropospheric data are mainly from surface sites and aircraft missions. Because of the limited temporal extent of aircraft observations, we have very limited information on tropospheric composition above the surface. This situation can be contrasted to the stratosphere, where satellites have provided critical and detailed chemical data on the global distribution of key trace gases.

Singh, Hanwant B.↗
NASA NTRS2001

Chemistry-Climate Interactions in the GISS GCM: Tropospheric Chemistry Model Description and Evaluation - Part 1

A tropospheric chemistry module has been developed for use within the Goddard Institute for Space Studies (GISS) general circulation model (GCM) to study interactions between chemistry and climate change. The model uses a simplified chemistry scheme based on CO-NOx-CH4 chemistry, and also includes a parameterization for emissions of isoprene, the most important non-methane hydrocarbon. The model reproduces present day annual cycles and mean distributions of key trace gases fairly well, based on extensive comparisons with available observations. Examining the simulated change between present day and pre-industrial conditions, we find that the model has a similar response to that seen in other simulations. It shows a 45% increase in the global tropospheric ozone burden, within the 25% - 57% range seen in other studies. Annual average zonal mean ozone increases by more than 125% at Northern Hemisphere middle latitudes near the surface. Comparison of model runs that allow the calculated ozone to interact with the GCM's radiation and meteorology with those that do not shows only minor differences for ozone. The common usage of ozone fields that are not calculated interactively seems to be adequate to simulate both the present day and the pre-industrial ozone distributions. However, use of coupled chemistry does alter the change in tropospheric oxidation capacity, enlarging the overall decrease in OH concentrations from the pre-industrial to the present by about 10% (-5.3% global annual average in uncoupled mode, -5.9% in coupled mode). This indicates that there may be systematic biases in the simulation of the pre-industrial to present day decrease in the oxidation capacity of the troposphere (though a 10% difference is well within the total uncertainty). Global annual average radiative forcing from pre-industrial to present day ozone change is 0.32 W/sq m. The forcing seems to be increased by about 10% when the chemistry is coupled to the GCM. Forcing values greater than 0.8 W/sq m are seen over large areas of the United States, Southern Europe, North Africa, the Middle East, Central Asia, and the Arctic. Radiative forcing is greater than 1.5 W/sq m over parts of these areas during Northern summer Though there are local differences, the radiative forcing is overall in good agreement with the results of other modeling studies in both its magnitude and spatial distribution, demonstrating that the simplified chemistry is adequate for climate studies.

Shindell, Drew T.↗
NASA NTRS1987

Lidar measurements from space for tropospheric chemistry investigations: Summary of workshop overview presentation

Over the past decade, NASA has played a lead role in defining the scientific objectives and technology requirements for spaceborne lidar investigations of the atmosphere. An assessment of the potential for conducting lidar measurements from space for investigations that pertain specifically to tropospheric chemistry is presented. A description of potential lidar measurement techniques is given, and the scientific requirements for tropospheric chemistry are reviewed. The current status of airborne lidar measurements of aerosols, O3, and H2O is discussed, and a brief description of the evolution of lidar technology to space is given. Also, the measurement of tropospheric gases with a spaceborne lidar system is evaluated for a wide range of gas species. From this general assessment, it appears feasible to measure aerosols, H2O, O3, NH3, CO, CH4, NO2, atmospheric pressure and temperature, and wind with a lidar from space provided that the appropriate laser and receiver technology is available. For the mid-1990's, it is expected that lidar technology will be available for the measurement of aerosols, H2O, and O3 from a space platform.

Browell, Edward V.↗
NASA NTRS1983

Proceedings of a Workshop on Research Needs in Heterogeneous Tropospheric Chemistry

The role of heterogeneous reactions and processes in the troposphere is critically assessed. The results of this assessment, including identification and prioritization of a number of important and scientifically tractable processes, as well as recommendations of ways in which they can be incorporated into the existing NASA tropospheric chemistry program are presented. Also presented is a detailed summary of the considerations that led to the group's recommendations.

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NASA NTRS1984

Tropospheric Chemistry

The fundamental processes that control the chemical composition and cycles of the global troposphere and how these processes and properties affect the physical behavior of the atmosphere are examined. The long-term information needs for tropospheric chemistry are: to be able to predict tropospheric responses to perturbations, both natural and anthropogenic, of these cycles, and to provide the information required for the maintenance and effective future management of the atmospheric component of our global life support system. The processes controlling global tropospheric biogeochemical cycles include: the input of trace species into the troposphere, their long-range transport and distribution as affected by the mean wind and vertical venting, their chemical transformations, including gas to particle conversion, leading to the appearance of aerosols or aqueous phase reactions inside cloud droplets, and their removal from the troposphere via wet (precipitation) and dry deposition.

Mohnen, V.↗
NASA NTRS2003

Impact of Flow-Dependent Error Correlations and Tropospheric Chemistry on Assimilated Ozone

The presentation compares different versions of a global three-dimensional ozone data assimilation system developed at NASA's Data Assimilation Office. The Solar Backscatter Ultraviolet/2 (SBUV/2) total and partial ozone column retrievals are the sole data assimilated in all of the experiments presented. We study the impact of changing the forecast error covariance model from a version assuming static correlations with a one that captures a short-term Lagrangian evolution of those correlations. This is further combined with a study of the impact of neglecting the tropospheric ozone production, loss and dry deposition rates, which are obtained from the Harvard GEOS-CHEM model. We compare statistical characteristics of the assimilated data and the results of validation against independent observations, obtained from WMO balloon-borne sondes and the Polar Ozone and Aerosol Measurement (POAM) III instrument. Experiments show that allowing forecast error correlations to evolve with the flow results in positive impact on assimilated ozone within the regions where data were not assimilated, particularly at high latitudes in both hemispheres. On the other hand, the main sensitivity to tropospheric chemistry is in the Tropics and sub-Tropics. The best agreement between the assimilated ozone and the in-situ sonde data is in the experiment using both flow-dependent error covariances and tropospheric chemistry.

Wargan, K.↗
NASA NTRS2000

Tropospheric Chemistry from Space

Measuring tropospheric chemical constituents from space has been only of the "Holy Grails" of remote sensing. Tropospheric remote sensing has been done in two phases, extracting troposheric constituent information from satellite instruments designed for other purposes and constituent measurements with instruments optimized for tropospheric detection. Examples from the first phase, tropospheric ozone and aerosols from Total Ozone Mapping Spectrometer (TOMS) and Global Ozone Monitoring Experiment (GOME) will be presented. Expected results from upcoming instruments and missions, Atmospheric Ultraviolet Radiance Analyzer (AURA), Ozone Monitoring Instrument (OMI), GOME2, and Scanning Imaging Spectrometer for Atmospheric Chartography (SCIAMACHY) will be presented.

Gleason, James↗
NASA NTRS1984

Global tropospheric chemistry: A plan for action

Prompted by an increasing awareness of the influence of human activity on the chemistry of the global troposphere, a panel was formed to (1) assess the requirement for a global study of the chemistry of the troposphere; (2) develop a scientific strategy for a comprehensive plan taking into account the existing and projected programs of the government; (3) assess the requirements of a global study in terms of theoretical knowledge, numerical modeling, instrumentation, observing platforms, ground-level observational techniques, and other related needs; and (4) outline the appropriate sequence and coordination required to achieve the most effective utilization of available resources. Part 1 presents a coordinated national blueprint for scientific investigations of biogeochemical cycles in the global troposphere. part 2 presents much of the background information of the present knowledge and gaps in the understanding of tropospheric chemical cycles and processes from which the proposed program was developed.

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NASA NTRS2001

Global Modeling of Tropospheric Chemistry with Assimilated Meteorology: Model Description and Evaluation

We present a first description and evaluation of GEOS-CHEM, a global three-dimensional (3-D) model of tropospheric chemistry driven by assimilated meteorological observations from the Goddard Earth Observing System (GEOS) of the NASA Data Assimilation Office (DAO). The model is applied to a 1-year simulation of tropospheric ozone-NOx-hydrocarbon chemistry for 1994, and is evaluated with observations both for 1994 and for other years. It reproduces usually to within 10 ppb the concentrations of ozone observed from the worldwide ozonesonde data network. It simulates correctly the seasonal phases and amplitudes of ozone concentrations for different regions and altitudes, but tends to underestimate the seasonal amplitude at northern midlatitudes. Observed concentrations of NO and peroxyacetylnitrate (PAN) observed in aircraft campaigns are generally reproduced to within a factor of 2 and often much better. Concentrations of HNO3 in the remote troposphere are overestimated typically by a factor of 2-3, a common problem in global models that may reflect a combination of insufficient precipitation scavenging and gas-aerosol partitioning not resolved by the model. The model yields an atmospheric lifetime of methylchloroform (proxy for global OH) of 5.1 years, as compared to a best estimate from observations of 5.5 plus or minus 0.8 years, and simulates H2O2 concentrations observed from aircraft with significant regional disagreements but no global bias. The OH concentrations are approximately 20% higher than in our previous global 3-D model which included an UV-absorbing aerosol. Concentrations of CO tend to be underestimated by the model, often by 10-30 ppb, which could reflect a combination of excessive OH (a 20% decrease in model OH could be accommodated by the methylchloroform constraint) and an underestimate of CO sources (particularly biogenic). The model underestimates observed acetone concentrations over the South Pacific in fall by a factor of 3; a missing source from the ocean may be implicated.

Bey, Isabelle↗
NASA NTRS1985

Tropospheric chemistry

The chemistry of the background troposphere, the source region, and the transition regions are discussed. The troposphere is governed by heterogeneous chemistry far more so than the stratosphere. Heterogeneous processes of interest involve scavenging of trace gases by aerosols, cloud and precipitation elements leading to aqueous phase chemical reactions and to temporary and permanent removal of material from the gas phase. Dry deposition is a major removal process for ozone, as well as for other gases of importance in tropospheric photochemistry. These processes are also discussed.

Mohnen, V. A.↗
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 NTRS2005

Linking Urban Air Pollution to Global Tropospheric Chemistry and Climate

The two major tasks of this project are to study: (a) the impact of urban nonlinear chemistry on chemical budgets of key pollutants in non-urban areas; and (b) the influence of air pollution control strategies in selected metropolitan areas, particularly of emerging economies in East and South Asia, on tropospheric chemistry and hence on regional and global climate.

Wang, Chien↗
NASA NTRS1994

Estimates of the changes in tropospheric chemistry which result from human activity and their dependence on NO(x) emissions and model resolution

As a consequence of the non-linear behavior of the chemistry of the atmosphere and because of the short lifetime of nitrogen oxides (NO(x)), two-dimensional models do not give an adequate description of the production and destruction rates of NO(x) and their effects on the distributions of the concentration of ozone and hydroxyl radical. In this study, we use a three-dimensional model to evaluate the contribution of increasing NO(x) emissions from industrial activity and biomass burning to changes in the chemical composition of the troposphere. By comparing results obtained from longitudinally-uniform and longitudinally-varying emissions of NO(x), we demonstrate that the geographical representation of the NO(x) emissions is crucial in simulating tropospheric chemistry.

Kanakidou, Maria↗
NASA NTRS1994

The sensitivity of tropospheric chemistry to cloud interactions

Clouds, although only occupying a relatively small fraction of the troposphere volume, can have a substantial impact on the chemistry of the troposphere. In newly formed clouds, or in clouds with air rapidly flowing through, the chemistry is expected to be far more active than in aged clouds with stagnant air. Thus, frequent cycling of air through shortlived clouds, i.e. cumulus clouds, is likely to be a much more efficient media for altering the composition of the atmosphere than an extensive cloud cover i.e. frontal cloud systems. The impact of clouds is tested out in a 2-D channel model encircling the globe in a latitudinal belt from 30 to 60 deg N. The model contains a detailed gas phase chemistry. In addition physiochemical interactions between the gas and aqueous phases are included. For species as H2O2, CH2O, O3, and SO2, Henry's law equilibria are assumed, whereas HNO3 and H2SO4 are regarded as completed dissolved in the aqueous phase. Absorption of HO2 and OH is assumed to be mass-transport limited. The chemistry of the aqueous phase is characterized by rapid cycling of odd hydrogen, (H2O2, HO2, and OH). O2(-) (produced through dissociation of HO2) reacting with dissolved O3 is a major source of OH in the aqueous phase. This reaction can be a significant sink for O3 in the troposphere. In the interstitial cloud air, odd hydrogen is depleted, whereas NO(x) remains in the gas phase, thus reducing ozone production due to the reaction between NO and HO2. Our calculations give markedly lower ozone levels when cloud interactions are included. This may in part explain the overpredictions of ozone levels often experienced in models neglecting cloud chemical interactions. In the present study, the existence of clouds, cloud types, and their lifetimes are modeled as pseudo random variables. Such pseudo random sequences are in reality deterministic and may, given the same starting values, be reproduced. The effects of cloud interactions on the overall chemistry of the troposphere are discussed. In particular, tests are performed to determine the sensitivity of cloud frequencies and cloud types.

Jonson, Jan E.↗
NASA NTRS1981

Tropospheric chemistry - A global perspective

Processes that affect the concentration of tropospheric OH are considered, taking into account linkages between the chemistry of OH and the chemistry of H, HO2, and H2O2. A review is presented of observational data of special relevance to OH, notably the distributions of CO, CH4, O3, H2O, HNO3, NO, and NO2. Most of the results presented in connection with the description of the model were obtained by solving time-dependent continuity equations. Rates for photolytic processes were allowed to vary diurnally with insolation. It is found that a well-calibrated and reliable model for OH places important constraints on global budgets for a variety of gases including CH4, H2, and CH3Cl in addition to CO. Accurate measurements of species such as CH3CCl3 can provide valuable checks on global models that must integrate over a variety of atmospheric conditions. However, emission rates for the relevant gases must be adequately quantified.

Logan, J. A.↗