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

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NASA NTRS2016

Regional and Global Climate Response to Anthropogenic SO2 Emissions from China in Three Climate Models

We use the HadGEM3-GA4, CESM1, and GISS ModelE2 climate models to investigate the global and regional aerosol burden, radiative flux, and surface temperature responses to removing anthropogenic sulfur dioxide (SO2) emissions from China. We find that the models differ by up to a factor of 6 in the simulated change in aerosol optical depth (AOD) and shortwave radiative flux over China that results from reduced sulfate aerosol, leading to a large range of magnitudes in the regional and global temperature responses. Two of the three models simulate a near-ubiquitous hemispheric warming due to the regional SO2 removal, with similarities in the local and remote pattern of response, but overall with a substantially different magnitude. The third model simulates almost no significant temperature response. We attribute the discrepancies in the response to a combination of substantial differences in the chemical conversion of SO2 to sulfate, translation of sulfate mass into AOD, cloud radiative interactions, and differences in the radiative forcing efficiency of sulfate aerosol in the models. The model with the strongest response (HadGEM3-GA4) compares best with observations of AOD regionally, however the other two models compare similarly (albeit poorly) and still disagree substantially in their simulated climate response, indicating that total AOD observations are far from sufficient to determine which model response is more plausible. Our results highlight that there remains a large uncertainty in the representation of both aerosol chemistry as well as direct and indirect aerosol radiative effects in current climate models, and reinforces that caution must be applied when interpreting the results of modelling studies of aerosol influences on climate. Model studies that implicate aerosols in climate responses should ideally explore a range of radiative forcing strengths representative of this uncertainty, in addition to thoroughly evaluating the models used against observations.

sulfates↗
DOE OSTI2021

Industrial emission inventories of iron and phosphorus for past, present and future

Global emission inventories of aerosol iron by species, and of phosphorus, were developed for inclusion in Earth system modeling that includes atmospheric transport. The time period covered was 1850-2010 to evaluate human influence. A variety of approaches to compare measured and modeled values of aerosol iron was synthesized to estimate how well anthropogenic emissions are known. Anthropogenic emissions are constrained within a factor of two and if there is a bias, it is an overestimation. The exception is shipping emissions, which may be underestimated. Direct radiative forcing by iron aerosol is small in the global average (0.02 W m -2 ) but reaches 0.25 W m -2 around source regions. Regions of high direct radiative forcing are poorly constrained by observations. The central value of change in oceanic net primary productivity due to iron deposition is about 0.26 PgC yr -1 , also highly localized. This leads to a decrease in atmospheric CO2 accumulation that corresponds to a forcing of 0.008 W m -2 since 1850 (0.003-0.18 W m -2 ). Emissions of particulate matter to 2050 were estimated in response to different policy scenarios, including the need for renewable energy installations under decarbonization scenarios. Under the business-as-usual scenario, the total metal demand is 195 Mt/yr in 2020, peaking at 270 Mt/yr in years 2040-2045; under the Rapid Decarbonization scenario, total metal demand is nearly doubled at its peak: 480 Mt/yr in year 2040. Primary particulate matter emissions attributable to processing metals for renewable energy are also amplified under rapid decarbonization, but total atmospheric emissions are much lower because of the shift away from combustion.

58 GEOSCIENCES↗
NASA NTRS2022

Pre- and Post-Production Processes Increasingly Dominate Greenhouse Gas Emissions From Agri-Food Systems

We present results from the FAOSTAT emissions shares database, covering emissions from agri-food systems and their shares to total anthropogenic emissions for 196 countries and 40 territories for the period 1990–2019. We find that in 2019, global agri-food system emissions were 16.5 (95 %; CI range: 11–22) billion metric tonnes (GtCO2 eq. yr(exp -1)), corresponding to 31%(range: 19 %–43 %) of total anthropogenic emissions. Of the agri-food system total, global emissions within the farm gate – from crop and livestock production processes including on-farm energy use – were 7.2 GtCO2 eq. yr(exp -1); emissions from land use change, due to deforestation and peatland degradation, were 3.5 GtCO2 eq. yr(exp -1); and emissions from pre- and post-production processes – manufacturing of fertilizers, food processing, packaging, transport, retail, household consumption and food waste disposal – were 5.8 GtCO2 eq. yr(exp -1). Over the study period 1990–2019, agri-food system emissions increased in total by 17 %, largely driven by a doubling of emissions from pre- and post-production processes. Conversely, the FAOSTAT data show that since 1990 land use emissions decreased by 25 %, while emissions within the farm gate increased 9 %. In 2019, in terms of individual greenhouse gases (GHGs), pre- and postproduction processes emitted the most CO2 (3.9 GtCO2 yr(exp -1)), preceding land use change (3.3 GtCO2 yr(exp -1)) and farm gate (1.2 GtCO2 yr(exp -1)) emissions. Conversely, farm gate activities were by far the major emitter of methane (140 MtCH4 yr(exp -1)) and of nitrous oxide (7.8 MtN2Oyr(exp -1)). Pre- and post-production processes were also significant emitters of methane (49 MtCH4 yr(exp -1)), mostly generated from the decay of solid food waste in landfills and open dumps. One key trend over the 30-year period since 1990 highlighted by our analysis is the increasingly important role of food-related emissions generated outside of agricultural land, in pre- and post-production processes along the agri-food system, at global, regional and national scales. In fact, our data show that by 2019, pre- and post-production processes had overtaken farm gate processes to become the largest GHG component of agri-food system emissions in Annex I parties (2.2 GtCO2 eq. yr(exp -1)). They also more than doubled in non-Annex I parties (to 3.5 GtCO2 eq. yr(exp -1)), becoming larger than emissions from land use change. By 2019 food supply chains had become the largest agri-food system component in China (1100 MtCO2 eq. yr(exp -1)), the USA (700 MtCO2 eq. yr(exp -1)) and the EU-27 (600 MtCO2 eq. yr(exp -1)). This has important repercussions for food-relevant national mitigation strategies, considering that until recently these have focused mainly on reductions of non-CO2 gases within the farm gate and on CO2 mitigation from land use change. The information used in this work is available as open data with DOI https://doi.org/10.5281/zenodo.5615082 (Tubiello et al., 2021d). It is also available to users via the FAOSTAT database (https://www.fao.org/faostat/en/#data/EM; FAO, 2021a), with annual updates.

FAOSTAT agri-food systems emissions database↗
NASA NTRS2016

Tropospheric Ozone Change from 1980 to 2010 Dominated by Equatorward Redistribution of Emissions

Ozone is an important air pollutant at the surface, and the third most important anthropogenic greenhouse gas in the troposphere. Since 1980, anthropogenic emissions of ozone precursors methane, non-methane volatile organic compounds, carbon monoxide and nitrogen oxides (NOx) have shifted from developed to developing regions. Emissions have thereby been redistributed equatorwards, where they are expected to have a stronger effect on the tropospheric ozone burden due to greater convection, reaction rates and NOx sensitivity. Here we use a global chemical transport model to simulate changes in tropospheric ozone concentrations from 1980 to 2010, and to separate the influences of changes in the spatial distribution of global anthropogenic emissions of short-lived pollutants, the magnitude of these emissions, and the global atmospheric methane concentration. We estimate that the increase in ozone burden due to the spatial distribution change slightly exceeds the combined influences of the increased emission magnitude and global methane. Emission increases in Southeast, East and South Asia may be most important for the ozone change, supported by an analysis of statistically significant increases in observed ozone above these regions. The spatial distribution of emissions dominates global tropospheric ozone, suggesting that the future ozone burden will be determined mainly by emissions from low latitudes.

Zhang, Yuqiang↗
NASA NTRS2017

Developing and Diagnosing Climate Change Indicators of Regional Aerosol Optical Properties

Given the importance of aerosol particles to radiative transfer via aerosol-radiation interactions, a methodology for tracking and diagnosing causes of temporal changes in regional-scale aerosol populations is illustrated. The aerosol optical properties tracked include estimates of total columnar burden (aerosol optical depth, AOD), dominant size mode (Ångström exponent, AE), and relative magnitude of radiation scattering versus absorption (single scattering albedo, SSA), along with metrics of the structure of the spatial field of these properties. Over well-defined regions of North America, there are generally negative temporal trends in mean and extreme AOD, and SSA. These are consistent with lower aerosol burdens and transition towards a relatively absorbing aerosol, driven primarily by declining sulfur dioxide emissions. Conversely, more remote regions are characterized by increasing mean and extreme AOD that is attributed to increased local wildfire emissions and long-range (transcontinental) transport. Regional and national reductions in anthropogenic emissions of aerosol precursors are leading to declining spatial autocorrelation in the aerosol fields and increased importance of local anthropogenic emissions in dictating aerosol burdens. However, synoptic types associated with high aerosol burdens are intensifying (becoming more warm and humid), and thus changes in synoptic meteorology may be offsetting aerosol burden reductions associated with emissions legislation.

Ryan C Sullivan↗
NASA NTRS2013

Evaluation of GEOS-5 Sulfur Dioxide Simulations During the Frostburg, MD 2010 Field Campaign.

Sulfur dioxide (SO2) is a major atmospheric pollutant with a strong anthropogenic component mostly produced by the combustion of fossil fuel and other industrial activities. As a precursor of sulfate aerosols that affect climate, air quality, and human health, this gas needs to be monitored on a global scale. Global climate and chemistry models including aerosol processes along with their radiative effects are important tools for climate and air quality research. Validation of these models against in-situ and satellite measurements is essential to ascertain the credibility of these models and to guide model improvements. In this study the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) module running on-line inside the Goddard Earth Observing System version 5 (GEOS-5) model is used to simulate aerosol and SO2 concentrations. Data taken in November 2010 over Frostburg, Maryland during an SO2 field campaign involving ground instrumentation and aircraft are used to evaluate GEOS-5 simulated SO2 concentrations. Preliminary data analysis indicated the model overestimated surface SO2 concentration, which motivated the examination of mixing processes in the model and the specification of SO2 anthropogenic emission rates. As a result of this analysis, a revision of anthropogenic emission inventories in GEOS-5 was implemented, and the vertical placement of SO2 sources was updated. Results show that these revisions improve the model agreement with observations locally and in regions outside the area of this field campaign. In particular, we use the ground-based measurements collected by the United States Environmental Protection Agency (US EPA) for the year 2010 to evaluate the revised model simulations over North America.

Air Quality Campaign↗
NASA NTRS2019

Toward Improving Short-Term Predictions of Fine Particulate Matter Over the United States Via Assimilation of Satellite Aerosol Optical Depth Retrievals

This study develops a new approach to improve simulations of the particulate matter of aerodynamic diameter smaller than 2.5μm (PM2.5) in the Community Multiscale Air Quality (CMAQ) model via assimilation of Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical depth(AOD) retrievals using the Grid point Statistical Interpolation (GSI) system. In contrast to previous studies that only consider errors due to transport, our computation of the background error covariance matrix incorporates uncertainties in anthropogenic emissions. To understand the impact of this approach, three experiments (one background and two assimilations) are performed over the contiguous United States(CONUS) from 15 July to 14 August 2014. The background CMAQ experiment significantly underestimates both the MODIS AOD and surface PM2.5levels. MODIS AOD assimilation pushes both the CMAQ AOD and surface PM2.5distributions toward the observed distributions, but CMAQ still underestimates the observations. Averaged over CONUS, the two assimilation experiments with and without including the anthropogenic emission uncertainties improve the correlation coefficient between the model and independent observations of PM2.5 by ~67% and ~48%, respectively, and reduces the mean bias by ~38% and~10%, respectively. The assimilation improves the model performance everywhere over CONUS, except the New York and Wisconsin, where CMAQ overestimates the observed PM2.5during nighttime after assimilation likely because of overcorrection of aerosol mass concentrations by the AOD assimilation. Future work should incorporate uncertainties in other processes (biomass burning and biogenic emissions, deposition, chemistry, transport, and boundary conditions) to further enhance the value of assimilating spaceborne AOD retrievals.

Assimilation↗
DOE OSTI2022

Atmospheric Radiative and Oceanic Biological Productivity Responses to Increasing Anthropogenic Combustion‐Iron Emission in the 1850–2010 Period

Abstract Anthropogenic emission is an important component of the present‐day iron cycle yet its long‐term impacts on climate are poorly understood. Iron mineralogy strongly affects its radiative and oceanic interactions and was unrepresented in previous studies. We perform simulations using a mineralogy‐based inventory and an atmospheric transport model and estimate the 1850–2010 global mean direct radiative forcing (DRF) to be +0.02 to +0.10 W/m 2 . We estimate that the CO 2 sequestration of 0.2–13 ppmv over the last 150 years due to enhanced phytoplankton productivity by anthropogenic iron deposition causes an avoided CO 2 forcing of −0.002 to −0.16 W/m 2 . While globally small, these impacts can be higher in specific regions; the anthropogenic DRF is +0.5 W/m 2 over areas with more coal combustion and metal smelting, and anthropogenic soluble iron sustains >10% of marine net primary productivity in the high‐latitude North Pacific Ocean, a region vulnerable to stratification due to climate change.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

A comprehensive and synthetic dataset for global, regional, and national greenhouse gas emissions by sector 1970–2018 with an extension to 2019

To track progress towards keeping global warming well below 2 °C or even 1.5 °C, as agreed in the Paris Agreement, comprehensive up-to-date and reliable information on anthropogenic emissions and removals of greenhouse gas (GHG) emissions is required. Here we compile a new synthetic dataset on anthropogenic GHG emissions for 1970–2018 with a fast-track extension to 2019. Our dataset is global in coverage and includes CO 2 emissions, CH 4 emissions, N 2 O emissions, as well as those from fluorinated gases (F-gases: HFCs, PFCs, SF 6 , NF 3 ) and provides country and sector details. We build this dataset from the version 6 release of the Emissions Database for Global Atmospheric Research (EDGAR v6) and three bookkeeping models for CO 2 emissions from land use, land-use change, and forestry (LULUCF). We assess the uncertainties of global greenhouse gases at the 90 % confidence interval (5th–95th percentile range) by combining statistical analysis and comparisons of global emissions inventories and top-down atmospheric measurements with an expert judgement informed by the relevant scientific literature. We identify important data gaps for F-gas emissions. The agreement between our bottom-up inventory estimates and top-down atmospheric-based emissions estimates is relatively close for some F-gas species (~ 10 % or less), but estimates can differ by an order of magnitude or more for others. Our aggregated F-gas estimate is about 10 % lower than top-down estimates in recent years. However, emissions from excluded F-gas species such as chlorofluorocarbons (CFCs) or hydrochlorofluorocarbons (HCFCs) are cumulatively larger than the sum of the reported species. Using global warming potential values with a 100-year time horizon from the Sixth Assessment Report by the Intergovernmental Panel on Climate Change (IPCC), global GHG emissions in 2018 amounted to 58 ± 6.1 GtCO 2 eq. consisting of CO 2 from fossil fuel combustion and industry (FFI) 38 ± 3.0 GtCO 2 , CO 2 -LULUCF 5.7 ± 4.0 GtCO 2 , CH 4 10 ± 3.1 GtCO 2 eq., N2O 2.6 ± 1.6 GtCO 2 eq., and F-gases 1.3 ± 0.40 GtCO 2 eq. Initial estimates suggest further growth of 1.3 GtCO 2 eq. in GHG emissions to reach 59 ± 6.6 GtCO 2 eq. by 2019. Our analysis of global trends in anthropogenic GHG emissions over the past 5 decades (1970–2018) highlights a pattern of varied but sustained emissions growth. There is high confidence that global anthropogenic GHG emissions have increased every decade, and emissions growth has been persistent across the different (groups of) gases. There is also high confidence that global anthropogenic GHG emissions levels were higher in 2009–2018 than in any previous decade and that GHG emissions levels grew throughout the most recent decade. While the average annual GHG emissions growth rate slowed between 2009 and 2018 (1.2 % yr –1 ) compared to 2000–2009 (2.4 % yr –1 ), the absolute increase in average annual GHG emissions by decade was never larger than between 2000–2009 and 2009–2018. Our analysis further reveals that there are no global sectors that show sustained reductions in GHG emissions. There are a number of countries that have reduced GHG emissions over the past decade, but these reductions are comparatively modest and outgrown by much larger emissions growth in some developing countries such as China, India, and Indonesia. There is a need to further develop independent, robust, and timely emissions estimates across all gases. As such, tracking progress in climate policy requires substantial investments in independent GHG emissions accounting and monitoring as well as in national and international statistical infrastructures. The data associated with this article (Minx et al., 2021) can be found at https://doi.org/10.5281/zenodo.5566761.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2013

Tropospheric Ozone Changes, Radiative Forcing and Attribution to Emissions in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

Ozone (O3) from 17 atmospheric chemistry models taking part in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) has been used to calculate tropospheric ozone radiative forcings (RFs). All models applied a common set of anthropogenic emissions, which are better constrained for the present-day than the past. Future anthropogenic emissions follow the four Representative Concentration Pathway (RCP) scenarios, which define a relatively narrow range of possible air pollution emissions. We calculate a value for the pre-industrial (1750) to present-day (2010) tropospheric ozone RF of 410 mW m−2. The model range of pre-industrial to present-day changes in O3 produces a spread (+/-1 standard deviation) in RFs of +/-17%. Three different radiation schemes were used - we find differences in RFs between schemes (for the same ozone fields) of +/-10 percent. Applying two different tropopause definitions gives differences in RFs of +/-3 percent. Given additional (unquantified) uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of +/-30 percent for the tropospheric ozone RF. Experiments carried out by a subset of six models attribute tropospheric ozone RF to increased emissions of methane (44+/-12 percent), nitrogen oxides (31 +/- 9 percent), carbon monoxide (15 +/- 3 percent) and non-methane volatile organic compounds (9 +/- 2 percent); earlier studies attributed more of the tropospheric ozone RF to methane and less to nitrogen oxides. Normalising RFs to changes in tropospheric column ozone, we find a global mean normalised RF of 42 mW m(−2) DU(−1), a value similar to previous work. Using normalised RFs and future tropospheric column ozone projections we calculate future tropospheric ozone RFs (mW m(−2); relative to 1750) for the four future scenarios (RCP2.6, RCP4.5, RCP6.0 and RCP8.5) of 350, 420, 370 and 460 (in 2030), and 200, 300, 280 and 600 (in 2100). Models show some coherent responses of ozone to climate change: decreases in the tropical lower troposphere, associated with increases in water vapour; and increases in the sub-tropical to mid-latitude upper troposphere, associated with increases in lightning and stratosphere-to-troposphere transport. Climate change has relatively small impacts on global mean tropospheric ozone RF.

climate change↗
NASA NTRS2021

Investigations on the Anthropogenic Reversal of the Natural Ozone Gradient Between Northern and Southern Midlatitudes

Our quantitative understanding of natural tropospheric ozone concentrations is limited by the paucity of reliable measurements before the 1980s. We utilize the existing measurements to compare the long-term ozone changes that occurred within the marine boundary layer at northern and southern midlatitudes. Since 1950 ozone concentrations have increased by a factor of 2.1 ± 0.2 in the Northern Hemisphere (NH) and are presently larger than in the Southern Hemisphere (SH), where only a much smaller increase has occurred. These changes are attributed to increased ozone production driven by anthropogenic emissions of photochemical ozone precursors that increased with industrial development. The greater ozone concentrations and increases in the NH are consistent with the predominant location of anthropogenic emission sources in that hemisphere. The available measurements indicate that this interhemispheric gradient was much smaller and was likely reversed in the pre-industrial troposphere with higher concentrations in the SH. Six Earth system model (ESM) simulations indicate similar total NH increases (1.9 with a standard deviation of 0.3), but they occurred more slowly over a longer time period, and the ESMs do not find higher pre-industrial ozone in the SH. Several uncertainties in the ESMs may cause these model–measurement disagreements: the assumed natural nitrogen oxide emissions may be too large, the relatively greater fraction of ozone injected by stratosphere–troposphere exchange to the NH may be overestimated, ozone surface deposition to ocean and land surfaces may not be accurately simulated, and model treatment of emissions of biogenic hydrocarbons and their photochemistry may not be adequate.

natural tropospheric ozone concentrations↗
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.↗
DOE OSTI2023

Properties and Controlling Processes of Aerosol and Cloud Condensation Nuclei in Marine Boundary Layer Over Eastern North Atlantic (Final Report)

Remote marine low cloud systems have large spatial and temporal coverages. Because of their relatively low optical thickness and background aerosol concentrations, marine low clouds are particularly susceptible to perturbations in aerosols associated with anthropogenic emissions. Recent studies show that a large fraction of the global aerosol indirect forcing can be attributed to changes in marine low clouds, despite their relatively long distance from most anthropogenic sources. Currently, there remain large uncertainties in the magnitude of the global aerosol indirect radiative forcing. One major contribution to this large uncertainty derives from poor understanding of the aerosols under natural conditions, the perturbation by anthropogenic emissions, and the processes that drive them. In this project, we took advantage of the comprehensive, multi-dimensional characterization of meteorological parameters, trace gases, aerosol, cloud, and drizzle fields during the Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) and the long-term measurements at the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) site on Graciosa Island. By synergistically combining in situ measurements, remote sensing retrievals, and model simulations, we quantified aerosol properties in the ENA, their vertical profiles, and variations with season, synoptic state, and airmass. We investigated key aerosol processes, including entrainment of free troposphere aerosol into marine boundary layer, new particle formation, growth of Aitken mode particles, and the influences of these processes on the cloud condensation nuclei (CCN) population in marine boundary layer. The representation of key aerosol processes in the Energy Exascale Earth System Model (E3SM) was evaluated using the observations. This project has led to 26 publications, which are listed at the end of this report.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

The acidity of atmospheric particles and clouds

Acidity, defined as pH, is a central component of aqueous chemistry. In the atmosphere, the acidity of condensed phases (aerosol particles, cloud water, and fog droplets) governs the phase partitioning of semivolatile gases such as HNO 3 , NH 3 , HCl, and organic acids and bases as well as chemical reaction rates. It has implications for the atmospheric lifetime of pollutants, deposition, and human health. Despite its fundamental role in atmospheric processes, only recently has this field seen a growth in the number of studies on particle acidity. Even with this growth, many fine-particle pH estimates must be based on thermodynamic model calculations since no operational techniques exist for direct measurements. Current information indicates acidic fine particles are ubiquitous, but observationally constrained pH estimates are limited in spatial and temporal coverage. Clouds and fogs are also generally acidic, but to a lesser degree than particles, and have a range of pH that is quite sensitive to anthropogenic emissions of sulfur and nitrogen oxides, as well as ambient ammonia. Historical measurements indicate that cloud and fog droplet pH has changed in recent decades in response to controls on anthropogenic emissions, while the limited trend data for aerosol particles indicate acidity may be relatively constant due to the semivolatile nature of the key acids and bases and buffering in particles. This paper reviews and synthesizes the current state of knowledge on the acidity of atmospheric condensed phases, specifically particles and cloud droplets. It includes recommendations for estimating acidity and pH, standard nomenclature, a synthesis of current pH estimates based on observations, and new model calculations on the local and global scale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2006

The Ozone Budget in the Upper Troposphere from Global Modeling Initiative (GMI)Simulations

Ozone concentrations in the upper troposphere are influenced by in-situ production, long-range tropospheric transport, and influx of stratospheric ozone, as well as by photochemical removal. Since ozone is an important greenhouse gas in this region, it is particularly important to understand how it will respond to changes in anthropogenic emissions and changes in stratospheric ozone fluxes.. This response will be determined by the relative balance of the different production, loss and transport processes. Ozone concentrations calculated by models will differ depending on the adopted meteorological fields, their chemical scheme, anthropogenic emissions, and treatment of the stratospheric influx. We performed simulations using the chemical-transport model from the Global Modeling Initiative (GMI) with meteorological fields from (It)h e NASA Goddard Institute for Space Studies (GISS) general circulation model (GCM), (2) the atmospheric GCM from NASA's Global Modeling and Assimilation Office(GMAO), and (3) assimilated winds from GMAO . These simulations adopt the same chemical mechanism and emissions, and adopt the Synthetic Ozone (SYNOZ) approach for treating the influx of stratospheric ozone -. In addition, we also performed simulations for a coupled troposphere-stratosphere model with a subset of the same winds. Simulations were done for both 4degx5deg and 2degx2.5deg resolution. Model results are being tested through comparison with a suite of atmospheric observations. In this presentation, we diagnose the ozone budget in the upper troposphere utilizing the suite of GMI simulations, to address the sensitivity of this budget to: a) the different meteorological fields used; b) the adoption of the SYNOZ boundary condition versus inclusion of a full stratosphere; c) model horizontal resolution. Model results are compared to observations to determine biases in particular simulations; by examining these comparisons in conjunction with the derived budgets, we may pinpoint deficiencies in the representation of chemical/dynamical processes.

Rodriquez, J.↗
NASA NTRS2003

Eastern Asian Emissions of Anthropogenic Halocarbons Deduced from Aircraft Concentration Data

The Montreal Protocol restricts production of ozone-depleting halocarbons worldwide. Enforcement of the protocol has relied mainly on annual government statistics of production and consumption of these compounds (bottom-up approach). We show here that aircraft observations of ha1ocarbon:CO enhancement ratios on regional to continental scales can be used to infer halocarbon emissions, providing independent verification of the bottom-up approach. We apply this topdown approach to aircraft observations of Asian outflow &om the TRACE-P mission over the western Pacific (March-April 2001) and derive emissions from eastern Asia (China, Japan, and Korea). We derive an eastern Asian carbon tetrachloride (CCl4) source of 21.5 Gg yr(sup -1), several-fold larger than previous estimates and amounting to -30% of the global budget for this gas. Our emission estimate for CFC-11 from eastern Asia is 50% higher than inventories derived from manufacturing records. Our emission estimates for methyl chloroform (CH3CC13) and CFC-12 are in agreement with existing inventories. For halon 1211 we find only a strong local source originating from the Shanghai area. Our emission estimates for the above gases result in a approximately equal to 40% increase in the ozone depletion potential (ODP) of Asian emissions relative to previous estimates, corresponding to a approximately equal to 10% global increase in ODP.

Palmer, Paul I.↗
NASA NTRS2008

An Instrument to Enable Identification of Anthropogenic CO2 Emissions Using Concurrent CO Measurements

We have developed an instrument concept that will enable the measurement of CO from the top of the atmosphere to the Earth's surface with very high sensitivity and at the high spatial and temporal resolutions required by the NRC Decadal Survey mission Active Sensing of Carbon Dioxide (CO2) over Nights, Days and Seasons (ASCENDS). We are developing an innovative CO sensor that will enable the ASCENDS mission to differentiate between anthropogenic and natural sources and sinks of global carbon. The NRC Decadal Survey places particular emphasis on retrieving CO information for the planetary boundary layer. Measurement made using both the 2.3 micron and 4.7 micron channels are needed to achieve the sensitivity required in the lower atmosphere where the degree of CO - CO2 correlation is indicative of anthropogenic sources of CO2. Measurements made using only the 4.7 micron channel cannot provide sufficient sensitivity to CO in the very lowest layers of the atmosphere. The fundamental method we use is Gas Filter Correlation Radiometry (GFCR), a highly successful technique used in other airborne and space-based missions for detecting trace species in the Earth's atmosphere. Our version of GFCR overcomes many of the limitations encountered by prior and existing instruments, allowing us to measure weak signals from small targets very quickly and with extremely high specificity by employing a new dual beam radiometer concept using a focal plane array. Our design will provide a means to make the desired CO measurements for the ASCENDS mission. A simple change in gas filter cell contents would allow the same hardware to measure CH4 with high precision under the nominal ASCENDS mission spatial and temporal constraints. All critical components in the sensor design are mature, many subsystems tested, and the system has been extensively modeled, bringing it to a present Technology Readiness Level (TRL) of 3 (though some individual components are at TRLs 6-9). We are presently developing critical components for the new spectrometer and advancing our understanding of the measurement requirements for both CO and CH4. This new GFCR technique/sensor will enable measurements of trace gases with high sensitivity while maintaining the inherent robustness and simplicity of the more traditional radiometer hardware. Initial estimates of cost/risk of a spacebased 2-channel GFCR indicate that our design is extremely cost effective and will fit within existing ASCENDS mission budget constraints as determined by the NRC Decadal Survey and a NASA-sponsored mission study.

Cook, William B.↗
NASA NTRS2012

Variability and Trends of Aerosol Properties over Kanpur, Northern India using AERONET Data (2001-10)

Natural and anthropogenic aerosols over northern India play an important role in influencing the regional radiation budget, causing climate implications to the overall hydrological cycle of South Asia. In the context of regional climate change and air quality, we discuss aerosol loading variability and trends at Kanpur AERONET station located in the central part of the Indo-Gangetic plains (IGP), during the last decade (2001-10). Ground-based radiometric measurements show an overall increase in column-integrated aerosol optical depth (AOD) on a yearly basis. This upward trend is mainly due to a sustained increase in the seasonal/monthly averaged AOD during the winter (Dec-Feb) and post-monsoon (Oct-Nov) seasons (dominated by anthropogenic emissions). In contrast, a neutral to weak declining trend is observed during late pre-monsoon (Mar-May) and monsoon (Jun-Sep) months, mainly influenced by inter-annual variations of dust outbreaks. A general decrease in coarse-mode aerosols associated with variable dust activity is observed, whereas the statistically significant increasing post-monsoon/winter AOD is reflected in a shift of the columnar size distribution towards relatively larger particles in the accumulation mode. Overall, the present study provides an insight into the pronounced seasonal behavior in aerosol loading trends and, in general, is in agreement with that associating the findings with those recently reported by satellite observations (MODIS and MISR) over northern India. Our results further suggest that anthropogenic emissions (due mainly to fossil-fuel and biomass combustion) over the IGP have continued to increase in the last decade.

AERONET↗