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DOE OSTI2025

The HTAP_v3.2 emission mosaic: merging regional and global monthly emissions (2000–2020) to support air quality modelling and policies

This study, performed under the umbrella of the Task Force on Hemispheric Transport of Air Pollution (TF-HTAP), responds to the need of the global and regional atmospheric modelling community of having a mosaic emission inventory of air pollutants that conforms to specific requirements: global coverage, long time series, spatially distributed emissions with high time resolution, and a high sectoral resolution. The mosaic approach of integrating official regional emission inventories based on locally reported data, with a global inventory based on a globally consistent methodology, allows modellers to perform simulations of a high scientific quality while also ensuring that the results remain relevant to policymakers. HTAP_v3.2, an ad-hoc global mosaic of anthropogenic inventories, is an update to the HTAP_v3 global mosaic inventory and has been developed by integrating official inventories over specific areas (North America, Europe, Asia including China, Japan and Korea) with the independent Emissions Database for Global Atmospheric Research (EDGAR) inventory for the remaining world regions. The results are spatially and temporally distributed emissions of SO 2 , NO x , CO, NMVOC, NH 3 , PM 10 , PM 2.5 , Black Carbon (BC), and Organic Carbon (OC), with a spatial resolution of 0.1 × 0.1° and time intervals of months and years covering the period 2000–2020 (https://doi.org/10.5281/zenodo.17086684, Crippa, 2025, https://edgar.jrc.ec.europa.eu/dataset_htap_v32, last access: 27 October 2025). The emissions are further disaggregated to 16 anthropogenic emitting sectors. This paper describes the methodology applied to develop such an emission mosaic, reports on source allocation, differences among existing inventories, and best practices for the mosaic compilation. One of the key strengths of the HTAP_v3.2 emission mosaic is its temporal coverage, enabling the analysis of emission trends over the past two decades. The development of a global emission mosaic over such long time series represents a unique product for global air quality modelling and for better-informed policy making, reflecting the community effort expended by the TF-HTAP to disentangle the complexity of transboundary transport of air pollution.

Guizzardi, Diego [European Commission, Ispra (Ital↗

NASA NTRS2013

A Multimodel Assessment of the Influence of Regional Anthropogenic Emission Reductions on Aerosol Direct Radiative Forcing and the Role of Intercontinental Transport

In this study, we assess changes of aerosol optical depth (AOD) and direct radiative forcing (DRF) in response to the reduction of anthropogenic emissions in four major pollution regions in the Northern Hemisphere by using results from nine global models in the framework of the Hemispheric Transport of Air Pollution (HTAP). DRF at top of atmosphere (TOA) and surface is estimated based on AOD results from the HTAP models and AOD-normalized DRF (NDRF) from a chemical transport model. The multimodel results show that, on average, a 20% reduction of anthropogenic emissions in North America, Europe, East Asia, and South Asia lowers the global mean AOD (all-sky TOA DRF) by 9.2% (9.0%), 3.5% (3.0%), and 9.4% (10.0%) for sulfate, particulate organic matter (POM), and black carbon (BC), respectively. Global annual average TOA all-sky forcing efficiency relative to particle or gaseous precursor emissions from the four regions (expressed as multimodel mean +/- one standard deviation) is -3.5 +/-0.8, -4.0 +/- 1.7, and 29.5+/-18.1mW / sq m per Tg for sulfate (relative to SO2), POM, and BC, respectively. The impacts of the regional emission reductions on AOD and DRF extend well beyond the source regions because of intercontinental transport (ICT). On an annual basis, ICT accounts for 11 +/- 5% to 31 +/- 9% of AOD and DRF in a receptor region at continental or subcontinental scale, with domestic emissions accounting for the remainder, depending on regions and species. For sulfate AOD, the largest ICT contribution of 31 +/- 9% occurs in South Asia, which is dominated by the emissions from Europe. For BC AOD, the largest ICT contribution of 28 +/- 18% occurs in North America, which is dominated by the emissions from East Asia. The large spreads among models highlight the need to improve aerosol processes in models, and evaluate and constrain models with observations.

Europe↗

NASA NTRS2016

Global and Regional Radiative Forcing from 20 Reductions in BC, OC and SO4 an HTAP2 Multi-Model Study

In the Hemispheric Transport of Air Pollution Phase 2 (HTAP2) exercise, a range of global atmospheric general circulation and chemical transport models performed coordinated perturbation experiments with 20% reductions in emissions of anthropogenic aerosols, or aerosol precursors, in a number of source regions. Here, we compare the resulting changes in the atmospheric load and vertically resolved profiles of black carbon (BC), organic aerosols (OA) and sulfate (SO4/ from 10 models that include treatment of aerosols. We use a set of temporally, horizontally and vertically resolved profiles of aerosol forcing efficiency (AFE) to estimate the impact of emission changes in six major source regions on global radiative forcing (RF) pertaining to the direct aerosol effect, finding values between. 51.9 and 210.8mW/sq m/Tg for BC, between -2.4 and -17.9mW/sq m/Tg for OA and between -3.6 and -10.3W/sq m/Tg for SO4. In most cases, the local influence dominates, but results show that mitigations in south and east Asia have substantial impacts on the radiative budget in all investigated receptor regions, especially for BC. In Russia and the Middle East, more than 80 % of the forcing for BC and OA is due to extra-regional emission reductions. Similarly, for North America, BC emissions control in east Asia is found to be more important than domestic mitigations, which is consistent with previous findings. Comparing fully resolved RF calculations to RF estimates based on vertically averaged AFE profiles allows us to quantify the importance of vertical resolution to RF estimates. We find that locally in the source regions, a 20% emission reduction strengthens the radiative forcing associated with SO4 by 25% when including the vertical dimension, as the AFE for SO4 is strongest near the surface. Conversely, the local RF from BC weakens by 37% since BC AFE is low close to the ground. The fraction of BC direct effect forcing attributable to intercontinental transport, on the other hand, is enhanced by one-third when accounting for the vertical aspect, because long-range transport primarily leads to aerosol changes at high altitudes, where the BC AFE is strong. While the surface temperature response may vary with the altitude of aerosol change, the analysis in the present study is not extended to estimates of temperature or precipitation changes.

profiles of aerosol forcing efficiency (AFE)↗

NASA NTRS2012

A HTAP Multi-Model Assessment of the Influence of Regional Anthropogenic Emission Reductions on Aerosol Direct Radiative Forcing and the Role of Intercontinental Transport

Yu, Hongbin↗

NASA NTRS2020

Local to Global Air Quality Simulations using the NASA GEOS Composition Forecast Model, GEOS-CF

We give an overview of the NASA Global Earth Observing System Composition Forecast model (GEOS-CF), a high-resolution (roughly 25-km) global composition model developed by the NASA Global Modeling and Assimilation Office (GMAO). This system combines the GEOS weather and aerosol model with the GEOS-Chem chemistry module to provide a holistic view of atmospheric composition that captures a wide range of air pollutants such as ozone,nitrogen oxides, volatile organic compounds, and fine particulate matter.Given the global extent of the model, GEOS-CF captures large-scale processes such as long-range transport of air pollutants, across ocean basins and continents.

Knowland, Emma K.↗

NASA NTRS2000

Observing Tropospheric Ozone From Space

The importance of tropospheric ozone embraces a spectrum of relevant scientific issues ranging from local environmental concerns, such as damage to the biosphere and human health, to those that impact global change questions, Such is climate warming. From an observational perspective, the challenge is to determine the tropospheric ozone global distribution. Because its lifetime is short compared with other important greenhouse gases that have been monitored over the past several decades, the distribution of tropospheric ozone cannot be inferred from a relatively small set of monitoring stations. Therefore, the best way to obtain a true global picture is from the use of space-based instrumentation where important spatial gradients over vast ocean expanses and other uninhabited areas can be properly characterized. In this paper, the development of the capability to measure tropospheric ozone from space over the past 15 years is summarized. Research in the late 1980s successfully led to the determination of the climatology of tropospheric ozone as a function of season; more recently, the methodology has improved to the extent where regional air pollution episodes can be characterized. The most recent modifications now provide quasi-global (50 N) to 50 S) maps on a daily basis. Such a data set would allow for the study of long-range (intercontinental) transport of air pollution and the quantification of how regional emissions feed into the global tropospheric ozone budget. Future measurement capabilities within this decade promise to offer the ability to provide Concurrent maps of the precursors to the in situ formation of tropospheric ozone from which the scientific community will gain unprecedented insight into the processes that control global tropospheric chemistry

Fishman, Jack↗

NASA NTRS1987

Chemistry of the global troposphere - Fluorocarbons as tracers of air motion

Winds and convective mixing from a general circulation model of the atmosphere have been applied in a chemical tracer model (CTM) to simulate the global distribution and temporal variability of chlorofluorocarbons (CFCs). The seasonal cycle in moist convection, with maximum activity over continents in summer, leads to an annual cycle in the surface concentration of CFCs. Emissions are retained in the lowest levels of the atmosphere during winter, and surface concentrations peak near sources. In this season, CFCs from European sources are carried by low-level winds into the Arctic. During summer, vertical exchange is more efficient, and pollutants are transported more rapidly to the middle atmosphere. Consequently, concentrations of CFCs during summer are relatively low near the surface and elevated in the middle troposphere. Time series analysis of data from Adrigole, Ireland, indicates that the model accurately simulates long-range transport of air pollution. The model reproduces global distributions and trends for CFC-11 and CFC-12 observed by the ALE experiment; however, subgrid diffusion must be introduced into the model in order to reproduce the observed interhemispheric gradient. Interhemispheric exchange occurs mainly in the upper tropical troposphere, producing a profile which increases with altitude in the Southern Hemisphere, in agreement with observations. The distribution of CFCs is such that it is necessary to apply important corrections to observations at surface stations in order to derive global distributions.

Prather, Michael↗

NASA NTRS2020

High Resolution Global Coupled Chemistry-Meteorology Simulations Using the NASA GEOS Composition Forecast System, GEOS-CF

We will give an overview of the NASA Global Earth Observing System Composition Forecast system (GEOS-CF), a high-resolution (0.25 degree) global composition model developed by the NASA Global Modeling and Assimilation Office (GMAO). This system combines the GEOS weather and aerosol model with the GEOS-Chem chemistry module (version 12) to provide a holistic view of atmospheric composition that captures a wide range of air pollutants such as ozone, nitrogen oxides, volatile organic compounds, and fine particulate matter. The spatial resolution of 0.25 degrees (approx. 25 km) is fine enough to resolve local features such as nighttime ozone titration previously resolved only by urban or regional models. Furthermore, since there are no boundary conditions for a global model, the GEOS-CF captures large-scale processes such as long-range transport of air pollutants from forest fires. Comparisons against surface observations highlight the model’s overall capability to reproduce the diurnal variability of air pollutants under a variety of meteorological conditions. In addition, we show how machine learning techniques can be used to correct for sub-grid variability, which further improves model estimates at a given surface observation site. The GEOS-CF system offers a new tool for scientists and the public health community alike and is being developed jointly with several government and non-profit partners. As an example, we will show the use of GEOS-CF during the Satellite Coastal and Oceanic Atmospheric Pollution Experiment (SCOAPE). The campaign, conducted in collaboration between NASA and the Bureau of Ocean Energy Management (BOEM), aims to investigate the response of onshore air quality to Outer Continental Shelf (OCS) oil and gas exploration, development and production. Detailed gas-phase chemistry, as provided by GEOS-CF, is critical to understand the formation of air pollution related to hydrocarbon emissions from offshore oil and gas activities. The accuracy of GEOS-CF can be further improved by incorporating detailed offshore emissions compiled by BOEM.

Knowland, K. Emma↗

NASA NTRS2011

NASA A-Train and Terra Observations of the 2010 Russian Wildfires

Wildfires raged throughout western Russia and parts of Eastern Europe during a persistent heat wave in the summer of 2010. Anomalously high surface temperatures (35 - 41 C) and low relative humidity (9 - 25 %) from mid- June to mid-August 2010 shown by analysis of radiosonde data from multiple sites in western Russia were ideal conditions for the wildfires to thrive. Measurements of outgoing longwave radiation (OLR) from the Atmospheric Infrared Sounder (AIRS) over western Russian indicate persistent subsidence during the heat wave. Daily three-day back-trajectories initiated over Moscow reveal a persistent anticyclonic circulation for 18 days in August, coincident with the most intense period of fire activity observed by Moderate Resolution Imaging Spectroradiometer (MODIS). This unfortunate meteorological coincidence allowed transport of polluted air from the region of intense fires to Moscow and the surrounding area. We demonstrate that the 2010 Russian wildfires are unique in the record of observations obtained by remote-sensing instruments on-board NASA satellites: Aura and Aqua (part of the A-Train Constellation) and Terra. Analysis of the distribution of MODIS fire products and aerosol optical thickness (AOT), UV aerosol index (AI) and single-scattering albedo (SSA) from Aura's Ozone Monitoring Instrument (OMI), and total column carbon monoxide (CO) from Aqua s Atmospheric Infrared Sounder (AIRS) show that the region in the center of western Russia surrounding Moscow (52-58 deg N, 33 -43 deg E) is most severely impacted by wildfire emissions. Over this area, AIRS CO, OMI AI, and MODIS AOT are significantly enhanced relative to the historical satellite record during the first 18 days in August when the anti-cyclonic circulation persisted. By mid-August, the anti-cyclonic circulation was replaced with westerly transport over Moscow and vicinity. The heat wave

Witte, J. C.↗

NASA NTRS2014

Impacts of Intercontinental Transport of Anthropogenic Fine Particulate Matter on Human Mortality

Fine particulate matter with diameter of 2.5 microns or less (PM2.5) is associated with premature mortality and can travel long distances, impacting air quality and health on intercontinental scales. We estimate the mortality impacts of 20 % anthropogenic primary PM2.5 and PM2.5 precursor emission reductions in each of four major industrial regions (North America, Europe, East Asia, and South Asia) using an ensemble of global chemical transport model simulations coordinated by the Task Force on Hemispheric Transport of Air Pollution and epidemiologically-derived concentration-response functions. We estimate that while 93-97 % of avoided deaths from reducing emissions in all four regions occur within the source region, 3-7 % (11,500; 95 % confidence interval, 8,800-14,200) occur outside the source region from concentrations transported between continents. Approximately 17 and 13 % of global deaths avoided by reducing North America and Europe emissions occur extraregionally, owing to large downwind populations, compared with 4 and 2 % for South and East Asia. The coarse resolution global models used here may underestimate intraregional health benefits occurring on local scales, affecting these relative contributions of extraregional versus intraregional health benefits. Compared with a previous study of 20 % ozone precursor emission reductions, we find that despite greater transport efficiency for ozone, absolute mortality impacts of intercontinental PM2.5 transport are comparable or greater for neighboring source-receptor pairs, due to the stronger effect of PM2.5 on mortality. However, uncertainties in modeling and concentration-response relationships are large for both estimates.

human health↗

NASA NTRS2008

3D Air Quality and the Clean Air Interstate Rule: Lagrangian Sampling of CMAQ Model Results to Aid Regional Accountability Metrics

The Clean Air Interstate Rule (CAIR) is expected to reduce transport of air pollutants (e.g. fine sulfate particles) in nonattainment areas in the Eastern United States. CAIR highlights the need for an integrated air quality observational and modeling system to understand sulfate as it moves in multiple dimensions, both spatially and temporally. Here, we demonstrate how results from an air quality model can be combined with a 3d monitoring network to provide decision makers with a tool to help quantify the impact of CAIR reductions in SO2 emissions on regional transport contributions to sulfate concentrations at surface monitors in the Baltimore, MD area, and help improve decision making for strategic implementation plans (SIPs). We sample results from the Community Multiscale Air Quality (CMAQ) model using ensemble back trajectories computed with the NASA Langley Research Center trajectory model to provide Lagrangian time series and vertical profile information, that can be compared with NASA satellite (MODIS), EPA surface, and lidar measurements. Results are used to assess the regional transport contribution to surface SO4 measurements in the Baltimore MSA, and to characterize the dominant source regions for low, medium, and high SO4 episodes.

Fairlie, T. D.↗

DOE OSTI2023

Global nitrogen and sulfur deposition mapping using a measurement–model fusion approach

Abstract. Global reactive nitrogen (N) deposition has more than tripled since 1860 and is expected to remain high due to food production and fossil fuel consumption. Global sulfur emissions have been decreasing worldwide over the last 30 years, but many regions are still experiencing unhealthily high levels of deposition. We update the 2010 global deposition budget for reactive nitrogen and sulfur components with new regional wet deposition measurements from Asia, improving the ensemble results of 11 global chemistry transport models from the second phase of the United Nations Economic Commission for Europe's Task Force on Hemispheric Transport of Air Pollution (HTAP II). The observationally adjusted global N deposition budget is 114.5 Tg N, representing a minor increase of 1 % from the model-only derived values, and the adjusted global sulfur deposition budget is 88.9 Tg S, representing a 6.5 % increase from the modeled values, using an interpolation distance of 2.5∘. Regionally, deposition adjustments can be up to ∼ 73 % for nitrogen and 112 % for sulfur. Our study demonstrates that a global measurement–model fusion approach can improve N and S deposition model estimates at a regional scale, with sufficient availability of observations; however, in large parts of the world, alternative approaches need to be explored. The analysis presented here represents a step forward toward the World Meteorological Organization's goal of global fusion products for accurately mapping harmful air pollution deposition.

Rubin, Hannah J. (ORCID:0000000182226924)↗

DOE OSTI2022

Extensive urban air pollution footprint evidenced by submicron organic aerosols molecular composition

Transport and transformation of urban air pollutants are among the major factors driving the changes in the atmospheric composition in the downwind rural/remote areas of a megacity. Here, we assess the impacts of urban air pollution in a subtropical forest through characterization of the organic markers in submicron aerosol particles. The aerosol samples were collected and analyzed using TD-PTR-ToF-MS, where 163 ions were detected. The concentration of these extracted ions accounts for 83% of the mass of submicron organic aerosols, which are accordingly characterized by a median formula of C 7 H 10 O 2 . Molecular speciation indicates that urban and biomass burning pollution contributed substantially to the budget of organic aerosols, which were enhanced particularly by the liquid water content and acidity of the aerosols. Our results evidence that the footprint of urban air pollution was extended to its downwind forested areas and caused changes in the concentration and composition of submicron aerosols.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2003

The East and Southeast Asia Initiatives: Aerosol Column Measurements

Airborne dusts from northern China contribute a significant part of the air quality problem and, to some extent, regional climatic impact in Asia during spring- time. However, with the economical growth in China, increases in the emission of air pollutants generated from industrial and vehicular sources will not only impact the radiation balance, but adverse health effects to humans all year round. In addition, both of these dust and air pollution clouds can transport swiftly across the Pacific reaching North America within a few days, possessing an even larger scale effect. The Asian dust and air pollution aerosols can be detected by its colored appearance on current Earth observing satellites (e.g., MODIS, SeaWiFS, TOMS, etc.) and its evolution monitored by satellites and surface network. Biomass burning has been a regular practice for land clearing and land conversion in many countries, especially those in Africa, South America, and Southeast Asia. However, the unique climatology of Southeast Asia is very different than that of Africa and South America, such that large-scale biomass burning causes smoke to interact extensively with clouds during the peak-burning season of March to April. Significant global sources of greenhouse gases (e.g., CO2, CH4), chemically active gases (e.g., NO, CO, HC, CH3,Br), and atmospheric aerosols are produced by biomass burning processes. These gases influence the Earth- atmosphere system, impacting both global climate and tropospheric chemistry. Some aerosols can serve as cloud condensation nuclei, which play an important role in determining cloud lifetime and precipitation, hence, altering the earth's radiation and water budget. Biomass burning also affects the biogeochemical cycling of nitrogen and carbon compounds from the soil to the atmosphere; the hydrological cycle (i.e., run off and evaporation); land surface reflectivity and emissivity; as well as ecosystem biodiversity and stability. Two new initiatives, EAST-AIRE (East Asian Study of Tropospheric Aerosols: an International Regional Experiment) and BASE-ASIA (Biomass-burning Aerosols in South East-Asia: Smoke Impact Assessment) will be presented and discussed their contribution to better understand the impacts of aerosols on regional-to- global climate, hydrological and carbon cycles, and tropospheric chemistry.

Tsay, Si-Chee↗

NASA NTRS2004

Dust, Pollution, and Biomass Burning Aerosols in Asian Pacific: A Column Satellite-Surface Perspective

Airborne dusts from northern China contribute a significant part of the air quality problem and, to some extent, regional climatic impact in Asia during spring-time. However, with the economical growth in China, increases in the emission of air pollutants generated from industrial and vehicular sources will not only impact the radiation balance, but adverse health effects to humans all year round. In addition, both of these dust and air pollution clouds can transport swiftly across the Pacific reaching North America within a few days, possessing an even larger scale effect. The Asian dust and air pollution aerosols can be detected by its colored appearance on current Earth observing satellites (e.g., MODIS, SeaWiFS, TOMS, etc.) and its evolution monitored by satellites and surface network. Biomass burning has been a regular practice for land clearing and land conversion in many countries, especially those in Africa, South America, and Southeast Asia. However, the unique climatology of Southeast Asia is very different than that of Africa and South America, such that large-scale biomass burning causes smoke to interact extensively with clouds during the peak-burning season of March to April. Significant global sources of greenhouse gases (e.g., CO2, CH4), chemically active gases (e.g., NO, CO, HC, CH3Br), and atmospheric aerosols are produced by biomass burning processes. These gases influence the Earth-atmosphere system, impacting both global climate and tropospheric chemistry. Some aerosols can serve as cloud condensation nuclei, which play an important role in determining cloud lifetime and precipitation, hence, altering the earth's radiation and water budget. Biomass burning also affects the biogeochemical cycling of nitrogen and carbon compounds from the soil to the atmosphere; the hydrological cycle (i.e., run off and evaporation); land surface reflectivity and emissivity; as well as ecosystem biodiversity and stability. Two new initiatives, EAST-AIRE (East Asian Study of Tropospheric Aerosols: an International Regional Experiment) and BASE-ASIA (Biomass-burning Aerosols in South East-Asia: Smoke Impact Assessment) will be presented and discussed their contribution to better understand the impacts of aerosols on regional-to-global climate, hydrological and carbon cycles, and tropospheric chemistry.

Tsay, Si-Chee↗

NASA NTRS1974

Airborne survey of major air basins in California

An instrumented aircraft was used to study the chemical and transport properties of air pollution in two major urban centers in California and to survey certain aspects of air pollution within this state. State-of-the-art measurement techniques and sampling procedures are discussed. It is found that meteorological transport mechanisms are better portrayed by vertical pollutant profiles. Airborne measurements define the nature of the mixing layer for atmospheric pollutants. Results show that the pollutants are found to be concentrated in distinct layers up to at least 18,000 feet and the O3 buildup occurring in advected air masses is a result of a continuous photochemical aging of air mass.

Gloria, H. R.↗

DOE OSTI2020

Modeling Air Pollutant Emissions in the Provincial Level Road Transportation Sector in Korea: A Case Study of the Zero-Emission Vehicle Subsidy

South Korea has been suffering from high PM2.5 pollution. Previous studies have contributed to establishing PM2.5 mitigation policies but have not considered provincial features and sector-interactions. In that sense, the integrated assessment model (IAM) could complement the shortcomings of previous studies. IAM, capable of analyzing PM2.5 pollution levels at the provincial level in Korea, however, has not been developed yet. Hence, this study (i) expands on IAM which can represent provincial-level spatial resolution in Korea (GCAM-Korea) with air pollutant emissions modeling which focuses on the road transportation sector and (ii) examines the zero-emission vehicles (ZEVs) subsidy policy’s effects on PM2.5 mitigation using the expanded GCAM-Korea. Simulation results show that PM2.5 emissions decrease by 0.6–4.1% compared to the baseline, and the Seoul metropolitan area contributes 38–44% to the overall PM2.5 emission reductions. As the ZEVs subsidy is weighted towards the light-duty vehicle 4-wheels (LDV4W) sector, various spillover effects are found: ZEVs’ share rises intensively in the LDV4W sector leading to an increase in its service costs, and at the same time, driving bus service costs to become relatively cheaper. This, in turn, drives an increase in bus service demand and emissions discharge. Furthermore, this type of impact of the ZEVs subsidy policy does not reduce internal combustion engine vehicles (ICEVs) in freight trucks, although diesel freight trucks are a major contributor to PM2.5 emissions and also to NOx.

Roh, Minyoung↗

NASA NTRS1986

Aerosols in polluted versus nonpolluted air masses Long-range transport and effects on clouds

To assess the influence of anthropogenic aerosols on the physics and chemistry of clouds in the northeastern United States, aerosol and cloud-drop size distributions, elemental composition of aerosols as a function of size, and ionic content of cloud water were measured on Whiteface Mountain, NY, during the summers of 1981 and 1982. In several case studies, the data were cross-correlated with different air mass types - background continental, polluted continental, and maritime - that were advected to the sampling site. The results are the following: (1) Anthropogenic sources hundreds of kilometers upwind cause the small-particle (accumulation) mode number to increase from hundreds of thousands per cubic centimeter and the mass loading to increase from a few to several tens of micrograms per cubic meter, mostly in the form of sulfur aerosols. (2) A significant fraction of anthropogenic sulfur appears to act as cloud condensation nuclei (CCN) to affect the cloud drop concentration. (3) Clouds in Atlantic maritime air masses have cloud drop spectra that are markedly different from those measured in continental clouds. The drop concentration is significantly lower, and the drop size spectra are heavily skewed toward large drops. (4) Effects of anthropogenic pollutants on cloud water ionic composition are an increase of nitrate by a factor of 50, an increase of sulfate by more than one order of magnitude, and an increase of ammonium ion by a factor of 7. The net effect of the changes in ionic concentrations is an increase in cloud water acidity. An anion deficit even in maritime clouds suggests an unknown, possibly biogenic, source that could be responsible for a pH below neutral, which is frequently observed in nonpolluted clouds.

Pueschel, R. F.↗