Long-term mortality burden trends attributed to black carbon and PM2·5 from wildfire emissions across the continental USA from 2000 to 2020: a deep learning modelling study.

BACKGROUND: Long-term improvements in air quality and public health in the continental USA were disrupted over the past decade by increased fire emissions that potentially offset the decrease in anthropogenic emissions. This study aims to estimate trends in black carbon and PM2·5 concentrations and their attributable mortality burden across the USA. METHODS: In this study, we derived daily concentrations of PM2·5 and its highly toxic black carbon component at a 1-km resolution in the USA from 2000 to 2020 via deep learning that integrated big data from satellites, models, and surface observations. We estimated the annual PM2·5-attributable and black carbon-attributable mortality burden at each 1-km2 grid using concentration-response functions collected from a national cohort study and a meta-analysis study, respectively. We investigated the spatiotemporal linear-regressed trends in PM2·5 and black carbon pollution and their associated premature deaths from 2000 to 2020, and the impact of wildfires on air quality and public health. FINDINGS: Our results showed that PM2·5 and black carbon estimates are reliable, with sample-based cross-validated coefficients of determination of 0·82 and 0·80, respectively, for daily estimates (0·97 and 0·95 for monthly estimates). Both PM2·5 and black carbon in the USA showed significantly decreasing trends overall during 2000 to 2020 (22% decrease for PM2·5 and 11% decrease for black carbon), leading to a reduction of around 4200 premature deaths per year (95% CI 2960-5050). However, since 2010, the decreasing trends of fine particles and premature deaths have reversed to increase in the western USA (55% increase in PM2·5, 86% increase in black carbon, and increase of 670 premature deaths [460-810]), while remaining mostly unchanged in the eastern USA. The western USA showed large interannual fluctuations that were attributable to the increasing incidence of wildfires. Furthermore, the black carbon-to-PM2·5 mass ratio increased annually by 2·4% across the USA, mainly due to increasing wildfire emissions in the western USA and more rapid reductions of other components in the eastern USA, suggesting a potential increase in the relative toxicity of PM2·5. 100% of populated areas in the USA have experienced at least one day of PM2·5 pollution exceeding the daily air quality guideline level of 15 µg/m3 during 2000-2020, with 99% experiencing at least 7 days and 85% experiencing at least 30 days. The recent widespread wildfires have greatly increased the daily exposure risks in the western USA, and have also impacted the midwestern USA due to the long-range transport of smoke. INTERPRETATION: Wildfires have become increasingly intensive and frequent in the western USA, resulting in a significant increase in smoke-related emissions in populated areas. This increase is likely to have contributed to a decline in air quality and an increase in attributable mortality. Reducing fire risk via effective policies besides mitigation of climate warming, such as wildfire prevention and management, forest restoration, and new revenue generation, could substantially improve air quality and public health in the coming decades. FUNDING: National Aeronautics and Space Administration (NASA) Applied Science programme, NASA MODIS maintenance programme, NASA MAIA satellite mission programme, NASA GMAO core fund, National Oceanic and Atmospheric Administration (NOAA) GEO-XO project, NOAA Atmospheric Chemistry, Carbon Cycle, and Climate (AC4) programme, and NOAA Educational Partnership Program with Minority Serving Institutions.

Evaluating the Performance of Low-Cost PM2.5 Sensors in Mobile Settings.

Low-cost sensors (LCSs) for measuring air pollution are increasingly being deployed in mobile applications, but questions concerning the quality of the measurements remain unanswered. For example, what is the best way to correct LCS data in a mobile setting? Which factors most significantly contribute to differences between mobile LCS data and those of higher-quality instruments? Can data from LCSs be used to identify hotspots and generate generalizable pollutant concentration maps? To help address these questions, we deployed low-cost PM2.5 sensors (Alphasense OPC-N3) and a research-grade instrument (TSI DustTrak) in a mobile laboratory in Boston, MA, USA. We first collocated these instruments with stationary PM2.5 reference monitors (Teledyne T640) at nearby regulatory sites. Next, using the reference measurements, we developed different models to correct the OPC-N3 and DustTrak measurements and then transferred the corrections to the mobile setting. We observed that more complex correction models appeared to perform better than simpler models in the stationary setting; however, when transferred to the mobile setting, corrected OPC-N3 measurements agreed less well with the corrected DustTrak data. In general, corrections developed by using minute-level collocation measurements transferred better to the mobile setting than corrections developed using hourly-averaged data. Mobile laboratory speed, OPC-N3 orientation relative to the direction of travel, date, hour-of-the-day, and road class together explain a small but significant amount of variation between corrected OPC-N3 and DustTrak measurements during the mobile deployment. Persistent hotspots identified by the OPC-N3s agreed with those identified by the DustTrak. Similarly, maps of PM2.5 distribution produced from the mobile corrected OPC-N3 and DustTrak measurements agreed well. These results suggest that identifying hotspots and developing generalizable maps of PM2.5 are appropriate use-cases for mobile LCS data.

An analysis of degradation in low-cost particulate matter sensors.

Low-cost sensors (LCS) are increasingly being used to measure fine particulate matter (PM2.5) concentrations in cities around the world. One of the most commonly deployed LCS is the PurpleAir with ~ 15,000 sensors deployed in the United States, alone. PurpleAir measurements are widely used by the public to evaluate PM2.5 levels in their neighborhoods. PurpleAir measurements are also increasingly being integrated into models by researchers to develop large-scale estimates of PM2.5. However, the change in sensor performance over time has not been well studied. It is important to understand the lifespan of these sensors to determine when they should be serviced or replaced, and when measurements from these devices should or should not be used for various applications. This paper fills this gap by leveraging the fact that: (1) Each PurpleAir sensor is comprised of two identical sensors and the divergence between their measurements can be observed, and (2) There are numerous PurpleAir sensors within 50 meters of regulatory monitors allowing for the comparison of measurements between these instruments. We propose empirically derived degradation outcomes for the PurpleAir sensors and evaluate how these outcomes change over time. On average, we find that the number of 'flagged' measurements, where the two sensors within each PurpleAir sensor disagree, increases with time to ~ 4% after 4 years of operation. Approximately 2 percent of all PurpleAir sensors were permanently degraded. The largest fraction of permanently degraded PurpleAir sensors appeared to be in the hot and humid climate zone, suggesting that sensors in these locations may need to be replaced more frequently. We also find that the bias of PurpleAir sensors, or the difference between corrected PM2.5 levels and the corresponding reference measurements, changed over time by -0.12 µg/m3(95% CI: -0.13 µg/m3, -0.10 µg/m3) per year. The average bias increases dramatically after 3.5 years. Further, climate zone is a significant modifier of the association between degradation outcomes and time.

Opportunistic experiments to constrain aerosol effective radiative forcing.

Aerosol-cloud interactions (ACIs) are considered to be the most uncertain driver of present-day radiative forcing due to human activities. The nonlinearity of cloud-state changes to aerosol perturbations make it challenging to attribute causality in observed relationships of aerosol radiative forcing. Using correlations to infer causality can be challenging when meteorological variability also drives both aerosol and cloud changes independently. Natural and anthropogenic aerosol perturbations from well-defined sources provide "opportunistic experiments" (also known as natural experiments) to investigate ACI in cases where causality may be more confidently inferred. These perturbations cover a wide range of locations and spatiotemporal scales, including point sources such as volcanic eruptions or industrial sources, plumes from biomass burning or forest fires, and tracks from individual ships or shipping corridors. We review the different experimental conditions and conduct a synthesis of the available satellite datasets and field campaigns to place these opportunistic experiments on a common footing, facilitating new insights and a clearer understanding of key uncertainties in aerosol radiative forcing. Cloud albedo perturbations are strongly sensitive to background meteorological conditions. Strong liquid water path increases due to aerosol perturbations are largely ruled out by averaging across experiments. Opportunistic experiments have significantly improved process-level understanding of ACI, but it remains unclear how reliably the relationships found can be scaled to the global level, thus demonstrating a need for deeper investigation in order to improve assessments of aerosol radiative forcing and climate change.

Monthly Global Estimates of Fine Particulate Matter and Their Uncertainty.

Annual global satellite-based estimates of fine particulate matter (PM2.5) are widely relied upon for air-quality assessment. Here, we develop and apply a methodology for monthly estimates and uncertainties during the period 1998-2019, which combines satellite retrievals of aerosol optical depth, chemical transport modeling, and ground-based measurements to allow for the characterization of seasonal and episodic exposure, as well as aid air-quality management. Many densely populated regions have their highest PM2.5 concentrations in winter, exceeding summertime concentrations by factors of 1.5-3.0 over Eastern Europe, Western Europe, South Asia, and East Asia. In South Asia, in January, regional population-weighted monthly mean PM2.5 concentrations exceed 90 µg/m3, with local concentrations of approximately 200 µg/m3 for parts of the Indo-Gangetic Plain. In East Asia, monthly mean PM2.5 concentrations have decreased over the period 2010-2019 by 1.6-2.6 µg/m3/year, with decreases beginning 2-3 years earlier in summer than in winter. We find evidence that global-monitored locations tend to be in cleaner regions than global mean PM2.5 exposure, with large measurement gaps in the Global South. Uncertainty estimates exhibit regional consistency with observed differences between ground-based and satellite-derived PM2.5. The evaluation of uncertainty for agglomerated values indicates that hybrid PM2.5 estimates provide precise regional-scale representation, with residual uncertainty inversely proportional to the sample size.

Effects of COVID-19 lockdowns on fine particulate matter concentrations.

Lockdowns during the COVID-19 pandemic provide an unprecedented opportunity to examine the effects of human activity on air quality. The effects on fine particulate matter (PM2.5) are of particular interest, as PM2.5 is the leading environmental risk factor for mortality globally. We map global PM2.5 concentrations for January to April 2020 with a focus on China, Europe, and North America using a combination of satellite data, simulation, and ground-based observations. We examine PM2.5 concentrations during lockdown periods in 2020 compared to the same periods in 2018 to 2019. We find changes in population-weighted mean PM2.5 concentrations during the lockdowns of -11 to -15 µg/m3 across China, +1 to -2 µg/m3 across Europe, and 0 to -2 µg/m3 across North America. We explain these changes through a combination of meteorology and emission reductions, mostly due to transportation. This work demonstrates regional differences in the sensitivity of PM2.5 to emission sources.

Large global variations in measured airborne metal concentrations driven by anthropogenic sources.

Globally consistent measurements of airborne metal concentrations in fine particulate matter (PM2.5) are important for understanding potential health impacts, prioritizing air pollution mitigation strategies, and enabling global chemical transport model development. PM2.5 filter samples (N ~ 800 from 19 locations) collected from a globally distributed surface particulate matter sampling network (SPARTAN) between January 2013 and April 2019 were analyzed for particulate mass and trace metals content. Metal concentrations exhibited pronounced spatial variation, primarily driven by anthropogenic activities. PM2.5 levels of lead, arsenic, chromium, and zinc were significantly enriched at some locations by factors of 100-3000 compared to crustal concentrations. Levels of metals in PM2.5 and PM10 exceeded health guidelines at multiple sites. For example, Dhaka and Kanpur sites exceeded the US National Ambient Air 3-month Quality Standard for lead (150 ng m-3). Kanpur, Hanoi, Beijing and Dhaka sites had annual mean arsenic concentrations that approached or exceeded the World Health Organization's risk level for arsenic (6.6 ng m-3). The high concentrations of several potentially harmful metals in densely populated cites worldwide motivates expanded measurements and analyses.

Global Estimates and Long-Term Trends of Fine Particulate Matter Concentrations (1998-2018).

Exposure to outdoor fine particulate matter (PM2.5) is a leading risk factor for mortality. We develop global estimates of annual PM2.5 concentrations and trends for 1998-2018 using advances in satellite observations, chemical transport modeling, and ground-based monitoring. Aerosol optical depths (AODs) from advanced satellite products including finer resolution, increased global coverage, and improved long-term stability are combined and related to surface PM2.5 concentrations using geophysical relationships between surface PM2.5 and AOD simulated by the GEOS-Chem chemical transport model with updated algorithms. The resultant annual mean geophysical PM2.5 estimates are highly consistent with globally distributed ground monitors (R2 = 0.81; slope = 0.90). Geographically weighted regression is applied to the geophysical PM2.5 estimates to predict and account for the residual bias with PM2.5 monitors, yielding even higher cross validated agreement (R2 = 0.90-0.92; slope = 0.90-0.97) with ground monitors and improved agreement compared to all earlier global estimates. The consistent long-term satellite AOD and simulation enable trend assessment over a 21 year period, identifying significant trends for eastern North America (-0.28 ± 0.03 µg/m3/yr), Europe (-0.15 ± 0.03 µg/m3/yr), India (1.13 ± 0.15 µg/m3/yr), and globally (0.04 ± 0.02 µg/m3/yr). The positive trend (2.44 ± 0.44 µg/m3/yr) for India over 2005-2013 and the negative trend (-3.37 ± 0.38 µg/m3/yr) for China over 2011-2018 are remarkable, with implications for the health of billions of people.

Estimates of African Dust Deposition Along the Trans-Atlantic Transit Using the Decade-long Record of Aerosol Measurements from CALIOP, MODIS, MISR, and IASI.

Deposition of mineral dust into ocean fertilizes ecosystems and influences biogeochemical cycles and climate. In-situ observations of dust deposition are scarce, and model simulations depend on the highly parameterized representations of dust processes with few constraints. By taking advantage of satellites' routine sampling on global and decadal scales, we estimate African dust deposition flux and loss frequency (LF, a ratio of deposition flux to mass loading) along the trans-Atlantic transit using the three-dimensional distributions of aerosol retrieved by spaceborne lidar (CALIOP) and radiometers (MODIS, MISR, and IASI). On the basis of a ten-year (2007-2016) and basin scale average, the amount of dust deposition into the tropical Atlantic Ocean is estimated at 136 - 222 Tg yr-1. The 65-83% of satellite-based estimates agree with the in-situ climatology within a factor of 2. The magnitudes of dust deposition are highest in boreal summer and lowest in fall, whereas the interannual variability as measured by the normalized standard deviation with mean is largest in spring (28-41%) and smallest (7-15%) in summer. The dust deposition displays high spatial heterogeneity, revealing that the meridional shifts of major dust deposition belts are modulated by the seasonal migration of the intertropical convergence zone (ITCZ). On the basis of the annual and basin mean, the dust LF derived from the satellite observations ranges from 0.078 to 0.100 d-1, which is lower than model simulations by up to factors of 2 to 5. The most efficient loss of dust occurs in winter, consistent with the higher possibility of low-altitude transported dust in southern trajectories being intercepted by rainfall associated with the ITCZ. The satellite-based estimates of dust deposition can be used to fill the geographical gaps and extend time span of in-situ measurements, study the dust-ocean interactions, and evaluate model simulations of dust processes.

Constraining chemical transport PM2.5 modeling outputs using surface monitor measurements and satellite retrievals: application over the San Joaquin Valley.

Advances in satellite retrieval of aerosol type can improve the accuracy of near-surface air quality characterization by providing broad regional context and decreasing metric uncertainties and errors. The frequent, spatially extensive and radiometrically consistent instantaneous constraints can be especially useful in areas away from ground monitors and progressively downwind of emission sources. We present a physical approach to constraining regional-scale estimates of PM2.5, its major chemical component species estimates, and related uncertainty estimates of chemical transport model (CTM; e.g., the Community Multi-scale Air Quality Model) outputs. This approach uses ground-based monitors where available, combined with aerosol optical depth and qualitative constraints on aerosol size, shape, and light-absorption properties from the Multi-angle Imaging SpectroRadiometer (MISR) on the NASA Earth Observing System's Terra satellite. The CTM complements these data by providing complete spatial and temporal coverage. Unlike widely used approaches that train statistical regression models, the technique developed here leverages CTM physical constraints such as the conservation of aerosol mass and meteorological consistency, independent of observations. The CTM also aids in identifying relationships between observed species concentrations and emission sources. Aerosol air mass types over populated regions of central California are characterized using satellite data acquired during the 2013 San Joaquin field deployment of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) project. We investigate the optimal application of incorporating 275 m horizontal-resolution aerosol air-mass-type maps and total-column aerosol optical depth from the MISR Research Aerosol retrieval algorithm (RA) into regional-scale CTM output. The impact on surface PM2.5 fields progressively downwind of large single sources is evaluated using contemporaneous surface observations. Spatiotemporal R 2 and RMSE values for the model, constrained by both satellite and surface monitor measurements based on 10-fold cross-validation, are 0.79 and 0.33 for PM2.5, 0.88 and 0.65 for NO3 -, 0.78 and 0.23 for SO4 2-, and 1.01 for NH+, 0.73 and 0.23 for OC, and 0.31 and 0.65 for EC, respectively. Regional cross-validation temporal and spatiotemporal R2 results for the satellite-based PM2.5 improve by 30 % and 13 %, respectively, in comparison to unconstrained CTM simulations and provide finer spatial resolution. SO4 2- cross-validation values showed the largest spatial and spatiotemporal R2 improvement, with a 43 % increase. Assessing this physical technique in a well- instrumented region opens the possibility of applying it globally, especially over areas where surface air quality measurements are scarce or entirely absent.

Global Sources of Fine Particulate Matter: Interpretation of PM2.5 Chemical Composition Observed by SPARTAN using a Global Chemical Transport Model.

Exposure to ambient fine particulate matter (PM2.5) is a leading risk factor for the global burden of disease. However, uncertainty remains about PM2.5 sources. We use a global chemical transport model (GEOS-Chem) simulation for 2014, constrained by satellite-based estimates of PM2.5 to interpret globally dispersed PM2.5 mass and composition measurements from the ground-based surface particulate matter network (SPARTAN). Measured site mean PM2.5 composition varies substantially for secondary inorganic aerosols (2.4-19.7 µg/m3), mineral dust (1.9-14.7 µg/m3), residual/organic matter (2.1-40.2 µg/m3), and black carbon (1.0-7.3 µg/m3). Interpretation of these measurements with the GEOS-Chem model yields insight into sources affecting each site. Globally, combustion sectors such as residential energy use (7.9 µg/m3), industry (6.5 µg/m3), and power generation (5.6 µg/m3) are leading sources of outdoor global population-weighted PM2.5 concentrations. Global population-weighted organic mass is driven by the residential energy sector (64%) whereas population-weighted secondary inorganic concentrations arise primarily from industry (33%) and power generation (32%). Simulation-measurement biases for ammonium nitrate and dust identify uncertainty in agricultural and crustal sources. Interpretation of initial PM2.5 mass and composition measurements from SPARTAN with the GEOS-Chem model constrained by satellite-based PM2.5 provides insight into sources and processes that influence the global spatial variation in PM2.5 composition.

Karymsky volcano eruptive plume properties based on MISR multi-angle imagery, and volcanological implications.

Space-based, operational instruments are in unique positions to monitor volcanic activity globally, especially in remote locations or where suborbital observing conditions are hazardous. The Multi-angle Imaging SpectroRadiometer (MISR) provides hyper-stereo imagery, from which the altitude and microphysical properties of suspended atmospheric aerosols can be derived. These capabilities are applied to plumes emitted at Karymsky volcano from 2000 to 2017. Observed plumes from Karymsky were emitted predominantly to an altitude of 2-4 km, with occasional events exceeding 6 km. MISR plume observations were most common when volcanic surface manifestations, such as lava flows, were identified by satellite-based thermal anomaly detection. The analyzed plumes predominantly contained large (1.28 µm effective radius), strongly absorbing particles indicative of ash-rich eruptions. Differences between the retrievals for Karymsky volcano's ash-rich plumes and the sulfur-rich plumes emitted during the 2014-2015 eruption of Holuhraun (Iceland) highlight the ability of MISR to distinguish particle types from such events. Observed plumes ranged from 30 to 220 km in length, and were imaged at a spatial resolution of 1.1 km. Retrieved particle properties display evidence of downwind particle fallout, particle aggregation and chemical evolution. In addition, changes in plume properties retrieved from the remote-sensing observations over time are interpreted in terms of shifts in eruption dynamics within the volcano itself, corroborated to the extent possible with suborbital data. Plumes emitted at Karymsky prior to 2010 display mixed emissions of ash and sulfate particles. After 2010, all plumes contain consistent particle components, indicative of entering an ash-dominated regime. Post-2010 event timing, relative to eruption phase, was found to influence the optical properties of observed plume particles, with light-absorption varying in a consistent sequence as each respective eruption phase progressed.

Aerosol Absorption: Progress Towards Global and Regional Constraints.

PURPOSE OF REVIEW: Some aerosols absorb solar radiation, altering cloud properties, atmospheric stability and circulation dynamics, and the water cycle. Here we review recent progress towards global and regional constraints on aerosol absorption from observations and modeling, considering physical properties and combined approaches crucial for understanding the total (natural and anthropogenic) influences of aerosols on the climate. RECENT FINDINGS: We emphasize developments in black carbon absorption alteration due to coating and ageing, brown carbon characterization, dust composition, absorbing aerosol above cloud, source modeling and size distributions, and validation of high-resolution modeling against a range of observations. SUMMARY: Both observations and modeling of total aerosol absorption, absorbing aerosol optical depths and single scattering albedo, as well as the vertical distribution of atmospheric absorption, still suffer from uncertainties and unknowns significant for climate applications. We offer a roadmap of developments needed to bring the field substantially forward.

Distinguishing remobilized ash from erupted volcanic plumes using space-borne multi-angle imaging.

Volcanic systems are comprised of a complex combination of ongoing eruptive activity and secondary hazards, such as remobilized ash plumes. Similarities in the visual characteristics of remobilized and erupted plumes, as imaged by satellite-based remote sensing, complicate the accurate classification of these events. The stereo imaging capabilities of the Multi-angle Imaging SpectroRadiometer (MISR) were used to determine the altitude and distribution of suspended particles. Remobilized ash shows distinct dispersion, with particles distributed within ~1.5 km of the surface. Particle transport is consistently constrained by local topography, limiting dispersion pathways downwind. The MISR Research Aerosol (RA) retrieval algorithm was used to assess plume particle microphysical properties. Remobilized ash plumes displayed a dominance of large particles with consistent absorption and angularity properties, distinct from emitted plumes. The combination of vertical distribution, topographic control, and particle microphysical properties makes it possible to distinguish remobilized ash flows from eruptive plumes, globally.

Reducing Multi-sensor Monthly Mean Aerosol Optical Depth Uncertainty Part II: Optimal Locations for Potential Ground Observation Deployments.

Surface remote sensing of aerosol properties provides "ground truth" for satellite and model validation, and is an important component of aerosol observation system. Due to the different characteristics of background aerosol variability, information obtained at different locations usually have different spatial representativeness, implying that the location should be carefully chosen so that its measurement could be extended to a greater area. In this study, we present an objective observation array design technique that automatically determines the optimal locations with the highest spatial representativeness based on the Ensemble Kalman Filter (EnKF) theory. The ensemble is constructed using aerosol optical depth (AOD) products from five satellite sensors. The optimal locations are solved sequentially by minimizing the total analysis error variance, which means that observations at these locations will reduce the background error variance to the largest extent. The location determined by the algorithm is further verified to have larger spatial representativeness than some other arbitrary location. In addition to the existing active AERONET sites, the 40 selected optimal locations are mostly concentrated on regions with both high AOD inhomogeneity and its spatial representativeness, namely the Sahel, South Africa, East Asia and North Pacific Islands. These places should be the focuses of establishing future AERONET sites in order to further reduce the uncertainty in the monthly mean AOD. Observations at these locations contribute to approximately 50% of the total background uncertainty reduction.

Aerosol indirect effects on the nighttime Arctic Ocean surface from thin, predominantly liquid clouds.

Aerosol indirect effects have potentially large impacts on the Arctic Ocean surface energy budget, but model estimates of regional-scale aerosol indirect effects are highly uncertain and poorly validated by observations. Here we demonstrate a new way to quantitatively estimate aerosol indirect effects on a regional scale from remote sensing observations. In this study, we focus on nighttime, optically thin, predominantly liquid clouds. The method is based on differences in cloud physical and microphysical characteristics in carefully selected clean, average and aerosol-impacted conditions. The cloud subset of focus covers just ~5% of cloudy Arctic Ocean regions, warming the Arctic Ocean surface by ~1-1.4 W m-2 regionally during polar night. However, within this cloud subset, aerosol and cloud conditions can be determined with high confidence using CALIPSO and CloudSat data and model output. This cloud subset is generally susceptible to aerosols, with a polar nighttime estimated maximum regionally integrated indirect cooling effect of ~ -0.11 W m-2 at the Arctic sea ice surface (~10% of the clean background cloud effect), excluding cloud fraction changes. Aerosol presence is related to reduced precipitation, cloud thickness, and radar reflectivity, and in some cases, an increased likelihood of cloud presence in the liquid phase. These observations are inconsistent with a glaciation indirect effect and are consistent with either a deactivation effect or less efficient secondary ice formation related to smaller liquid cloud droplets. However, this cloud subset shows large differences in surface and meteorological forcing in shallow and higher altitude clouds and between sea ice and open ocean regions. For example, optically thin, predominantly liquid clouds are much more likely to overlay another cloud over the open ocean, which may reduce aerosol indirect effects on the surface. Also, shallow clouds over open ocean do not appear to respond to aerosols as strongly as over stratified sea ice environments, indicating a larger influence of meteorological forcing over aerosol microphysics in these types of clouds over the rapidly changing Arctic Ocean.

SAM-CAAM: A Concept for Acquiring Systematic Aircraft Measurements to Characterize Aerosol Air Masses.

A modest operational program of systematic aircraft measurements can resolve key satellite-aerosol-data-record limitations. Satellite observations provide frequent, global aerosol-amount maps, but offer only loose aerosol property constraints needed for climate and air quality applications. We define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ. The flight program could characterize major aerosol air-mass types statistically, at a level-of-detail unobtainable from space. It would: (1) enhance satellite aerosol retrieval products with better climatology assumptions, and (2) improve translation between satellite-retrieved optical properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space, improve aerosol constraints on climate modeling, help interrelate remote-sensing, in situ, and modeling aerosol-type definitions, and contribute to future satellite aerosol missions. Fifteen Required Variables are identified, and four Payload Options of increasing ambition are defined, to constrain these quantities. "Option C" could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration, and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable, even if aerosol loading varies.

Improving our fundamental understanding of the role of aerosol-cloud interactions in the climate system.

The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth's clouds is the most uncertain component of the overall global radiative forcing from preindustrial time. General circulation models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol-cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions, but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol-cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. We suggest strategies for improving estimates of aerosol-cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.

Global Estimates of Fine Particulate Matter using a Combined Geophysical-Statistical Method with Information from Satellites, Models, and Monitors.

We estimated global fine particulate matter (PM2.5) concentrations using information from satellite-, simulation- and monitor-based sources by applying a Geographically Weighted Regression (GWR) to global geophysically based satellite-derived PM2.5 estimates. Aerosol optical depth from multiple satellite products (MISR, MODIS Dark Target, MODIS and SeaWiFS Deep Blue, and MODIS MAIAC) was combined with simulation (GEOS-Chem) based upon their relative uncertainties as determined using ground-based sun photometer (AERONET) observations for 1998-2014. The GWR predictors included simulated aerosol composition and land use information. The resultant PM2.5 estimates were highly consistent (R(2) = 0.81) with out-of-sample cross-validated PM2.5 concentrations from monitors. The global population-weighted annual average PM2.5 concentrations were 3-fold higher than the 10 µg/m(3) WHO guideline, driven by exposures in Asian and African regions. Estimates in regions with high contributions from mineral dust were associated with higher uncertainty, resulting from both sparse ground-based monitoring, and challenging conditions for retrieval and simulation. This approach demonstrates that the addition of even sparse ground-based measurements to more globally continuous PM2.5 data sources can yield valuable improvements to PM2.5 characterization on a global scale.