New seasonal pattern of pollution emerges from changing North American wildfires.

Rising emissions from wildfires over recent decades in the Pacific Northwest are known to counteract the reductions in human-produced aerosol pollution over North America. Since amplified Pacific Northwest wildfires are predicted under accelerating climate change, it is essential to understand both local and transported contributions to air pollution in North America. Here, we find corresponding increases for carbon monoxide emitted from the Pacific Northwest wildfires and observe significant impacts on both local and down-wind air pollution. Between 2002 and 2018, the Pacific Northwest atmospheric carbon monoxide abundance increased in August, while other months showed decreasing carbon monoxide, so modifying the seasonal pattern. These seasonal pattern changes extend over large regions of North America, to the Central USA and Northeast North America regions, indicating that transported wildfire pollution could potentially impact the health of millions of people.

Improving surface PM2.5 forecasts in the United States using an ensemble of chemical transport model outputs: 2. bias correction with satellite data for rural areas.

This work serves as the second of a two-part study to improve surface PM2.5 forecasts in the continental U.S. through the integrated use of multi-satellite aerosol optical depth (AOD) products (MODIS Terra/Aqua and VIIRS DT/DB), multi chemical transport model (CTM) (GEOS-Chem, WRF-Chem and CMAQ) outputs and ground observations. In part I of the study, a multi-model ensemble Kalman filter (KF) technique using three CTM outputs and ground observations was developed to correct forecast bias and generate a single best forecast of PM2.5 for next day over non-rural areas that have surface PM2.5 measurements in the proximity of 125 km. Here, with AOD data, we extended the bias correction into rural areas where the closest air quality monitoring station is at least 125 - 300 km away. First, we ensembled all of satellite AOD products to yield the single best AOD. Second, we corrected daily PM2.5 in rural areas from multiple models through the AOD spatial pattern between these areas and non-rural areas, referred to as "extended ground truth" or EGT, for today. Lastly, we applied the KF technique to update the bias in the forecast for next day using the EGT. Our results find that the ensemble of bias-corrected daily PM2.5 from three models for both today and next day show the best performance. Together, the two-part study develops a multi-model and multi-AOD bias correction technique that has the potential to improve PM2.5 forecasts in both rural and non-rural areas in near real time, and be readily implemented at state levels.

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.

Interannual variability and trends of combustion aerosol and dust in major continental outflows revealed by MODIS retrievals and CAM5 simulations during 2003-2017.

Emissions and long-range transport of mineral dust and combustion-related aerosol from burning fossil fuels and biomass vary from year to year, driven by the evolution of the economy and changes in meteorological conditions and environmental regulations. This study offers both satellite and model perspectives on the interannual variability and possible trends of combustion aerosol and dust in major continental outflow regions over the past 15 years (2003-2017). The decade-long record of aerosol optical depth (AOD, denoted as τ), separately for combustion aerosol (τ c) and dust (τ d), over global oceans is derived from the Collection 6 aerosol products of the Moderate Resolution Imaging Spectroradiometer (MODIS) onboard both Terra and Aqua. These MODIS Aqua datasets, complemented by aerosol source-tagged simulations using the Community Atmospheric Model version 5 (CAM5), are then analyzed to understand the interannual variability and potential trends of τ c and τ d in the major continental outflows. Both MODIS and CAM5 consistently yield a similar decreasing trend of -0.017 to -0.020 per decade for τ c over the North Atlantic Ocean and the Mediterranean Sea that is attributable to reduced emissions from North America and Europe, respectively. On the contrary, both MODIS and CAM5 display an increasing trend of +0.017 to +0.036 per decade for τ c over the tropical Indian Ocean, the Bay of Bengal, and the Arabian Sea, which reflects the influence of increased anthropogenic emissions from South Asia and the Middle East in the last 2 decades. Over the northwestern Pacific Ocean, which is often affected by East Asian emissions of pollution and dust, the MODIS retrievals show a decreasing trend of -0.021 per decade for τ c and -0.012 per decade for τ d, which is, however, not reproduced by the CAM5 model. In other outflow regions strongly influenced by biomass burning smoke or dust, both MODIS retrievals and CAM5 simulations show no statistically significant trends; the MODIS-observed interannual variability is usually larger than that of the CAM5 simulation.

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.

Exploring aerosols near clouds with high-spatial-resolution aircraft remote sensing during SEAC4RS.

Since aerosols are important to our climate system, we seek to observe the variability of aerosol properties within cloud systems. When applied to the satellite-borne Moderate-resolution Imaging Spectroradiometer (MODIS), the Dark Target (DT) retrieval algorithm provides global aerosol optical depth (AOD at 0.55 µm) in cloud-free scenes. Since MODIS' resolution (500 m pixels, 3 km or 10 km product) is too coarse for studying near-cloud aerosol, we ported the DT algorithm to the high-resolution (~50 m pixels) enhanced-MODIS Airborne Simulator (eMAS), which flew on the high-altitude ER-2 during the Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) Airborne Science Campaign over the U.S. in 2013. We find that even with aggressive cloud screening, the ~0.5 km eMAS retrievals show enhanced AOD, especially within 6 km of a detected cloud. To determine the cause of the enhanced AOD, we analyze additional eMAS products (cloud retrievals and degraded-resolution AOD), co-registered Cloud Physics Lidar (CPL) profiles, MODIS aerosol retrievals, and ground-based Aerosol Robotic Network (AERONET) observations. We also define spatial metrics to indicate local cloud distributions near each retrieval, and then separate into near-cloud and far-from-cloud environments. The comparisons show that low cloud masking is robust, and unscreened thin cirrus would have only a small impact on retrieved AOD. Some of the enhancement is consistent with clear-cloud transition zone microphysics such as aerosol swelling. However, 3D radiation interaction between clouds and the surrounding clear air appears to be the primary cause of the high AOD near clouds.

Exploring systematic offsets between aerosol products from the two MODIS sensors.

Long-term measurements of global aerosol loading and optical properties are essential for assessing climate-related questions. Using observations of spectral reflectance and radiance, the dark-target (DT) aerosol retrieval algorithm is applied to Moderate-resolution Imaging Spectroradiometer sensors on both Terra (MODIS-T) and Aqua (MODIS-A) satellites, deriving products (known as MOD04 and MYD04, respectively) of global aerosol optical depth (AOD at 0.55 µm) over both land and ocean, and Angstrom Exponent (AE derived from 0.55 and 0.86 µm) over ocean. Here, we analyse the overlapping time series (since mid-2002) of the Collection 6 (C6) aerosol products. Global monthly mean AOD from MOD04 (Terra with morning overpass) is consistently higher than MYD04 (Aqua with afternoon overpass) by ~13% (~0.02 over land and ~0.015 over ocean), and this offset (MOD04 - MYD04), has seasonal as well as long-term variability. Focusing on 2008, and deriving yearly gridded mean AOD and AE, we find that over ocean, the MOD04 (morning) AOD is higher and the AE is lower. Over land, there is more variability, but only biomass-burning regions tend to have AOD lower for MOD04. Using simulated aerosol fields from the Goddard Earth Observing System (GEOS-5) Earth system model, and sampling separately (in time and space) along each MODIS-observed swath during 2008, the magnitudes of morning versus afternoon offsets of AOD and AE are smaller than those in the C6 products. Since the differences are not easily attributed to either aerosol diurnal cycles or sampling issues, we test additional corrections to the input reflectance data. The first, known as C6+, corrects for long-term changes to each sensors' polarization sensitivity, response-versus-scan angle, and to cross-calibration from MODIS-T to MODIS-A. A second convolves the de-trending and cross-calibration into scaling factors. Each method was applied upstream of the aerosol retrieval, using 2008 data. While both methods reduced the overall AOD offset over land from 0.02 to 0.01, neither significantly reduced the AOD offset over ocean. The overall negative AE offset was reduced. A Collection (C6.1) of all MODIS-atmosphere products was released, but we expect that the C6.1 aerosol products will maintain similar overall AOD and AE offsets. We conclude that: a) users should not interpret global differences between Terra and Aqua aerosol products as representing a true diurnal signal in the aerosol. b) Because the MODIS-A product appears to have overall smaller bias compared to ground-truth, it may be more suitable for some applications, however c) since the AOD offset is only ~0.02 and within noise level for single retrievals, both MODIS products may be adequate for most applications.

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.

MODIS Retrieval of Aerosol Optical Depth over Turbid Coastal Water.

We present a new approach to retrieve Aerosol Optical Depth (AOD) using the Moderate Resolution Imaging Spectroradiometer (MODIS) over the turbid coastal water. This approach supplements the operational Dark Target (DT) aerosol retrieval algorithm that currently does not conduct AOD retrieval in shallow waters that have visible sediments or sea-floor (i.e., Class 2 waters). Over the global coastal water regions in cloud-free conditions, coastal screening leads to ~20% unavailability of AOD retrievals. Here, we refine the MODIS DT algorithm by considering that water-leaving radiance at 2.1 µm to be negligible regardless of water turbidity, and therefore the 2.1 µm reflectance at the top of the atmosphere is sensitive to both change of fine-mode and coarse-mode AODs. By assuming that the aerosol single scattering properties over coastal turbid water are similar to those over the adjacent open-ocean pixels, the new algorithm can derive AOD over these shallow waters. The test algorithm yields ~18% more MODIS-AERONET collocated pairs for six AERONET stations in the coastal water regions. Furthermore, comparison of the new retrieval with these AERONET observations show that the new AOD retrievals have equivalent or better accuracy than those retrieved by the MODIS operational algorithm's over coastal land and non-turbid coastal water product. Combining the new retrievals with the existing MODIS operational retrievals yields an overall improvement of AOD over those coastal water regions. Most importantly, this refinement extends the spatial and temporal coverage of MODIS AOD retrievals over the coastal regions where 60% of human population resides. This expanded coverage is crucial for better understanding of impact of aerosol particles on coastal air quality and climate.

Retrieval of aerosol optical properties using MERIS observations: Algorithm and some first results.

The MEdium Resolution Imaging Spectrometer (MERIS) instrument on board ESA Envisat made measurements from 2002 to 2012. Although MERIS was limited in spectral coverage, accurate Aerosol Optical Thickness (AOT) from MERIS data are retrieved by using appropriate additional information. We introduce a new AOT retrieval algorithm for MERIS over land surfaces, referred to as eXtensible Bremen AErosol Retrieval (XBAER). XBAER is similar to the "dark-target" (DT) retrieval algorithm used for Moderate-resolution Imaging Spectroradiometer (MODIS), in that it uses a lookup table (LUT) to match to satellite-observed reflectance and derive the AOT. Instead of a global parameterization of surface spectral reflectance, XBAER uses a set of spectral coefficients to prescribe surface properties. In this manner, XBAER is not limited to dark surfaces (vegetation) and retrieves AOT over bright surface (desert, semiarid, and urban areas). Preliminary validation of the MERIS-derived AOT and the ground-based Aerosol Robotic Network (AERONET) measurements yield good agreement, the resulting regression equation is y = (0.92 × ± 0.07) + (0.05 ± 0.01) and Pearson correlation coefficient of R = 0.78. Global monthly means of AOT have been compared from XBAER, MODIS and other satellite-derived datasets.

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.