Anthropogenic Decline of African Dust: Insights From the Holocene Records and Beyond.

African dust exhibits strong variability on a range of time scales. Here we show that the interhemispheric contrast in Atlantic SST (ICAS) drives African dust variability at decadal to millennial timescales, and the strong anthropogenic increase of the ICAS in the future will decrease African dust loading to a level never seen during the Holocene. We provide a physical framework to understand the relationship between the ICAS and African dust activity: positive ICAS anomalies push the Intertropical Convergence Zone (ITCZ) northward and decrease surface wind speed over African dust source regions, which reduces dust emission and transport. It provides a unified framework for and is consistent with relationships in the literature. We find strong observational and proxy-record support for the ICAS-ITCZ-dust relationship during the past 160 and 17,000 years. Model-projected anthropogenic increase of the ICAS will reduce African dust by as much as 60%, which has broad consequences.

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.

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.

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.

Atmospheric Correction of Satellite Ocean-Color Imagery During the PACE Era.

The Plankton, Aerosol, Cloud, ocean Ecosystem (PACE) mission will carry into space the Ocean Color Instrument (OCI), a spectrometer measuring at 5nm spectral resolution in the ultraviolet (UV) to near infrared (NIR) with additional spectral bands in the shortwave infrared (SWIR), and two multi-angle polarimeters that will overlap the OCI spectral range and spatial coverage, i. e., the Spectrometer for Planetary Exploration (SPEXone) and the Hyper-Angular Rainbow Polarimeter (HARP2). These instruments, especially when used in synergy, have great potential for improving estimates of water reflectance in the post Earth Observing System (EOS) era. Extending the top-of-atmosphere (TOA) observations to the UV, where aerosol absorption is effective, adding spectral bands in the SWIR, where even the most turbid waters are black and sensitivity to the aerosol coarse mode is higher than at shorter wavelengths, and measuring in the oxygen A-band to estimate aerosol altitude will enable greater accuracy in atmospheric correction for ocean color science. The multi-angular and polarized measurements, sensitive to aerosol properties (e.g., size distribution, index of refraction), can further help to identify or constrain the aerosol model, or to retrieve directly water reflectance. Algorithms that exploit the new capabilities are presented, and their ability to improve accuracy is discussed. They embrace a modern, adapted heritage two-step algorithm and alternative schemes (deterministic, statistical) that aim at inverting the TOA signal in a single step. These schemes, by the nature of their construction, their robustness, their generalization properties, and their ability to associate uncertainties, are expected to become the new standard in the future. A strategy for atmospheric correction is presented that ensures continuity and consistency with past and present ocean-color missions while enabling full exploitation of the new dimensions and possibilities. Despite the major improvements anticipated with the PACE instruments, gaps/issues remain to be filled/tackled. They include dealing properly with whitecaps, taking into account Earth-curvature effects, correcting for adjacency effects, accounting for the coupling between scattering and absorption, modeling accurately water reflectance, and acquiring a sufficiently representative dataset of water reflectance in the UV to SWIR. Dedicated efforts, experimental and theoretical, are in order to gather the necessary information and rectify inadequacies. Ideas and solutions are put forward to address the unresolved issues. Thanks to its design and characteristics, the PACE mission will mark the beginning of a new era of unprecedented accuracy in ocean-color radiometry from space.

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.

Plankton Aerosol, Cloud, Ocean Ecosystem Mission: atmosphere measurements for air quality applications.

We present the instrumentation and products of the NASA Plankton Aerosol, Cloud, ocean Ecosystem (PACE) mission relevant to air quality management. Since PACE will launch in the 2022 to 2023 timeframe, this paper discusses several activities in anticipation of a robust air quality applications program using PACE products. Products from the PACE ocean color imager and two multiangle polarimeters will be used synergistically to retrieve properties relevant to air quality applications. These instruments provide high spectral and spatial resolution measurements used to derive key properties of aerosols and clouds including effective particle radii, particle shapes, aerosol and cloud optical depths, refractive indices and single scattering albedos all of which are critical for characterizing airmasses for managing air quality, hazardous episodes of wildfire and volcanic emissions, and long range transport of pollution. Because of the number of products with potential societal benefits, the PACE mission is highly pertinent to NASA's Applied Sciences Program's efforts to promote, discover, and demonstrate innovative, practical, and sustainable uses of the Earth observations. We discuss plans to support these efforts by establishing a prelaunch early adopter program and outline communication strategies to engage the air quality user community.

Retrievals of aerosol optical and microphysical properties from Imaging Polar Nephelometer scattering measurements.

A method for the retrieval of aerosol optical and microphysical properties from in situ light-scattering measurements is presented and the results are compared with existing measurement techniques. The Generalized Retrieval of Aerosol and Surface Properties (GRASP) is applied to airborne and laboratory measurements made by a novel polar nephelometer. This instrument, the Polarized Imaging Nephelometer (PI-Neph), is capable of making high-accuracy field measurements of phase function and degree of linear polarization, at three visible wavelengths, over a wide angular range of 3 to 177°. The resulting retrieval produces particle size distributions (PSDs) that agree, within experimental error, with measurements made by commercial optical particle counters (OPCs). Additionally, the retrieved real part of the refractive index is generally found to be within the predicted error of 0.02 from the expected values for three species of humidified salt particles, with a refractive index that is well established. The airborne measurements used in this work were made aboard the NASA DC-8 aircraft during the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field campaign, and the inversion of this data represents the first aerosol retrievals of airborne polar nephelometer data. The results provide confidence in the real refractive index product, as well as in the retrieval's ability to accurately determine PSD, without assumptions about refractive index that are required by the majority of OPCs.

Aerosols from overseas rival domestic emissions over North America.

Many types of aerosols have lifetimes long enough for their transcontinental transport, making them potentially important contributors to air quality and climate change in remote locations. We estimate that the mass of aerosols arriving at North American shores from overseas is comparable with the total mass of particulates emitted domestically. Curbing domestic emissions of particulates and precursor gases, therefore, is not sufficient to mitigate aerosol impacts in North America. The imported contribution is dominated by dust leaving Asia, not by combustion-generated particles. Thus, even a reduction of industrial emissions of the emerging economies of Asia could be overwhelmed by an increase of dust emissions due to changes in meteorological conditions and potential desertification.

Smoke invigoration versus inhibition of clouds over the Amazon.

The effect of anthropogenic aerosols on clouds is one of the most important and least understood aspects of human-induced climate change. Small changes in the amount of cloud coverage can produce a climate forcing equivalent in magnitude and opposite in sign to that caused by anthropogenic greenhouse gases, and changes in cloud height can shift the effect of clouds from cooling to warming. Focusing on the Amazon, we show a smooth transition between two opposing effects of aerosols on clouds: the microphysical and the radiative. We show how a feedback between the optical properties of aerosols and the cloud fraction can modify the aerosol forcing, changing the total radiative energy and redistributing it over the atmospheric column.

The effect of smoke, dust, and pollution aerosol on shallow cloud development over the Atlantic Ocean.

Clouds developing in a polluted environment tend to have more numerous but smaller droplets. This property may lead to suppression of precipitation and longer cloud lifetime. Absorption of incoming solar radiation by aerosols, however, can reduce the cloud cover. The net aerosol effect on clouds is currently the largest uncertainty in evaluating climate forcing. Using large statistics of 1-km resolution MODIS (Moderate Resolution Imaging Spectroradiometer) satellite data, we study the aerosol effect on shallow water clouds, separately in four regions of the Atlantic Ocean, for June through August 2002: marine aerosol (30 degrees S-20 degrees S), smoke (20 degrees S-5 degrees N), mineral dust (5 degrees N-25 degrees N), and pollution aerosols (30 degrees N- 60 degrees N). All four aerosol types affect the cloud droplet size. We also find that the coverage of shallow clouds increases in all of the cases by 0.2-0.4 from clean to polluted, smoky, or dusty conditions. Covariability analysis with meteorological parameters associates most of this change to aerosol, for each of the four regions and 3 months studied. In our opinion, there is low probability that the net aerosol effect can be explained by coincidental, unresolved, changes in meteorological conditions that also accumulate aerosol, or errors in the data, although further in situ measurements and model developments are needed to fully understand the processes. The radiative effect at the top of the atmosphere incurred by the aerosol effect on the shallow clouds and solar radiation is -11 +/- 3 W/m2 for the 3 months studied; 2/3 of it is due to the aerosol-induced cloud changes, and 1/3 is due to aerosol direct radiative effect.

Measurement of the effect of Amazon smoke on inhibition of cloud formation.

Urban air pollution and smoke from fires have been modeled to reduce cloud formation by absorbing sunlight, thereby cooling the surface and heating the atmosphere. Satellite data over the Amazon region during the biomass burning season showed that scattered cumulus cloud cover was reduced from 38%in clean conditions to 0%for heavy smoke (optical depth of 1.3). This response to the smoke radiative effect reverses the regional smoke instantaneous forcing of climate from -28 watts per square meter in cloud-free conditions to +8 watts per square meter once the reduction of cloud cover is accounted for.