Intercontinental transport of pollution and dust aerosols: implications for regional air quality

International audienceWe use the global model GOCART to examine the impact of pollution and dust aerosols emitted from their major sources on surface fine particulate matter concentrations at regional and hemispheric scales. Focusing on the North America region in 2001, we use measurements from the IMPROVE network in the United States to evaluate the model-simulated surface concentrations of the "reconstructed fine mass" (RCFM) and its components of ammonium sulfate, black carbon (BC), organic matter (OM), and fine mode dust. We then quantify the RCFM budget in terms of the RCFM composition, type, and origin to find that in the eastern U.S., ammonium sulfate is the dominant RCFM component (~60%) whereas in the western U.S., dust and OM are just as important as sulfate but have considerable seasonal variations, especially in the NW. On an annual average, North America regional pollution accounts for nearly 30?40% of the surface RCFM in the western U.S., and for a much higher proportion of 65?70% in the eastern U.S. By contrast, pollution from outside of North America contributes to just 2?6% (~0.2 ?g m?3) of the total RCFM over the U.S. on an annual average. In comparison, long-range transport of dust is more efficient than that of pollution, which brings 3 to 4 times more fine particles to the U.S. (0.5?0.8 ?g m?3 on an annual average) with a maximum influence in spring and over the NW. Of the major pollution regions, Europe has the largest potential to affect the surface aerosol concentrations in other continents due to its shorter distance from receptor continents and its larger fraction of sulfate-producing precursor gas in the outflow. With the IPCC emission scenario for the year 2000, we find that European emissions increase levels of ammonium sulfate by 1?5 ?g m?3 over the surface of northern Africa and western Asia, and its contribution to eastern Asia (?0.2 ?g m?3) is twice as much as the Asian contribution to North America. Asia and North America pollution emissions exert strong impacts on their neighboring oceans, but their influences on other continents are relatively small (?10%) due to the long traveling distance across the oceans and efficient removal during transport. Among the major dust source regions, Asia displays a significant influence over large areas in the Northern Hemisphere except over the North Atlantic and the tropics, where African dust dominates. The trans-Pacific transport of Asian dust is much more efficient than that of Asian pollution because of the higher elevation and lower removal rate of dust. We notice that the African dust can travel eastward through a pathway spanning across Asia and North Pacific to settle down over the surface of western North America. African dust transported through such a pathway is difficult to detect because it usually merges and travels together with the Asian dust

Monitoring the impact of desert dust outbreaks for air quality for health studies

We review the major features of desert dust outbreaks that are relevant to the assessment of dust impacts upon human health. Our ultimate goal is to provide scientific guidance for the acquisition of relevant population exposure information for epidemiological studies tackling the short and long term health effects of desert dust. We first describe the source regions and the typical levels of dust particles in regions close and far away from the source areas, along with their size, composition, and bio-aerosol load. We then describe the processes by which dust may become mixed with anthropogenic particulate matter (PM) and/or alter its load in receptor areas. Short term health effects are found during desert dust episodes in different regions of the world, but in a number of cases the results differ when it comes to associate the effects to the bulk PM, the desert dust-PM, or non-desert dust-PM. These differences are likely due to the different monitoring strategies applied in the epidemiological studies, and to the differences on atmospheric and emission (natural and anthropogenic) patterns of desert dust around the world. We finally propose methods to allow the discrimination of health effects by PM fraction during dust outbreaks, and a strategy to implement desert dust alert and monitoring systems for health studies and air quality management.The systematic review was funded by WHO with as part of a Grant Agreement with Ministry of Foreign Affairs, Norway. Thanks are also given to the Spanish Ministry for the Ecological Transition for long term support in the last 2 decades to our projects on African dust effects on air quality over Spain; to the Spanish Ministry of Science, Innovation and Universities and FEDER Funds for the HOUSE project (CGL2016-78594-R), and to the Generalitat de Catalunya (AGAUR 2017 SGR41). Carlos Pérez García-Pando acknowledges long-term support from the AXA Research Fund, as well as the support received through the Ramón y Cajal program (grant RYC-2015-18690) of the Spanish Ministry of Science, Innovation and Universities.Peer ReviewedPostprint (published version

Retrieving global sources of aerosols from MODIS observations by inverting GOCART model

International audienceKnowledge of the global distribution of tropospheric aerosols is important for studying the effects of aerosols on global climate. Chemical transport models rely on archived meteorological fields, accounting for aerosol sources, transport and removal processes can simulate the global distribution of atmospheric aerosols. However, the accuracy of global aerosol modeling is limited. Uncertainty in location and strength of aerosol emission sources is a major factor in limiting modeling accuracy. This paper describes an effort to develop an algorithm for retrieving global sources of aerosol from satellite observations by inverting the GOCART aerosol transport model. To optimize inversion algorithm performance, the inversion was formulated as a generalized multi-term least-squares-type fitting. This concept uses the principles of statistical optimization and unites diverse retrieval techniques into a single flexible inversion procedure. It is particularly useful for choosing and refining a priori constraints in the retrieval algorithm. For example, it is demonstrated that a priori limitations on the partial derivatives of retrieved characteristics, which are widely used in atmospheric remote sensing, can also be useful in inverse modeling for constraining time and space variability of the retrieved global aerosol emissions. The similarities and differences with the standard "Kalman filter" inverse modeling approach and the "Phillips-Tikhonov-Twomey" constrained inversion widely used in remote sensing are discussed. In order to retain the originally high space and time resolution of the global model in the inversion of a long record of observations, the algorithm was expressed using adjoint operators in a form convenient for practical development of the inversion from codes implementing forward model simulations. The inversion algorithm was implemented using the GOCART aerosol transport model. The numerical tests we conducted showed successful retrievals of global aerosol emissions with a 2°×2.5° resolution by inverting the GOCART output. For achieving satisfactory retrieval from satellite sensors such as MODIS, the emissions were assumed constant within the 24 h diurnal cycle and aerosol differences in chemical composition were neglected. Such additional assumptions were needed to constrain the inversion due to limitations of satellite temporal coverage and sensitivity to aerosol parameters. As a result, the algorithm was defined for the retrieval of emission sources of fine and coarse mode aerosols from the MODIS fine and coarse mode aerosol optical thickness data respectively. Numerical tests showed that such assumptions are justifiable, taking into account the accuracy of the model and observations and that it provides valuable retrievals of the location and the strength of the aerosol emissions. The algorithm was applied to MODIS observations during two weeks in August 2000. The global placement of fine mode aerosol sources retrieved from inverting MODIS observations was coherent with available independent knowledge. This was particularly encouraging since the inverse method did not use any a priori information about the sources and it was initialized under a "zero aerosol emission" assumption. The retrieval reproduced the instantaneous global MODIS observations with a standard deviation in fitting of aerosol optical thickness of ~0.04. The optical thickness during high aerosol loading events was reproduced with a standard deviation of ~48%. Applications of the algorithm for the retrieval of coarse mode aerosol emissions were less successful, mainly due to the currently existing lack of MODIS data over high reflectance desert dust sources. Possibilities for enhancing the global satellite data inversion by using diverse a priori constraints on the retrieval are demonstrated. The potential and limitations of applying our approach for the retrieval of global aerosol sources from aerosol remote sensing are discussed

How reliable are CMIP5 models in simulating dust optical depth?

Dust aerosol plays an important role in the climate system by affecting the radiative and energy balances. Biases in dust modeling may result in biases in simulating global energy budget and regional climate. It is thus very important to understand how well dust is simulated in the Coupled Model Intercomparison Project Phase 5 (CMIP5) models. Here seven CMIP5 models using interactive dust emission schemes are examined against satellite-derived dust optical depth (DOD) during 2004–2016.It is found that multi-model mean can largely capture the global spatial pattern and zonal mean of DOD over land in present-day climatology in MAM and JJA. Global mean land DOD is underestimated by −25.2&thinsp;% in MAM to −6.4&thinsp;% in DJF. While seasonal cycle, magnitude, and spatial pattern are generally captured by the multi-model mean over major dust source regions such as North Africa and the Middle East, these variables are not so well represented by most of the models in South Africa and Australia. Interannual variations in DOD are not captured by most of the models or by the multi-model mean. Models also do not capture the observed connections between DOD and local controlling factors such as surface wind speed, bareness, and precipitation. The constraints from surface bareness are largely underestimated while the influences of surface wind and precipitation are overestimated.Projections of DOD change in the late half of the 21st century under the Representative Concentration Pathways 8.5 scenario in which the multi-model mean is compared with that projected by a regression model. Despite the uncertainties associated with both projections, results show some similarities between the two, e.g., DOD pattern over North Africa in DJF and JJA, an increase in DOD in the central Arabian Peninsula in all seasons, and a decrease over northern China from MAM to SON.</p

Links between topography, wind, deflation, lakes and dust: The case of the Bodélé Depression, Chad

The Bodélé Depression, Chad is the planet's largest single source of dust. Deflation from the Bodélé could be seen as a simple coincidence of two key prerequisites: strong surface winds and a large source of suitable sediment. But here we hypothesise that long term links between topography, winds, deflation and dust ensure the maintenance of the dust source such that these two apparently coincidental key ingredients are connected by land-atmosphere processes with topography acting as the overall controlling agent. We use a variety of observational and numerical techniques, including a regional climate model, to show that: 1) contemporary deflation from the Bodélé is delineated by topography and a surface wind stress maximum; 2) the Tibesti and Ennedi mountains play a key role in the generation of the erosive winds in the form of the Bodélé Low Level Jet (LLJ); 3) enhanced deflation from a stronger Bodélé LLJ during drier phases, for example, the Last Glacial Maximum, was probably sufficient to create the shallow lake in which diatoms lived during wetter phases, such as the Holocene pluvial. Winds may therefore have helped to create the depression in which erodible diatom material accumulated. Instead of a simple coincidence of nature, dust from the world's largest source may result from the operation of long term processes on paleo timescales which have led to ideal conditions for dust generation in the world's largest dust source. Similar processes plausibly operate in other dust hotspots in topographic depressions

Retrieving global aerosol sources from satellites using inverse modeling

International audienceUnderstanding aerosol effects on global climate requires knowing the global distribution of tropospheric aerosols. By accounting for aerosol sources, transports, and removal processes, chemical transport models simulate the global aerosol distribution using archived meteorological fields. We develop an algorithm for retrieving global aerosol sources from satellite observations of aerosol distribution by inverting the GOCART aerosol transport model. The inversion is based on a generalized, multi-term least-squares-type fitting, allowing flexible selection and refinement of a priori algorithm constraints. For example, limitations can be placed on retrieved quantity partial derivatives, to constrain global aerosol emission space and time variability in the results. Similarities and differences between commonly used inverse modeling and remote sensing techniques are analyzed. To retain the high space and time resolution of long-period, global observational records, the algorithm is expressed using adjoint operators. Successful global aerosol emission retrievals at 2°×2.5 resolution were obtained by inverting GOCART aerosol transport model output, assuming constant emissions over the diurnal cycle, and neglecting aerosol compositional differences. In addition, fine and coarse mode aerosol emission sources were inverted separately from MODIS fine and coarse mode aerosol optical thickness data, respectively. These assumptions are justified, based on observational coverage and accuracy limitations, producing valuable aerosol source locations and emission strengths. From two weeks of daily MODIS observations during August 2000, the global placement of fine mode aerosol sources agreed with available independent knowledge, even though the inverse method did not use any a priori information about aerosol sources, and was initialized with a "zero aerosol emission" assumption. Retrieving coarse mode aerosol emissions was less successful, mainly because MODIS aerosol data over highly reflecting desert dust sources is lacking. The broader implications of applying our approach are also discussed

The Dirac operator on untrapped surfaces

We establish a sharp extrinsic lower bound for the first eigenvalue of the Dirac operator of an untrapped surface in initial data sets without apparent horizon in terms of the norm of its mean curvature vector. The equality case leads to rigidity results for the constraint equations with spherical boundary as well as uniqueness results for constant mean curvature surfaces in Minkowski space.Comment: 16 page

Changes in the aerosol direct radiative forcing from 2001 to 2015: observational constraints and regional mechanisms

We present estimates of changes in the direct aerosol effects (DRE) and its anthropogenic component (DRF) from 2001 to 2015 using the GFDL chemistry–climate model AM3 driven by CMIP6 historical emissions. AM3 is evaluated against observed changes in the clear-sky shortwave direct aerosol effect (DREswclr) derived from the Clouds and the Earth's Radiant Energy System (CERES) over polluted regions. From 2001 to 2015, observations suggest that DREclrsw increases (i.e., less radiation is scattered to space by aerosols) over western Europe (0.7–1&thinsp;W&thinsp;m−2&thinsp;decade−1) and the eastern US (0.9–1.4&thinsp;W&thinsp;m−2&thinsp;decade−1), decreases over India (−1 to −1.6&thinsp;W&thinsp;m−2&thinsp;decade−1), and does not change significantly over eastern China. AM3 captures these observed regional changes in DREclrsw well in the US and western Europe, where they are dominated by the decline of sulfate aerosols, but not in Asia, where the model overestimates the decrease of DREclrsw. Over India, the model bias can be partly attributed to a decrease of the dust optical depth, which is not captured by our model and offsets some of the increase of anthropogenic aerosols. Over China, we find that the decline of SO2 emissions after 2007 is not represented in the CMIP6 emission inventory. Accounting for this decline, using the Modular Emission Inventory for China, and for the heterogeneous oxidation of SO2 significantly reduces the model bias. For both India and China, our simulations indicate that nitrate and black carbon contribute more to changes in DREclrsw than in the US and Europe. Indeed, our model suggests that black carbon (+0.12&thinsp;W&thinsp;m−2) dominates the relatively weak change in DRF from 2001 to 2015 (+0.03&thinsp;W&thinsp;m−2). Over this period, the changes in the forcing from nitrate and sulfate are both small and of the same magnitude (−0.03&thinsp;W&thinsp;m−2 each). This is in sharp contrast to the forcing from 1850 to 2001 in which forcings by sulfate and black carbon largely cancel each other out, with minor contributions from nitrate. The differences between these time periods can be well understood from changes in emissions alone for black carbon but not for nitrate and sulfate; this reflects non-linear changes in the photochemical production of nitrate and sulfate associated with changes in both the magnitude and spatial distribution of anthropogenic emissions.</p

The effect of harmonized emissions on aerosol properties in global models – an AeroCom experiment

The effects of unified aerosol sources on global aerosol fields simulated by different models are examined in this paper. We compare results from two AeroCom experiments, one with different (ExpA) and one with unified emissions, injection heights, and particle sizes at the source (ExpB). Surprisingly, harmonization of aerosol sources has only a small impact on the simulated diversity for aerosol burden, and consequently optical properties, as the results are largely controlled by model-specific transport, removal, chemistry (leading to the formation of secondary aerosols) and parameterizations of aerosol microphysics (e.g. the split between deposition pathways) and to a lesser extent on the spatial and temporal distributions of the (precursor) emissions. The burdens of black carbon and especially sea salt become more coherent in ExpB only, because the large ExpA diversity for these two species was caused by few outliers. The experiment also indicated that despite prescribing emission fluxes and size distributions, ambiguities in the implementation in individual models can lead to substantial differences. These results indicate the need for a better understanding of aerosol life cycles at process level (including spatial dispersal and interaction with meteorological parameters) in order to obtain more reliable results from global aerosol simulations. This is particularly important as such model results are used to assess the consequences of specific air pollution abatement strategies