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At least 145 records · Page 8

Role of Climate Change in Global Predictions of Future Tropospheric Ozone and Aerosols

A unified tropospheric chemistry-aerosol model within the Goddard Institute for Space Studies general circulation model II is applied to simulate an equilibrium CO2-forced climate in the year 2100 to examine the effects of climate change on global distributions of tropospheric ozone and sulfate, nitrate, ammonium, black carbon, primary organic carbon, secondary organic carbon, sea salt, and mineral dust aerosols. The year 2100 CO2 concentration as well as the anthropogenic emissions of ozone precursors and aerosols/aerosol precursors are based on the Intergovernmental Panel on Climate Change Special Report on Emissions Scenarios (SRES) A2. Year 2100 global O3 and aerosol burdens predicted with changes in both climate and emissions are generally 5-20% lower than those simulated with changes in emissions alone; as exceptions, the nitrate burden is 38% lower, and the secondary organic aerosol burden is 17% higher. Although the CO2-driven climate change alone is predicted to reduce the global O3 concentrations over or near populated and biomass burning areas because of slower transport, enhanced biogenic hydrocarbon emissions, decomposition of peroxyacetyl nitrate at higher temperatures, and the increase of O3 production by increased water vapor at high NOx levels. The warmer climate influences aerosol burdens by increasing aerosol wet deposition, altering climate-sensitive emissions, and shifting aerosol thermodynamic equilibrium. Climate change affects the estimates of the year 2100 direct radiative forcing as a result of the climate-induced changes in burdens and different climatological conditions; with full gas-aerosol coupling and accounting for ozone and direct radiative forcings by the O2, sulfate, nitrate, black carbon, and organic carbon are predicted to be +0.93, -0.72, -1.0, +1.26, and -0.56 W m(exp -2), respectively, using present-day climate and year 2100 emissions, while they are predicted to be +0.76, -0.72, 0.74, +0.97, and -0.58 W m(exp -2), respectively, with year 2100 climate and emissions.

Liao, Hong↗

Aerosol Absorption and Radiative Forcing

We present a comprehensive examination of aerosol absorption with a focus on evaluating the sensitivity of the global distribution of aerosol absorption to key uncertainties in the process representation. For this purpose we extended the comprehensive aerosol-climate model ECHAM5-HAM by effective medium approximations for the calculation of aerosol effective refractive indices, updated black carbon refractive indices, new cloud radiative properties considering the effect of aerosol inclusions, as well as by modules for the calculation of long-wave aerosol radiative properties and instantaneous aerosol forcing. The evaluation of the simulated aerosol absorption optical depth with the AERONET sun-photometer network shows a good agreement in the large scale global patterns. On a regional basis it becomes evident that the update of the BC refractive indices to Bond and Bergstrom (2006) significantly improves the previous underestimation of the aerosol absorption optical depth. In the global annual-mean, absorption acts to reduce the shortwave anthropogenic aerosol top-of-atmosphere (TOA) radiative forcing clear-sky from -0.79 to -0.53 W m(sup -2) (33%) and all-sky from -0.47 to -0.13W m(sup -2 (72%). Our results confirm that basic assumptions about the BC refractive index play a key role for aerosol absorption and radiative forcing. The effect of the usage of more accurate effective medium approximations is comparably small. We demonstrate that the diversity in the AeroCom land-surface albedo fields contributes to the uncertainty in the simulated anthropogenic aerosol radiative forcings: the usage of an upper versus lower bound of the AeroCom land albedos introduces a global annual-mean TOA forcing range of 0.19W m(sup -2) (36%) clear-sky and of 0.12W m(sup -2) (92%) all-sky. The consideration of black carbon inclusions on cloud radiative properties results in a small global annual-mean all-sky absorption of 0.05W m(sup -2) and a positive TOA forcing perturbation of 0.02W m(sup -2). The long-wave aerosol radiative effects are small for anthropogenic aerosols but become of relevance for the larger natural dust and sea-salt aerosols.

Stier, Philip↗

Maritime Aerosol Network (MAN) as a Component of AERONET

The World Ocean produces a large amount of natural aerosols that have all impact on the Earth's albedo and climate. Sea-salt is the major contributor to aerosol optical depth over the oceans. [Mahowald et al. 2006; Chin et al. 2002; Satheesh et al. 1999; Winter and Chylek, 1997] and therefore affects the radiative balance over the ocean through the direct [Haywood et al. 1999] and indirect aerosol effect [O'Dowd et al. 1999]. Aerosols over the oceans (produced marine and advected from land sources) are important for various atmospheric processes [Lewis and Schwartz, 2004] and remote sensing studies [Gordon, 1997].

Smirnov, A.↗

Simulations of the Aerosol Index and the Absorption Aerosol Optical Depth and Comparisons with OMI Retrievals During ARCTAS-2008 Campaign

We have computed the Aerosol Index (AI) at 354 nm, useful for observing the presence of absorbing aerosols in the atmosphere, from aerosol simulations conducted with the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) module running online the GEOS-5 Atmospheric GCM. The model simulates five aerosol types: dust, sea salt, black carbon, organic carbon and sulfate aerosol and can be run in replay or data assimilation modes. In the assimilation mode, information's provided by the space-based MODIS and MISR sensors constrains the model aerosol state. Aerosol optical properties are then derived from the simulated mass concentration and the Al is determined at the OMI footprint using the radiative transfer code VLIDORT. In parallel, model derived Absorption Aerosol Optical Depth (AAOD) is compared with OMI retrievals. We have focused our study during ARCTAS (June - July 2008), a period with a good sampling of dust and biomass burning events. Our ultimate goal is to use OMI measurements as independent validation for our MODIS/MISR assimilation. Towards this goal we document the limitation of OMI aerosol absorption measurements on a global scale, in particular sensitivity to aerosol vertical profile and cloud contamination effects, deriving the appropriate averaging kernels. More specifically, model simulated (full) column integrated AAOD is compared with model derived Al, this way identifying those regions and conditions under which OMI cannot detect absorbing aerosols. Making use of ATrain cloud measurements from MODIS, C1oudSat and CALIPSO we also investigate the global impact on clouds on OMI derived Al, and the extent to which GEOS-5 clouds can offer a first order representation of these effects.

Source record↗

Simulations of Aerosol Microphysics in the NASA GEOS-5 Model

Aerosol-cloud-chemistry interactions have potentially large but uncertain impacts on Earth's climate. One path to addressing these uncertainties is to construct models that incorporate various components of the Earth system and to test these models against data. To that end, we have previously incorporated the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) module online in the NASA Goddard Earth Observing System model (GEOS-5). GEOS-5 provides a platform for Earth system modeling, incorporating atmospheric and ocean general circulation models, a land surface model, a data assimilation system, and treatments of atmospheric chemistry and hydrologic cycle. Including GOCART online in this framework has provided a path for interactive aerosol-climate studies; however, GOCART only tracks the mass of aerosols as external mixtures and does not include the detailed treatments of aerosol size distribution and composition (internal mixtures) needed for aerosol-cloud-chemistry-climate studies. To address that need we have incorporated the Community Aerosol and Radiation Model for Atmospheres (CARMA) online in GEOS-5. CARMA is a sectional aerosol-cloud microphysical model, capable of treating both aerosol size and composition explicitly be resolving the aerosol distribution into a variable number of size and composition groupings. Here we present first simulations of dust, sea salt, and smoke aerosols in GEOS-5 as treated by CARMA. These simulations are compared to available aerosol satellite, ground, and aircraft data and as well compared to the simulated distributions in our current GOCART based system.

Colarco, Peter↗

New Aerosol Models for the Retrieval of Aerosol Optical Thickness and Normalized Water-Leaving Radiances from the SeaWiFS and MODIS Sensors Over Coastal Regions and Open Oceans

We describe the development of a new suite of aerosol models for the retrieval of atmospheric and oceanic optical properties from the SeaWiFs and MODIS sensors, including aerosol optical thickness (tau), angstrom coefficient (alpha), and water-leaving radiance (L(sub w)). The new aerosol models are derived from Aerosol Robotic Network (AERONET) observations and have bimodal lognormal distributions that are narrower than previous models used by the Ocean Biology Processing Group. We analyzed AERONET data over open ocean and coastal regions and found that the seasonal variability in the modal radii, particularly in the coastal region, was related to the relative humidity, These findings were incorporated into the models by making the modal radii, as well as the refractive indices, explicitly dependent on relative humidity, From those findings, we constructed a new suite of aerosol models. We considered eight relative humidity values (30%, 50%, 70%, 75%, 80%, 85%, 90%. and 95%) and, for each relative humidity value, we constructed ten distributions by varying the fine-mode fraction from zero to 1. In all. 80 distributions (8Rh x 10 fine-mode fractions) were created to process the satellite data. We. also assumed that the coarse-mode particles were nonabsorbing (sea salt) and that all observed absorptions were entirely due to fine-mode particles. The composition of fine mode was varied to ensure that the new models exhibited the same spectral dependence of single scattering albedo as observed in the AERONET data,

Ahmad, Ziauddin↗

Aerosol Observability and Predictability: From Research to Operations for Chemical Weather Forecasting. Lagrangian Displacement Ensembles for Aerosol Data Assimilation

A challenge common to many constituent data assimilation applications is the fact that one observes a much smaller fraction of the phase space that one wishes to estimate. For example, remotely sensed estimates of the column average concentrations are available, while one is faced with the problem of estimating 3D concentrations for initializing a prognostic model. This problem is exacerbated in the case of aerosols because the observable Aerosol Optical Depth (AOD) is not only a column integrated quantity, but it also sums over a large number of species (dust, sea-salt, carbonaceous and sulfate aerosols. An aerosol transport model when driven by high-resolution, state-of-the-art analysis of meteorological fields and realistic emissions can produce skillful forecasts even when no aerosol data is assimilated. The main task of aerosol data assimilation is to address the bias arising from inaccurate emissions, and Lagrangian misplacement of plumes induced by errors in the driving meteorological fields. As long as one decouples the meteorological and aerosol assimilation as we do here, the classic baroclinic growth of error is no longer the main order of business. We will describe an aerosol data assimilation scheme in which the analysis update step is conducted in observation space, using an adaptive maximum-likelihood scheme for estimating background errors in AOD space. This scheme includes e explicit sequential bias estimation as in Dee and da Silva. Unlikely existing aerosol data assimilation schemes we do not obtain analysis increments of the 3D concentrations by scaling the background profiles. Instead we explore the Lagrangian characteristics of the problem for generating local displacement ensembles. These high-resolution state-dependent ensembles are then used to parameterize the background errors and generate 3D aerosol increments. The algorithm has computational complexity running at a resolution of 1/4 degree, globally. We will present the result of assimilating AOD retrievals from MODIS (on both Aqua and TERRA satellites) from AERONET for validation. The impact on the GEOS-5 Aerosol Forecasting will be fully documented.

da Silva, Arlindo↗

Reducing the Uncertainties in Direct Aerosol Radiative Forcing

Airborne particles, which include desert and soil dust, wildfire smoke, sea salt, volcanic ash, black carbon, natural and anthropogenic sulfate, nitrate, and organic aerosol, affect Earth's climate, in part by reflecting and absorbing sunlight. This paper reviews current status, and evaluates future prospects for reducing the uncertainty aerosols contribute to the energy budget of Earth, which at present represents a leading factor limiting the quality of climate predictions. Information from satellites is critical for this work, because they provide frequent, global coverage of the diverse and variable atmospheric aerosol load. Both aerosol amount and type must be determined. Satellites are very close to measuring aerosol amount at the level-of-accuracy needed, but aerosol type, especially how bright the airborne particles are, cannot be constrained adequately by current techniques. However, satellite instruments can map out aerosol air mass type, which is a qualitative classification rather than a quantitative measurement, and targeted suborbital measurements can provide the required particle property detail. So combining satellite and suborbital measurements, and then using this combination to constrain climate models, will produce a major advance in climate prediction.

Kahn, Ralph A.↗

Parameterization of Aerosol Sinks in Chemical Transport Models

The modelers point of view is that the aerosol problem is one of sources, evolution, and sinks. Relative to evolution and sink processes, enormous attention is given to the problem of aerosols sources, whether inventory based (e.g., fossil fuel emissions) or dynamic (e.g., dust, sea salt, biomass burning). On the other hand, aerosol losses in models are a major factor in controlling the aerosol distribution and lifetime. Here we shine some light on how aerosol sinks are treated in modern chemical transport models. We discuss the mechanisms of dry and wet loss processes and the parameterizations for those processes in a single model (GEOS-5). We survey the literature of other modeling studies. We additionally compare the budgets of aerosol losses in several of the ICAP models.

Colarco, Peter↗

El Nino-Southern Oscillation Correlated Aerosol Angstrom Exponent Anomaly Over the Tropical Pacific Discovered in Satellite Measurements

El Nino.Southern Oscillation (ENSO) is the dominant mode of interannual variability in the tropical atmosphere. ENSO could potentially impact local and global aerosol properties through atmospheric circulation anomalies and teleconnections. By analyzing aerosol properties, including aerosol optical depth (AOD) and Angstrom exponent (AE; often used as a qualitative indicator of aerosol particle size) from the Moderate Resolution Imaging Spectrometer, the Multiangle Imaging Spectroradiometer and the Sea ]viewing Wide Field ]of ]view Sensor for the period 2000.2011, we find a strong correlation between the AE data and the multivariate ENSO index (MEI) over the tropical Pacific. Over the western tropical Pacific (WTP), AE increases during El Nino events and decreases during La Nina events, while the opposite is true over the eastern tropical Pacific (ETP). The difference between AE anomalies in the WTP and ETP has a higher correlation coefficient (>0.7) with the MEI than the individual time series and could be considered another type of ENSO index. As no significant ENSO correlation is found in AOD over the same region, the change in AE (and hence aerosol size) is likely to be associated with aerosol composition changes due to anomalous meteorological conditions induced by the ENSO. Several physical parameters or mechanisms that might be responsible for the correlation are discussed. Preliminary analysis indicates surface wind anomaly might be the major contributor, as it reduces sea ]salt production and aerosol transport during El Nino events. Precipitation and cloud fraction are also found to be correlated with tropical Pacific AE. Possible mechanisms, including wet removal and cloud shielding effects, are considered. Variations in relative humidity, tropospheric ozone concentration, and ocean color during El Nino have been ruled out. Further investigation is needed to fully understand this AE ]ENSO covariability and the underlying physical processes responsible for it.

Li, Jing↗

An Assessment of the Surface Longwave Direct Radiative Effect of Airborne Dust in Zhangye China During the Asian Monsoon Year Field Experiment (2008)

Tiny suspensions of solid particles or liquid droplets, called aerosols, hover in earth's atmosphere and can be found over just about anywhere including oceans, deserts, vegetated areas, and other global regions. Aerosols come in a variety of sizes, shapes, and compositions which depend on such factors as their origin and how long they have been in the atmosphere (i.e., their residence time). Some of the more common types of aerosols include mineral dust and sea salt which get lifted from the desert and ocean surfaces, respectively by mechanical forces such as strong winds. Depending on their size, aerosols will either fall out gravitationally, as in the case of larger particles, or will remain resident in the atmosphere where they can undergo further change through interactions with other aerosols and cloud particles. Not only do aerosols affect air quality where they pose a health risk, they can also perturb the distribution of radiation in the earth-atmosphere system which can inevitably lead to changes in our climate. One aerosol that has been in the forefront of many recent studies, particularly those examining its radiative effects, is mineral dust. The large spatial coverage of desert source regions and the fact that dust can radiatively interact with such a large part of the electromagnetic spectrum due to its range in particle size, makes it an important aerosol to study. Dust can directly scatter and absorb solar and infrared radiation which can subsequently alter the amount of radiation that would otherwise be present in the absence of dust at any level of the atmosphere like the surface. This is known as radiative forcing. At the surface dust can block incoming solar energy, however at infrared wavelengths, dust acts to partially compensate the solar losses. Evaluating the solar radiative effect of dust aerosols is relatively straightforward due in part to the relatively large signal-to-noise ratio in the measurements. At infrared wavelengths, on the other hand, the effect is rather difficult to ascertain since the measured dust signal level is on the same order as the instrumental uncertainties. Although the radiative impact of dust is much smaller in the infrared, it can still have a noticeable influence on the distribution of energy in the Earth-atmosphere system. This is mainly attributed to the strong light-absorptive properties commonly found in many earth minerals.

Hansell, Richard A.↗

Critical Reflectance Derived from MODIS: Application for the Retrieval of Aerosol Absorption over Desert Regions

Aerosols are tiny suspended particles in the atmosphere that scatter and absorb sunlight. Smoke particles are aerosols, as are sea salt, particulate pollution and airborne dust. When you look down at the earth from space sometimes you can see vast palls of whitish smoke or brownish dust being transported by winds. The reason that you can see these aerosols is because they are reflecting incoming sunlight back to the view in space. The reason for the difference in color between the different types of aerosol is that the particles arc also absorbing sunlight at different wavelengths. Dust appears brownish or reddish because it absorbs light in the blue wavelengths and scatters more reddish light to space, Knowing how much light is scattered versus how much is absorbed, and knowin~ that as a function of wavelength is essential to being able to quantify the role aerosols play in the energy balance of the earth and in climate change. It is not easy measuring the absorption properties of aerosols when they are suspended in the atmosphere. People have been doing this one substance at a time in the laboratory, but substances mix when they are in the atmosphere and the net absorption effect of all the particles in a column of air is a goal of remote sensing that has not yet been completely successful. In this paper we use a technique based on observing the point at which aerosols change from brightening the surface beneath to darkening it. If aerosols brighten a surface. they must scatter more light to space. If they darken the surface. they must be absorbing more. That cross over point is called the critical reflectance and in this paper we show that critical reflectance is a monotonic function of the intrinsic absorption properties of the particles. This parameter we call the single scattering albedo. We apply the technique to MODIS imagery over the Sahara and Sahel regions to retrieve the single scattering albedo in seven wavelengths, compare these retrievals to ground-based retrievals from AERONET instruments and compute error bars on each retrieval. The results show that we can retrieve single scattering albedo for pure dust to within +/-0.02 and mixtures of dust and smoke to within +/-0.03. No other space based instrument has achieved a retrieval of single scattering albedo that spans the spectrum from 0.47 microns to 2.13 microns and produces regional maps of aerosol absorption showing gradients and changes. Applied in a more operational fashion, such information will narrow uncertainties in estimating aerosol forcing on climate.

Wells, Kelley C.↗

Aerosol Remote Sensing from AERONET, the Ground-Based Satellite

Atmospheric particles including mineral dust, biomass burning smoke, pollution from carbonaceous aerosols and sulfates, sea salt, impact air quality and climate. The Aerosol Robotic Network (AERONET) program, established in the early 1990s, is a federation of ground-based remote sensing aerosol networks of Sun/sky radiometers distributed around the world, which provides a long-term, continuous and readily accessible public domain database of aerosol optical (e.g., aerosol optical depth) and microphysical (e.g., aerosol volume size distribution) properties for aerosol characterization, validation of satellite retrievals, and synergism with Earth science databases. Climatological aerosol properties will be presented at key worldwide locations exhibiting discrete dominant aerosol types. Further, AERONET's temporary mesoscale network campaign (e.g., UAE2, TIGERZ, DRAGON-USA.) results that attempt to quantify spatial and temporal variability of aerosol properties, establish validation of ground-based aerosol retrievals using aircraft profile measurements, and measure aerosol properties on compatible spatial scales with satellite retrievals and aerosol transport models allowing for more robust validation will be discussed.

Holben, Brent N.↗

The Use of Satellite-Measured Aerosol Optical Depth to Constrain Biomass Burning Emissions Source Strength in a Global Model GOCART

Small particles in the atmosphere, called "atmospheric aerosol" have a direct effect on Earth climate through scattering and absorbing sunlight, and also an indirect effect by changing the properties of clouds, as they interact with solar radiation as well. Aerosol typically stays in the atmosphere for several days, and can be transported long distances, affecting air quality, visibility, and human health not only near the source, but also far downwind. Smoke from vegetation fires is one of the main sources of atmospheric aerosol; other sources include anthropogenic pollution, dust, and sea salt. Chemistry transport models (CTMs) are among the major tools for studying the atmospheric and climate effects of aerosol. Due to the considerable variation of aerosol concentrations and properties on many temporal and spatial scales, and the complexity of the processes involved, the uncertainties in aerosol effects on climate are large, as is featured in the latest report of Intergovernmental Panel on Climate Change (IPCC) in 2007. Reducing this uncertainty in the models is very important both for predicting future climate scenarios and for regional air quality forecasting and mitigation. During vegetation fires, also called biomass burning (BB) events, complex mixture of gases and particles is emitted. The amount of BB emissions is usually estimated taking into account the intensity and size of the fire and the properties of burning vegetation. These estimates are input into CTMs to simulate BB aerosol. Unfortunately, due to large variability of fire and vegetation properties, the quantity of BB emissions is very difficult to estimate and BB emission inventories provide numbers that can differ by up to the order of magnitude in some regions. Larger uncertainties in data input make uncertainties in model output larger as well. A powerful way to narrow the range of possible model estimates is to compare model output to observations. We use satellite observations of aerosol properties, specifically aerosol optical depth, which is directly proportional to the amount of aerosol in the atmosphere, and compare it to the model output. Assuming the model represents aerosol transport and particle properties correctly, the amount of BB emissions determines the simulated aerosol optical depth. In this study, we explore the regional performance of 13 commonly used emission estimates. These are each input to global Goddard Chemistry Aerosol Radiation and Transport (GOCART) model. We then evaluate how well each emission estimate reproduces the smoke aerosol optical depth measured by the MODIS instrument. We compared GOCART-simulate aerosol optical depth with that measured from the satellite for 124 fire cases around the world during 2006 and 2007. We summarize the regional performance of each emission inventory and discuss reasons for their differences by considering the assumptions made during their development. We also show that because stronger wind disperses smoke plumes more readily, in cases with stronger wind, a larger increase in emission amount is needed to increase aerosol optical depth. In quiet, low-wind-speed environments, BB emissions produce a more significant increase in aerosol optical depth, other things being equal. Using the region-specific, quantitative relationships derived in our paper, together with the wind speed obtained from another source for a given fire case, we can constrain the amount of emission required in the model to reproduce the observations. The results of this paper are useful to the developers of BB emission inventories, as they show the strengths and weaknesses of individual emission inventories in different regions of the globe, and also for modelers who use these inventories and wish to improve their model results.

Petrenko, Mariya↗

Dirtier Air from a Weaker Monsoon

The level of air pollution in China has much increased in the past decades, causing serious health problems. Among the main pollutants are aerosols, also known as particulate matter: tiny, invisible particles that are suspended in the air. These particles contribute substantially to premature mortality associated with cardiopulmonary diseases and lung cancer1. The increase of the aerosol level in China has been commonly attributed to the fast rise in pollutant emissions from the rapid economic development in the region. However, writing in Geophysical Research Letters, Jianlei Zhu and colleagues2 tell a different side of the story: using a chemical transport model and observation data, they show that the decadal scale weakening of the East Asian summer monsoon has also contributed to the increase of aerosol concentrations in China. The life cycle of atmospheric aerosols starts with its emission or formation in the atmosphere. Some aerosol components such as dust, soot and sea salt are emitted directly as particles to the atmosphere, but others are formed there by way of photochemical reactions. For example, sulphate and nitrate aerosols are produced from their respective precursor gases, sulphur dioxide and nitrogen oxides. Aerosol particles can be transported away from their source locations by winds or vertical motion of the air. Eventually, they are removed from the atmosphere by means of dry deposition and wet scavenging by precipitation. Measurements generally show that aerosol concentrations over Asia are lowest during the summer monsoon season3, because intense rainfall efficiently removes them from the air. The East Asian summer monsoon extends over subtropics and mid-latitudes. Its rainfall tends to concentrate in rain belts that stretch out for many thousands of kilometres and affect China, Korea, Japan and the surrounding area. Observations suggest that the East Asian summer monsoon circulation and precipitation have been in decline since the 1970s4. In particular, a weaker East Asian summer monsoon is characterized by weaker southerly or southwesterly winds, a deficit in rainfall over northern China and larger rainfalls in southern China. By contrast, when the East Asian summer monsoon is strong, the southerly winds and strong rainfalls extend to northern China. The decadal scale decline in the strength of the East Asian summer monsoon since the 1970s would imply an increase in aerosol concentrations in northern China, north of 28deg N, and a decrease in southern China if emissions were kept the same. One obvious reason for this direction of aerosol change is that the reduction of monsoon rainfall in northern China would cause less wet scavenging of aerosols by precipitation. Zhu et al.2 investigated this relationship between aerosol concentrations and the strength of the East Asian summer monsoon and showed that the two parameters have strong negative correlations: the summer aerosol concentrations near the surface over eastern China.

Chin, Mian↗

Tropospheric Bromine Chemistry: Implications for Present and Pre-industrial Ozone and Mercury

We present a new model for the global tropospheric chemistry of inorganic bromine (Bry) coupled to oxidant-aerosol chemistry in the GEOS-Chem chemical transport model (CTM). Sources of tropospheric Bry include debromination of sea-salt aerosol, photolysis and oxidation of short-lived bromocarbons, and transport from the stratosphere. Comparison to a GOME-2 satellite climatology of tropospheric BrO columns shows that the model can reproduce the observed increase of BrO with latitude, the northern mid-latitudes maximum in winter, and the Arctic maximum in spring. This successful simulation is contingent on the HOBr + HBr reaction taking place in aqueous aerosols and ice clouds. Bromine chemistry in the model decreases tropospheric ozone mixing ratios by <1-8 nmol/mol (6.5% globally), with the largest effects in the northern extratropics in spring. The global mean tropospheric OH concentration decreases by 4 %. Inclusion of bromine chemistry improves the ability of global models (GEOS-Chem and p-TOMCAT) to simulate observed 19th-century ozone and its seasonality. Bromine effects on tropospheric ozone are comparable in the present-day and pre-industrial atmospheres so that estimates of anthropogenic radiative forcing are minimally affected. Br atom concentrations are 40% higher in the pre-industrial atmosphere due to lower ozone, which would decrease by a factor of 2 the atmospheric lifetime of elemental mercury against oxidation by Br. This suggests that historical anthropogenic mercury emissions may have mostly deposited to northern mid-latitudes, enriching the corresponding surface reservoirs. The persistent rise in background surface ozone at northern mid-latitudes during the past decades could possibly contribute to the observations of elevated mercury in subsurface waters of the North Atlantic.

bromine↗

A 4-D Climatology (1979-2009) of the Monthly Tropospheric Aerosol Optical Depth Distribution over the Mediterranean Region from a Comparative Evaluation and Blending of Remote Sensing and Model Products

Since the 1980s several spaceborne sensors have been used to retrieve the aerosol optical depth (AOD) over the Mediterranean region. In parallel, AOD climatologies coming from different numerical model simulations are now also available, permitting to distinguish the contribution of several aerosol types to the total AOD. In this work, we perform a comparative analysis of this unique multiyear database in terms of total AOD and of its apportionment by the five main aerosol types (soil dust, seasalt, sulfate, black and organic carbon). We use 9 different satellite-derived monthly AOD products: NOAA/AVHRR, SeaWiFS (2 products), TERRA/MISR, TERRA/MODIS, AQUA/MODIS, ENVISAT/MERIS, PARASOL/POLDER and MSG/SEVIRI, as well as 3 more historical datasets: NIMBUS7/CZCS, TOMS (onboard NIMBUS7 and Earth- Probe) and METEOSAT/MVIRI. Monthly model datasets include the aerosol climatology from Tegen et al. (1997), the climate-chemistry models LMDz-OR-INCA and RegCM-4, the multi-model mean coming from the ACCMIP exercise, and the reanalyses GEMS and MACC. Ground-based Level- 2 AERONET AOD observations from 47 stations around the basin are used here to evaluate the model and satellite data. The sensor MODIS (on AQUA and TERRA) has the best average AOD scores over this region, showing a relevant spatio-temporal variability and highlighting high dust loads over Northern Africa and the sea (spring and summer), and sulfate aerosols over continental Europe (summer). The comparison also shows limitations of certain datasets (especially MERIS and SeaWiFS standard products). Models reproduce the main patterns of the AOD variability over the basin. The MACC reanalysis is the closest to AERONET data, but appears to underestimate dust over Northern Africa, where RegCM-4 is found closer to MODIS thanks to its interactive scheme for dust emissions. The vertical dimension is also investigated using the CALIOP instrument. This study confirms differences of vertical distribution between dust aerosols showing a large vertical spread, and other continental and marine aerosols which are confined in the boundary layer. From this compilation, we propose a 4-D blended product from model and satellite data, consisting in monthly time series of 3-D aerosol distribution at a 50 km horizontal resolution over the Euro-Mediterranean marine and continental region for the 2003-2009 period. The product is based on the total AOD from AQUA/MODIS, apportioned into sulfates, black and organic carbon from the MACC reanalysis, and into dust and sea-salt aerosols from RegCM-4 simulations, which are distributed vertically based on CALIOP climatology.We extend the 2003-2009 reconstruction to the past up to 1979 using the 2003-2009 average and applying the decreasing trend in sulfate aerosols from LMDz-OR-INCA, whose AOD trends over Europe and the Mediterranean are median among the ACCMIP models. Finally optical properties of the different aerosol types in this region are proposed from Mie calculations so that this reconstruction can be included in regional climate models for aerosol radiative forcing and aerosol-climate studies.

troposphere↗

Impact of Radiatively Interactive Dust Aerosols in the NASA GEOS-5 Climate Model: Sensitivity to Dust Particle Shape and Refractive Index

We investigate the radiative effects of dust aerosols in the NASA GEOS-5 atmospheric general circulation model. GEOS-5 is improved with the inclusion of a sectional aerosol and cloud microphysics module, the Community Aerosol and Radiation Model for Atmospheres (CARMA). Into CARMA we introduce treatment of the dust and sea salt aerosol lifecycle, including sources, transport evolution, and sinks. The aerosols are radiatively coupled to GEOS-5, and we perform a series of multi-decade AMIP-style simulations in which dust optical properties (spectral refractive index and particle shape distribution) are varied. Optical properties assuming spherical dust particles are from Mie theory, while those for non-spherical shape distributions are drawn from a recently available database for tri-axial ellipsoids. The climatologies of the various simulations generally compare well to data from the MODIS, MISR, and CALIOP space-based sensors, the ground-based AERONET, and surface measurements of dust deposition and concentration. Focusing on the summertime Saharan dust cycle we show significant variability in our simulations resulting from different choices of dust optical properties. Atmospheric heating due to dust enhances surface winds over important Saharan dust sources, and we find a positive feedback where increased dust absorption leads to increased dust emissions. We further find that increased dust absorption leads to a strengthening of the summertime Hadley cell circulation, increasing dust lofting to higher altitudes and strengthening the African Easterly Jet. This leads to a longer atmospheric residence time, higher altitude, and generally more northward transport of dust in simulations with the most absorbing dust optical properties. We find that particle shape, although important for radiance simulations, is a minor effect compared to choices of refractive index, although total atmospheric forcing is enhanced by greater than 10 percent for simulations incorporating a spheroidal shape distribution versus ellipsoidal or spherical shapes.

radiative forcing↗