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A global modeling study on carbonaceous aerosol microphysical characteristics and radiative effects

Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, indirect and semi-direct aerosol effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative effects. Our best estimate for net direct and indirect aerosol radiative flux change between 1750 and 2000 is −0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative flux change can vary between −0.32 to −0.75 W/m2 depending on these carbonaceous particle properties at emission. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Absorption of black carbon aerosols is amplified by sulfate and nitrate coatings and, even more strongly, by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative fluxeswhen sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to a reduction in positive radiative flux.
Quantification of DMS aerosol-cloud-climate interactions using the ECHAM5-HAMMOZ model in a current climate scenario

The contribution of ocean dimethyl sulfide (DMS) emissions to changes in cloud microphysical properties is quantified seasonally and globally for present day climate conditions using an aerosol-chemistry-climate general circulation model, ECHAM5-HAMMOZ, coupled to a cloud microphysics scheme. We evaluate DMS aerosol-cloud-climate linkages over the southern oceans where anthropogenic influence is minimal. The changes in the number of activated particles, cloud droplet number concentration (CDNC), cloud droplet effective radius, cloud cover and the radiative forcing are examined by analyzing two simulations: a baseline simulation with ocean DMS emissions derived from a prescribed climatology and one in which the ocean DMS emissions are switched off. Our simulations show that the model realistically simulates the seasonality in the number of activated particles and CDNC, peaking during Southern Hemisphere (SH) summer coincident with increased phytoplankton blooms and gradually declining with a minimum in SH winter. In comparison to a simulation with no DMS, the CDNC level over the southern oceans is 128% larger in the baseline simulation averaged over the austral summer months. Our results also show an increased number of smaller sized cloud droplets during this period. We estimate a maximum decrease of up to 15–18% in the droplet radius and a mean increase in cloud cover by around 2.5% over the southern oceans during SH summer in the simulation with ocean DMS compared to when the DMS emissions are switched off. The global annual mean top of the atmosphere DMS aerosol all sky radiative forcing is −2.03 W/m2, whereas, over the southern oceans during SH summer, the mean DMS aerosol radiative forcing reaches −9.32 W/m2.
Hygroscopicity distribution concept for measurement data analysis and modeling of aerosol particle mixing state with regard to hygroscopic growth and CCN activation

This paper presents a general concept and mathematical framework of particle hygroscopicity distribution for the analysis and modeling of aerosol hygroscopic growth and cloud condensation nucleus (CCN) activity. The cumulative distribution function of particle hygroscopicity, H(κ, Dd) is defined as the number fraction of particles with a given dry diameter, Dd, and with an effective hygroscopicity parameter smaller than the parameter κ. From hygroscopicity tandem differential mobility analyzer (HTDMA) and size-resolved CCN measurement data, H(κ, Dd) can be derived by solving the κ-Köhler model equation. Alternatively, H(κ, Dd) can be predicted from measurement or model data resolving the chemical composition of single particles. A range of model scenarios are used to explain and illustrate the concept, and exemplary practical applications are shown with HTDMA and CCN measurement data from polluted megacity and pristine rainforest air. Lognormal distribution functions are found to be suitable for approximately describing the hygroscopicity distributions of the investigated atmospheric aerosol samples. For detailed characterization of aerosol hygroscopicity distributions, including externally mixed particles of low hygroscopicity such as freshly emitted soot, we suggest that size-resolved CCN measurements with a wide range and high resolution of water vapor supersaturation and dry particle diameter should be combined with comprehensive HTDMA measurements and size-resolved or single-particle measurements of aerosol chemical composition, including refractory components. In field and laboratory experiments, hygroscopicity distribution data from HTDMA and CCN measurements can complement mixing state information from optical, chemical and volatility-based techniques. Moreover, we propose and intend to use hygroscopicity distribution functions in model studies investigating the influence of aerosol mixing state on the formation of cloud droplets.
Measured black carbon deposition on the Sierra Nevada snow pack and implication for snow pack retreat

Modeling studies show that the darkening of snow and ice by black carbon deposition is a major factor for the rapid disappearance of arctic sea ice, mountain glaciers and snow packs. This study provides one of the first direct measurements for the efficient removal of black carbon from the atmosphere by snow and its subsequent deposition to the snow packs of California. The early melting of the snow packs in the Sierras is one of the contributing factors to the severe water problems in California. BC concentrations in falling snow were measured at two mountain locations and in rain at a coastal site. All three stations reveal large BC concentrations in precipitation, ranging from 1.7 ng/g to 12.9 ng/g. The BC concentrations in the air after the snow fall were negligible suggesting an extremely efficient removal of BC by snow. The data suggest that below cloud scavenging, rather than ice nuclei, was the dominant source of BC in the snow. A five-year comparison of BC, dust, and total fine aerosol mass concentrations at multiple sites reveals that the measurements made at the sampling sites were representative of large scale deposition in the Sierra Nevada. The relative concentration of iron and calcium in the mountain aerosol indicates that one-quarter to one-third of the BC may have been transported from Asia.
A meridional structure of static stability and ozone vertical gradient around the tropopause in the Southern Hemisphere extratropics

An analysis of the static stability and ozone vertical gradient in the ozone tropopause based (OTB) coordinate is applied to the ozonesonde data at 10 stations in the Southern Hemisphere (SH) extratropics. The tropopause inversion layer (TIL) with a static stability maximum just above the tropopause shows similar seasonal variations at two Antarctic stations, which are latitudinally far from each other. Since the sunshine hour varies with time in a quite different way between these two stations, it implies that the radiative heating due to solar ultraviolet absorption of ozone does not contribute to the seasonal variation of the TIL. A meridional section of the static stability in the OTB coordinate shows that the static stability just above the tropopause has a large latitudinal gradient between 60° S and 70° S in austral winter because of the absence of the TIL over the Antarctic. It is accompanied by an increase of westerly shear with height above the tropopause, so that the polar-night jet is formed above this latitude region. This result suggests a close relationship between the absence of the TIL and the stratospheric polar vortex in the Antarctic winter. A vertical gradient of ozone mixing ratio, referred to as ozone vertical gradient, around the tropopause shows similar latitudinal and seasonal variations with the static stability in the SH extratropics. In a height region above the TIL, a small ozone vertical gradient in the midlatitudes associated with the Antarctic ozone hole is observed in a height region of the subvortex but not around the polar vortex. This is a clear evidence of active latitudinal mixing between the midlatitudes and subvortex.
Atmospheric Brown Clouds in the Himalayas: first two years of continuous observations at the Nepal Climate Observatory-Pyramid (5079 m)

This paper provides a detailed description of the atmospheric conditions characterizing the high Himalayas, thanks to continuous observations begun in March 2006 at the Nepal Climate Observatory-Pyramid (NCO-P) located at 5079 m a.s.l. on the southern foothills of Mt. Everest, in the framework of ABC-UNEP and SHARE-Ev-K2-CNR projects. The work presents a characterization of meteorological conditions and air-mass circulation at NCO-P during the first two years of activity. The mean values of atmospheric pressure, temperature and wind speed recorded at the site were: 551 hPa, −3.0 °C, 4.7 m s−1, respectively. The highest seasonal values of temperature (1.7 °C) and relative humidity (94%) were registered during the monsoon season, which was also characterized by thick clouds, present in about 80% of the afternoon hours, and by a frequency of cloud-free sky of less than 10%. The lowest temperature and relative humidity seasonal values were registered during winter, −6.3 °C and 22%, respectively, the season being characterised by mainly cloud-free sky conditions and rare thick clouds. The summer monsoon influenced rain precipitation (seasonal mean: 237 mm), while wind was dominated by flows from the bottom of the valley (S–SW) and upper mountain (N–NE). The atmospheric composition at NCO-P has been studied thanks to measurements of black carbon (BC), aerosol scattering coefficient, PM1, coarse particles and ozone. The annual behaviour of the measured parameters shows the highest seasonal values during the pre-monsoon (BC: 316.9 ng m−3, PM1: 3.9 μg m−3, scattering coefficient: 11.9 Mm−1, coarse particles: 0.37 cm−3 and O3: 60.9 ppbv), while the lowest concentrations occurred during the monsoon (BC: 49.6 ng m−3, PM1: 0.6 μg m−3, scattering coefficient: 2.2 Mm−1, and O3: 38.9 ppbv) and, for coarse particles, during the post-monsoon (0.07 cm−3. At NCO-P, the synoptic-scale circulation regimes present three principal contributions: Westerly, South-Westerly and Regional, as shown by the analysis of in-situ meteorological parameters and 5-day LAGRANTO back-trajectories. The influence of the brown cloud (AOD>0.4) extending over Indo–Gangetic Plains up to the Himalayan foothills has been evaluated by analysing the in-situ concentrations of the ABC constituents. This analysis revealed that brown cloud hot spots mainly influence the South Himalayas during the pre-monsoon, in the presence of very high levels of atmospheric compounds (BC: 1974.1 ng m−3, PM1: 23.5 μg m−3, scattering coefficient: 57.7 Mm−1, coarse particles: 0.64 cm−3, O3: 69.2 ppbv, respectively). During this season 20% of the days were characterised by a strong brown cloud influence during the afternoon, leading to a 5-fold increased in the BC and PM1 values, in comparison with seasonal means. Our investigations provide clear evidence that, especially during the pre-monsoon, the southern side of the high Himalayan valleys represent a "direct channel" able to transport brown cloud pollutants up to 5000 m a.s.l., where the pristine atmospheric composition can be strongly influenced.
Chemical and aerosol characterisation of the troposphere over West Africa during the monsoon period as part of AMMA

During June, July and August 2006 five aircraft took part in a campaign over West Africa to observe the aerosol content and chemical composition of the troposphere and lower stratosphere as part of the African Monsoon Multidisciplinary Analysis (AMMA) project. These are the first such measurements in this region during the monsoon period. In addition to providing an overview of the tropospheric composition, this paper provides a description of the measurement strategy (flights performed, instrumental payloads, wing-tip to wing-tip comparisons) and points to some of the important findings discussed in more detail in other papers in this special issue. The ozone data exhibits an "S" shaped vertical profile which appears to result from significant losses in the lower troposphere due to rapid deposition to forested areas and photochemical destruction in the moist monsoon air, and convective uplift of ozone-poor air to the upper troposphere. This profile is disturbed, particularly in the south of the region, by the intrusions in the lower and middle troposphere of air from the southern hemisphere impacted by biomass burning. Comparisons with longer term data sets suggest the impact of these intrusions on West Africa in 2006 was greater than in other recent wet seasons. There is evidence for net photochemical production of ozone in these biomass burning plumes as well as in urban plumes, in particular that from Lagos, convective outflow in the upper troposphere and in boundary layer air affected by nitrogen oxide emissions from recently wetted soils. This latter effect, along with enhanced deposition to the forested areas, contributes to a latitudinal gradient of ozone in the lower troposphere. Biogenic volatile organic compounds are also important in defining the composition both for the boundary layer and upper tropospheric convective outflow. Mineral dust was found to be the most abundant and ubiquitous aerosol type in the atmosphere over Western Africa. Data collected within AMMA indicate that injection of dust to altitudes favourable for long-range transport (i.e. in the upper Sahelian planetary boundary layer) can occur behind the leading edge of mesoscale convective system (MCS) cold-pools. Research within AMMA also provides the first estimates of secondary organic aerosols across the West African Sahel and have shown that organic mass loadings vary between 0 and 2 μg m−3 with a median concentration of 1.07 μg m−3. The vertical distribution of nucleation mode particle concentrations reveals that significant and fairly strong particle formation events did occur for a considerable fraction of measurement time above 8 km (and only there). Very low concentrations were observed in general in the fresh outflow of active MCSs, likely as the result of efficient wet removal of aerosol particles due to heavy precipitation inside the convective cells of the MCSs. This wet removal initially affects all particle size ranges as clearly shown by all measurements in the vicinity of MCSs.
High variability of the heterogeneous ice nucleation potential of oxalic acid dihydrate and sodium oxalate

The heterogeneous ice nucleation potential of airborne oxalic acid dihydrate and sodium oxalate particles in the deposition and condensation mode has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 244 and 228 K. Previous laboratory studies have highlighted the particular role of oxalic acid dihydrate as the only species amongst a variety of other investigated dicarboxylic acids to be capable of acting as a heterogeneous ice nucleus in both the deposition and immersion mode. We could confirm a high deposition mode ice activity for 0.03 to 0.8 μm sized oxalic acid dihydrate particles that were either formed by nucleation from a gaseous oxalic acid/air mixture or by rapid crystallisation of highly supersaturated aqueous oxalic acid solution droplets. The critical saturation ratio with respect to ice required for deposition nucleation was found to be less than 1.1 and the size-dependent ice-active fraction of the aerosol population was in the range from 0.1 to 22%. In contrast, oxalic acid dihydrate particles that had crystallised from less supersaturated solution droplets and had been allowed to slowly grow in a supersaturated environment from still unfrozen oxalic acid solution droplets over a time period of several hours were found to be much poorer heterogeneous ice nuclei. We speculate that under these conditions a crystal surface structure with less-active sites for the initiation of ice nucleation was generated. Such particles partially proved to be almost ice-inactive in both the deposition and condensation mode. At times, the heterogeneous ice nucleation ability of oxalic acid dihydrate significantly changed when the particles had been processed in preceding cloud droplet activation steps. Such behaviour was also observed for the second investigated species, namely sodium oxalate. Our experiments address the atmospheric scenario that coating layers of oxalic acid or its salts may be formed by physical and chemical processing on pre-existing particulates such as mineral dust and soot. Given the broad diversity of the observed heterogeneous ice nucleability of the oxalate species, it is not straightforward to predict whether an oxalate coating layer will improve or reduce the ice nucleation ability of the seed aerosol particles.
Low sensitivity of cloud condensation nuclei to changes in the sea-air flux of dimethyl-sulphide

The emission of dimethyl-sulphide (DMS) gas by phytoplankton and the subsequent formation of aerosol has long been suggested as an important climate regulation mechanism. The key aerosol quantity is the number concentration of cloud condensation nuclei (CCN), but until recently global models did not include the necessary aerosol physics to quantify CCN. Here we use a global aerosol microphysics model to calculate the sensitivity of CCN to changes in DMS emission using multiple present-day and future sea-surface DMS climatologies. Calculated annual fluxes of DMS to the atmosphere for the five model-derived and one observations based present day climatologies are in the range 15.1 to 32.3 Tg a−1 sulphur. The impact of DMS climatology on surface level CCN concentrations was calculated in terms of summer and winter hemispheric mean values of ΔCCN/ΔFluxDMS, which varied between −43 and +166 cm−3/(mg m−2 day−1 sulphur), with a mean of 63 cm−3/(mg m−2 day−1 sulphur). The range is due to CCN production in the atmosphere being strongly dependent on the spatial distribution of the emitted DMS. The relative sensitivity of CCN to DMS (i.e. fractional change in CCN divided by fractional change in DMS flux) depends on the abundance of non-DMS derived aerosol in each hemisphere. The relative sensitivity averaged over the five present day DMS climatologies is estimated to be 0.02 in the northern hemisphere (i.e. a 0.02% change in CCN for a 1% change in DMS) and 0.07 in the southern hemisphere where aerosol abundance is lower. In a globally warmed scenario in which the DMS flux increases by ~1% relative to present day we estimate a ~0.1% increase in global mean CCN at the surface. The largest CCN response occurs in the Southern Ocean, contributing to a Southern Hemisphere mean annual increase of less than 0.2%. We show that the changes in DMS flux and CCN concentration between the present day and global warming scenario are similar to interannual differences due to variability in windspeed. In summary, although DMS makes a significant contribution to global marine CCN concentrations, the sensitivity of CCN to potential future changes in DMS flux is very low. This finding, together with the predicted small changes in future seawater DMS concentrations, suggests that the role of DMS in climate regulation is very weak.
Heterogeneous chemistry of monocarboxylic acids on α-Al2O3 at different relative humidities

A study of the atmospheric heterogeneous reactions of formic acid, acetic acid, and propionic acid on α-Al2O3 was performed at ambient condition by using a diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) reactor. From the analysis of the spectral features, observations of carboxylates formation provide strong evidence for an efficient reactive uptake process. Comparison of the calculated and experimental vibrational frequencies of adsorbed carboxylates establishes the bridging coordinated structures on the surface. The uptake coefficients of formic acid, acetic acid, and propionic acid on α-Al2O3 particles are (2.07±0.26)×10−3 or (2.37±0.30) ×10−7, (5.00±0.69)×10−3 or (5.99±0.78)×10−7, and (3.04±0.63)×10−3 or (3.03±0.52)×10−7, respectively (using geometric or BET surface area). Furthermore, the effect of varying relative humidity (RH) on these heterogeneous reactions was studied. The uptake coefficients of monocarboxylic acids on α-Al2O3 particles increase initially (RH<20%) and then decrease with the increased RH (RH>20%) which was due to the effect of water on carboxylic acid solvation, particle surface hydroxylation, and competition for reactive sites. On the basis of the results of experimental simulation, the mechanism of heterogeneous reaction of α-Al2O3 with carboxylic acids at ambient RH was discussed. The loss of atmospheric monocarboxylic acids due to reactive uptake on available mineral dust particles may be competitive with homogeneous loss pathways, especially in dusty urban and desertified environments.