Why Is the Climate Forcing of Sulfate Aerosols So Uncertain?

Sulfate aerosol particles have strong scattering effect on the solar radiation transfer which results in increasing the planet albedo and, hence, tend to cool the earth-atmosphere system. Also, aerosols can act as the cloud condensation nuclei (CCN) which tend to increase the albedo of clouds and cool the global warming. The ARPEGE-Climat version 3 AGCM with FMR radiation scheme is used to estimate the direct and indirect radiative forcing of sulfate aerosols. For minimizing the uncertainties in assessing this kind of cooling effect, all kinds of factors are analyzed which have been mixed in the assessment process and may lead to the different results of the radiative forcing of aerosols. It is noticed that one of the uncertainties to assess the climate forcing of aerosols by GCM results from the different definition of radiative forcing that was used. In order to clarify this vague idea, the off-line case for considering no feedbacks and on-line case for including all the feedbacks have been used for assessment. The direct forcing of sulfate aerosols in off-line case is ?0.57 W/ m2 and ?0.38 W/ m2 for the clear sky and all sky respectively. The value of on-line case appears to be a little larger than that in off-line case chiefly due to the feedback of clouds. The indirect forcing of sulfate aerosols in off-line case is ?1.4 W/ m2 and ?1.0 W/ m2 in on-line case. The radiative forcing of sulfate aerosols has obvious regional characteristics. There is a larger negative radiative forcing over North America, Europe and East Asia. If the direct and indirect forcing are added together, it is enough to offset the positive radiative forcing induced by the greenhouse gases in these regions. Key words Radiative forcing - Feedback - Uncertainties - Sulfate aerosols

Variation of sulfate aerosol concentrations over the western Pacific and their effect on clouds, radiation and precipitation

Under bilateral cooperation between the United States of America and the People's Republic of China, a series of research cruises were conducted over the western Pacific Ocean. It was found that a) the non-sea-salt sulfate aerosol particles are the major source of cloud condensation nuclei, b) the population of clouds and the total albedo are proportional to the concentration of condensation nuclei and consequently to the concentration of the non-sea-salt aerosol particles, and c) the amount of rainfall is inversely proportional to the concentration of non-sea-salt sulfate aerosol particles. It seems that anthropogenic sulfate aerosol particles affect the regional planetary albedo and climate and that the contribution from biogenically derived sulfate aerosol particles is of lesser importance.

Geographic and temporal variations of sulfate aerosols over the Pacific Ocean

To investigate the life cycle of marine sulfate aerosols, chemicophysical characteristics of marine aerosolswere measured during five cruises in the Pacific Ocean. Dimethyl sulfide concentrations in seawater and in the air were also measured. The geographic variation of sulfate-aerosol concentrations was studied in relation to biogenic and anthropogenic sources,transport with air trajectories, and chemical transformations in the atmosphere. The highest concentrations were found near Asian and American ports, indicating anthropogenic pollution is the major sulfate aerosols source. Higher concentrations were observed in the upwelling regions than in the oligotrophic areas. Along the coastal regions, both mass and number concentrations of sulfate aerosols depended on wind direction and wind speed, and land-breeze and sea-breeze oscillations; no clear diurnal variation was detected. In pelagic areas, along the equator, the concentrations of small sulfate particles showed a maximum in the afternoon and the minimum at night , indicating photo-oxidation as an important process for gas-to-particle conversion. Higher sulfate-aerosol concentrations were observed in spring than in autumn and higher concentrations were found during the La Nina anomaly than during the El Nino anomaly. Biogenic source of sulfate aerosols has an important role in the remote ocean. Case studies of sulfate-aerosol distributions are discussed.

A critical review of sulfate aerosol formation mechanisms during winter polluted periods

Sulfate aerosol contributes to particulate matter pollution and plays a key role in aerosol radiative forcing,impacting human health and climate change.Atmospheric models tend to substantially underestimate sulfate concentrations during haze episodes,indicating that there are still missing mechanisms not considered by the models.Despite recent good progress in understanding the missing sulfate sources,knowledge on different sulfate formation pathways during polluted periods still involves large uncertainties and the dominant mechanism is under heated debate,calling for more field,laboratory,and modeling work.Here,we review the traditional sulfate formation mechanisms in cloud water and also discuss the potential factors affecting multiphase S(Ⅳ)oxidation.Then recent progress in multiphase S(Ⅳ)oxidation mechanisms is summarized.Sulfate formation rates by different prevailing oxidation pathways under typical winter-haze conditions are also calculated and compared.Based on the literature reviewed,we put forward control of the atmospheric oxidation capacity as a means to abate sulfate aerosol pollution.Finally,we conclude with a concise set of research priorities for improving our understanding of sulfate formation mechanisms during polluted periods.

Improving simulations of sulfate aerosols during winter haze over Northern China： the impacts of heterogeneous oxidation by NO2

We implemented the online coupled WRF-Chem model to reproduce the 2013 January haze event in North China, and evaluated simulated meteorological and chemical fields using multiple observations. The comparisons suggest that temperature and relative humidity （RH） were simulated well （mean biases are 0.2K and 2.7%, respectively）, but wind speeds were overestimated （mean bias is 0.5 m.s -1）. At the Beijing station, sulfur dioxide （SO2） concentrations were overpredicted and sulfhte concentrations were largely underpredicted, which may result from uncertainties in SO2 emissions and missing heterogeneous oxidation in current model. We conducted three parallel experiments to examine the impacts of doubling SO2 emissions and incorporating heterogeneous oxidation of dissolved SO2 by nitrogen dioxide （NO2） on sulfate formation during winter haze. The results suggest that doubling SO2 emissions do not significantly affect sulthte concentrations, but adding heterogeneous oxidation of dissolved SO2 by NO, substantially improve simulations of sulfate and other inorganic aerosols. Although the enhanced SO2 to sulfate conversion in the HetS （heterogeneous oxidation by NO2） case reduces SO2 concentrations, it is still largely overestimated by the model, indicating the overestimations of SO2 concentrations in the North China Plain （NCP） are mostly due to errors in SO2 emission inventory.

Characteristics of Anthropogenic Sulfate and Carbonaceous Aerosols over East Asia: Regional Modeling and Observation

The authors present spatial and temporal characteristics of anthropogenic sulfate and carbonaceous aerosols over East Asia using a 3-D coupled regional climate-chemistry-aerosol model, and compare the simulation with the limited aerosol observations over the region. The aerosol module consists of SO2, SO4^2-, hydrophobic and hydrophilic black carbon （BC） and organic carbon compounds （OC）, including emission, advections, dry and wet deposition, and chemical production and conversion. The simulated patterns of SO2 are closely tied to its emission rate, with sharp gradients between the highly polluted regions and more rural areas. Chemical conversion （especially in the aqueous phase） and dry deposition remove 60% and 30% of the total SO2 emission, respectively. The SO4^2- shows less horizontal gradient and seasonality than SO2, with wet deposition （60%） and export （27%） being two major sinks. Carbonaceous aerosols are spatially smoother than sulfur species. The aging process transforms more than 80% of hydrophobic BC and OC to hydrophilic components, which are removed by wet deposition （60%） and export （30%）. The simulated spatial and seasonal SO4^2-, BC and OC aerosol concentrations and total aerosol optical depth are generally consistent with the observations in rural areas over East Asia, with lower bias in simulated OC aerosols, likely due to the underestimation of anthropogenic OC emissions and missing treatment of secondary organic carbon. The results suggest that our model is a useful tool for characterizing the anthropogenic aerosol cycle and for assessing its potential climatic and environmental effects in future studies.

Seasonal and Spatial Variation of Radiative Effects of Anthropogenic Sulfate Aerosol

On the basis of the emission data of the industrial sulphur dioxide (SO_2) and observed climate fields over East Asia, the distribution of anthropogenic sulfate aerosol(SO_4~2-) with seasonal variation in the troposphere is simulated and analyzed by a regional sulfur transport model, and the direct radiative effects of SO_4~2- under different weather conditions are also calculated using the discrete ordinate method. The results show that the concentration of SO_4~2- has significant seasonal and spatial variations resulting from the effects of SO_2 emission source and precipitation and wind fields. Both the concentration of SO_2 and its radiative forcing have the largest values in October and the lowest in July. SO_4~2- causes the decrease of the radiation flux absorbed by earth-atmosphere and the cooling of air temperature by scattering more solar radiation back into space. Besides, the radiative and climatic effects of SO_4~2- are related to the types and height and optical thickness, etc., of the clouds.

THE DIRECT EFFECTS OF AEROSOLS AND DECADAL VARIATION OF GLOBAL SEA SURFACE TEMPERATURE ON THE EAST ASIAN SUMMER PRECIPITATION IN CAM3.0

Using the CAM3.0 model, we investigated the respective effects of aerosol concentration increasing and decadal variation of global sea surface temperature(SST) around year 1976/77 on the East Asian precipitation in boreal summer. By doubling the concentration of the sulfate aerosol and black carbon aerosol separately and synchronously in East Asia(100-150 °E, 20-50 °N), the climate effects of these aerosols are specifically investigated. The results show that both the decadal SST changing and aerosol concentration increasing could lead to rainfall decreasing in the center of East Asia, but increasing in the regions along southeast coast areas of China. However, the different patterns of rainfall over ocean and lower wind field over Asian continent between aerosol experiments and SST experiments in CAM3.0 indicate the presence of different mechanisms. In the increased aerosol concentration experiments, scattering effect is the main climate effect for both sulfate and black carbon aerosols in the Eastern Asian summer. Especially in the increased sulfate aerosol concentration experiment, the climate scattering effect of aerosol leads to the most significant temperature decreasing, sinking convection anomalies and decreased rainfall in the troposphere over the central part of East Asia. However, in an increased black carbon aerosol concentration experiment, weakened sinking convection anomalies exist at the southerly position. This weakened sinking and its compensating rising convection anomalies in the south lead to the heavy rainfall over southeast coast areas of China. When concentrations of both sulfate and black carbon aerosols increase synchronously, the anomalous rainfall distribution is somewhat like that in the increased black carbon concentration aerosol experiment but with less intensity.

Numerical Simulation of Global Temperature Change during the 20th Century with the IAP/LASG GOALS Model

The IAP/LASG GOALS coupled model is used to simulate the climate change during the 20th century using historical greenhouse gases concentrations, the mass mixing ratio of sulfate aerosols simulated by a CTM model, and reconstruction of solar variability spanning the period 1900 to 1997. Four simulations, including a control simulation and three forcing simulations, are conducted. Comparison with the observational record for the period indicates that the three forcing experiments simulate reasonable temporal and spatial distributions of the temperature change. The global warming during the 20th century is caused mainly by increasing greenhouse gas concentration especially since the late 1980s; sulfate aerosols offset a portion of the global warming and the reduction of global temperature is up to about 0.11℃ over the century; additionally, the effect of solar variability is not negligible in the simulation of climate change over the 20th century.

Hygroscopicity of particles generated from photooxidation of α-pinene under diferent oxidation conditions in the presence of sulfate seed aerosols

Smog chamber experiments were conducted to investigate the hygroscopicity of particles generated from photooxidation of α-pinene/NOx with different sulfate seed aerosols or oxidation conditions. Hygroscopicity of particles was measured by a tandem differential mobility analyzer （TDMA） in terms of hygroscopic growth factor （Gf）, with a relative humidity of 85%. With sulfate seed aerosols present, Gf of the aerosols decreased very fast before notable secondary organic aerosols （SOA） formation was observed, indicating a heterogeneous process between inorganic seeds and organic products might take place as soon as oxidation begins, rather than only happening after gas-aerosol partition of organic products starts. The final SOA-coated sulfate particles had similar or lower Gf than seed-free SOA. The hygroscopicity of the final particles was not dependent on the thickness but on the hygroscopicity properties of the SOA, which were influenced by the initial sulfate seed particles. In the two designed aging processes, Gf of the particles increased more significantly with introduction of OH radical than with ozone. However, the hygroscopicity of SOA was very low even after a long time of aging, implying that either SOA aging in the chamber was very slow or the Gf of SOA did not change significantly in aging. Using an aerosol composition speciation monitor （ACSM） and matrix factorization （PMF） method, two factors for the components of SOA were identified, but the correlation between SOA hygroscopicity and the proportion of the more highly oxidized factor could be either positive or negative depending on the speciation of seed aerosols present.

Characteristics of dry deposited mineral particles associated with weather conditions in the adjacent sea areas of East China during a cruise in spring 2011

Dry deposited particles, larger than 1.3 μm, were collected under clear, cloudy, and foggy conditions during a cruise, traversing the Yellow Sea and the East China Sea from 23 March to 8 April 2011. In these areas, air masses are influenced by pollution outflows from the Asian continent. The size and elemental composition of dry deposited particles were investigated using a scanning electron microscope. Number-size distributions of these particles were approximately lognormal. Under clear conditions, the mode size was about 5.0 μm, with a mean diameter of 6.9 μm. Under cloudy and foggy conditions, the mean diameters were 5.7 and 6.0 μm, respectively, but the mode sizes were vague. Non-mixed mineral particles, sea salt, and mixed mineral-sea salt particles were the major particle types. Correspondingly, Al and Si were the most frequently detected elements. Frequencies of K-, Ca-, and S-containing particles were highest under foggy conditions, while the frequency of Na-containing particles was lowest. These results indicate that fog favored sulfate production on the particles and led to the deposited mineral particles more abundant in secondary salt, suggesting the importance to consider the dependence of the comoosition of deoosited mineral narticles on weather as well as narticle size.