Volcanic sulfur emissions: Estimates of source strength and its contribution to the global sulfate distribution

Anthropogenic emission of SO2 and conversion into SO42- is argued to be the most important factor damping and modulating the global greenhouse effect. Recent estimates of the relative strength of the three important sources of volatile sulfur (SO2 from fossil fuel combustion ∼78 Tg S/yr, from biomass burning ∼2 Tg S/yr, and from natural sources ∼25 Tg S/yr) suggest an overwhelming effect of the anthropogenic emissions for climate forcing. However, the radiatively relevant product SO42- may have different patterns due to the distribution of the sources (some very dense areas near the surface for anthropogenic SO2, formation of SO2 from dimethylsulfide in the marine boundary layer, and emission of volcanic SO2 mostly in the free atmosphere in rural areas). In this paper we study the relative contribution of volcanic SO2 emissions to the atmospheric sulfur budget applying an atmospheric general circulation model including a full sulfur cycle and prescribed source distributions. An off-line analysis tool is applied to determine the radiative forcing of sulfate aerosols. The results show that natural S sources are at least as important as the anthropogenic ones, even though their source strength is much smaller. The reasons are different lifetimes due to different production and emission processes. Therefore, we should improve our knowledge about the volcanic volatile sources and their time-space variability

Gas/particle partitioning and global distribution of polycyclic aromatic hydrocarbons – A modelling approach

The global atmospheric distribution and long-range transport (LRT) potential of three polycyclic aromatic hydrocarbons (PAH) - anthracene, fluoranthene and benzo[a]pyrene - are studied. The model used is a global aerosol-chemistry-transport-model, which is based on an atmospheric general circulation model. The model includes an in-built dynamic aerosol model coupled to two-dimensional surface compartments. Several parameterisations of gas/particle partitioning and different assumptions of degradation in the aerosol particulate phase were tested. PAHs are mostly distributed in the source regions but reach the Arctic and the Antarctic. The Canadian Arctic is predicted to be significantly less affected by mid-latitude PAH emissions than the European Arctic. Re-volatilisation is significant for semivolatile PAHs. Accumulation of semivolatile PAHs in polar regions, however, is not indicated. The model study suggests that gas/particle partitioning in air drastically influences the atmospheric cycling, the total environmental fate (e.g. compartmental distributions) and the LRT potential of the substances studied. A parameterisation which calculates the gas/particle partitioning assuming absorption into organic matter and adsorption to black carbon (soot) agrees best with the observations at remote sites. The study provides evidence that the degradation in the particulate phase must be slower than that in the gas-phase. The predicted concentrations of the semivolatile PAHs anthracene and fluoranthene in near-ground air at remote sites in mid and high northern latitudes are in line with measured concentrations, if adsorption of the substances to soot combined with absorption in particulate organic matter is assumed to determine gas/particle partitioning, but cannot be explained by adsorption alone (Junge-Pankow parameterisation of gas/particle partitioning). The results suggest that PAHs absorbed in the organic matrix of particulate matter is shielded from the gas-phase. (C) 2009 Elsevier Ltd. All rights reserved. [References: 42

Brightening of the global cloud field by nitric acid and the associated radiative forcing

Clouds cool Earth's climate by reflecting 20% of the incoming solar energy, while also trapping part of the outgoing radiation. The effect of human activities on clouds is poorly understood, but the present-day anthropogenic cooling via changes of cloud albedo and lifetime could be of the same order as warming from anthropogenic addition in CO<sub>2</sub>. Soluble trace gases can increase water condensation to particles, possibly leading to activation of smaller aerosols and more numerous cloud droplets. We have studied the effect of nitric acid on the aerosol indirect effect with the global aerosol-climate model ECHAM5.5-HAM2. Including the nitric acid effect in the model increases cloud droplet number concentrations globally by 7%. The nitric acid contribution to the present-day cloud albedo effect was found to be −0.32 W m<sup>−2</sup> and to the total indirect effect −0.46 W m<sup>−2</sup>. The contribution to the cloud albedo effect is shown to increase to −0.37 W m<sup>−2</sup> by the year 2100, if considering only the reductions in available cloud condensation nuclei. Overall, the effect of nitric acid can play a large part in aerosol cooling during the following decades with decreasing SO<sub>2</sub> emissions and increasing NO<sub>x</sub> and greenhouse gases

Sensitivity of aerosol concentrations and cloud properties to nucleation and secondary organic distribution in ECHAM5-HAM global circulation model

The global aerosol-climate model ECHAM5-HAM was modified to improve the representation of new particle formation in the boundary layer. Activation-type nucleation mechanism was introduced to produce observed nucleation rates in the lower troposphere. A simple and computationally efficient model for biogenic secondary organic aerosol (BSOA) formation was implemented. Here we study the sensitivity of the aerosol and cloud droplet number concentrations (CDNC) to these additions. Activation-type nucleation significantly increases aerosol number concentrations in the boundary layer. Increased particle number concentrations have a significant effect also on cloud droplet number concentrations and therefore on cloud properties. We performed calculations with activation nucleation coefficient values of 2×10⁻⁷s⁻¹, 2×10⁻⁶s⁻¹ and 2×10⁻⁵s⁻¹ to evaluate the sensitivity to this parameter. For BSOA we have used yields of 0.025, 0.07 and 0.15 to estimate the amount of monoterpene oxidation products available for condensation. The hybrid BSOA formation scheme induces large regional changes to size distribution of organic carbon, and therefore affects particle optical properties and cloud droplet number concentrations locally. Although activation-type nucleation improves modeled aerosol number concentrations in the boundary layer, the use of a global activation coefficient generally leads to overestimation of aerosol number. Overestimation can also arise from underestimation of primary emissions

Sensitivity of aerosol concentrations and cloud properties to nucleation and secondary organic distribution in ECHAM5-HAM global circulation model

The global aerosol-climate model ECHAM5-HAM was modified to improve the representation of new particle formation in the boundary layer. Activation-type nucleation mechanism was introduced to produce observed nucleation rates in the lower troposphere. A simple and computationally efficient model for biogenic secondary organic aerosol (BSOA) formation was implemented. Here we study the sensitivity of the aerosol and cloud droplet number concentrations (CDNC) to these additions. Activation-type nucleation significantly increases aerosol number concentrations in the boundary layer. Increased particle number concentrations have a significant effect also on cloud droplet number concentrations and therefore on cloud properties. We performed calculations with activation nucleation coefficient values of 2 x 10(-7) s(-1), 2 x 10(-6) s(-1) and 2 x 10(-5) s(-1) to evaluate the sensitivity to this parameter. For BSOA we have used yields of 0.025, 0.07 and 0.15 to estimate the amount of monoterpene oxidation products available for condensation. The hybrid BSOA formation scheme induces large regional changes to size distribution of organic carbon, and therefore affects particle optical properties and cloud droplet number concentrations locally. Although activation-type nucleation improves modeled aerosol number concentrations in the boundary layer, the use of a global activation coefficient generally leads to overestimation of aerosol number. Overestimation can also arise from underestimation of primary emissions.The global aerosol-climate model ECHAM5-HAM was modified to improve the representation of new particle formation in the boundary layer. Activation-type nucleation mechanism was introduced to produce observed nucleation rates in the lower troposphere. A simple and computationally efficient model for biogenic secondary organic aerosol (BSOA) formation was implemented. Here we study the sensitivity of the aerosol and cloud droplet number concentrations (CDNC) to these additions. Activation-type nucleation significantly increases aerosol number concentrations in the boundary layer. Increased particle number concentrations have a significant effect also on cloud droplet number concentrations and therefore on cloud properties. We performed calculations with activation nucleation coefficient values of 2 x 10(-7) s(-1), 2 x 10(-6) s(-1) and 2 x 10(-5) s(-1) to evaluate the sensitivity to this parameter. For BSOA we have used yields of 0.025, 0.07 and 0.15 to estimate the amount of monoterpene oxidation products available for condensation. The hybrid BSOA formation scheme induces large regional changes to size distribution of organic carbon, and therefore affects particle optical properties and cloud droplet number concentrations locally. Although activation-type nucleation improves modeled aerosol number concentrations in the boundary layer, the use of a global activation coefficient generally leads to overestimation of aerosol number. Overestimation can also arise from underestimation of primary emissions.The global aerosol-climate model ECHAM5-HAM was modified to improve the representation of new particle formation in the boundary layer. Activation-type nucleation mechanism was introduced to produce observed nucleation rates in the lower troposphere. A simple and computationally efficient model for biogenic secondary organic aerosol (BSOA) formation was implemented. Here we study the sensitivity of the aerosol and cloud droplet number concentrations (CDNC) to these additions. Activation-type nucleation significantly increases aerosol number concentrations in the boundary layer. Increased particle number concentrations have a significant effect also on cloud droplet number concentrations and therefore on cloud properties. We performed calculations with activation nucleation coefficient values of 2 x 10(-7) s(-1), 2 x 10(-6) s(-1) and 2 x 10(-5) s(-1) to evaluate the sensitivity to this parameter. For BSOA we have used yields of 0.025, 0.07 and 0.15 to estimate the amount of monoterpene oxidation products available for condensation. The hybrid BSOA formation scheme induces large regional changes to size distribution of organic carbon, and therefore affects particle optical properties and cloud droplet number concentrations locally. Although activation-type nucleation improves modeled aerosol number concentrations in the boundary layer, the use of a global activation coefficient generally leads to overestimation of aerosol number. Overestimation can also arise from underestimation of primary emissions.Peer reviewe

Analysis and quantification of the diversities of aerosol life cycles within AeroCom

Simulation results of global aerosol models have been assembled in the framework of the AeroCom intercomparison exercise. In this paper, we analyze the life cycles of dust, sea salt, sulfate, black carbon and particulate organic matter as simulated by sixteen global aerosol models. The diversities among the models for the sources and sinks, burdens, particle sizes, water uptakes, and spatial dispersals have been established. These diversities have large consequences for the calculated radiative forcing and the aerosol concentrations at the surface. The AeroCom all-models-average emissions are dominated by the mass of sea salt (SS), followed by dust (DU), sulfate (SO_4), particulate organic matter (POM), and finally black carbon (BC). Interactive parameterizations of the emissions and contrasting particles sizes of SS and DU lead generally to higher diversities of these species, and for total aerosol. The lower diversity of the emissions of the fine aerosols, BC, POM, and SO_4, is due to the use of similar emission inventories, and does therefore not necessarily indicate a better understanding of their sources. The diversity of SO_4-sources is mainly caused by the disagreement on depositional loss of precursor gases and on chemical production. The diversities of the emissions are passed on to the burdens, but the latter are also strongly affected by the model-specific treatments of transport and aerosol processes. The burdens of dry masses decrease from largest to smallest: DU, SS, SO_4, POM, and BC. The all-models-average residence time is shortest for SS with about half a day, followed by S_O4 and DU with four days, and POM and BC with six and seven days, respectively. The wet deposition rate is controlled by the solubility and increases from DU, BC, POM to SO_4 and SS. It is the dominant sink for SO_4, BC, and POM, and contributes about one third to the total removal rate coefficients of SS and DU species. For SS and DU we find high diversities for the removal rate coefficients and deposition pathways. Models do neither agree on the split between wet and dry deposition, nor on that between sedimentation and turbulent dry Deposition. We diagnose an extremely high diversity for the uptake of ambient water vapor that influences the particle size and thus the sink rate coefficients. Furthermore, we find little agreement among the model results for the partitioning of wet removal into scavenging by convective and stratiform rain. Large differences exist for aerosol dispersal both in the vertical and in the horizontal direction. In some models, a minimum of total aerosol concentration is simulated at the surface. Aerosol dispersal is most pronounced for SO4 and BC and lowest for SS. Diversities are higher for meridional than for vertical dispersal, they are similar for a given species and highest for SS and DU. For these two components we do not find a correlation between vertical and meridional aerosol dispersal. In addition the degree of dispersals of SS and DU is not related to their residence times. SO_4, BC, and POM, however, show increased meridional dispersal in models with larger vertical dispersal, and dispersal is larger for longer simulated residence times

The regional aerosol-climate model REMO-HAM

REMO-HAM is a new regional aerosol-climate model. It is based on the REMO regional climate model and includes most of the major aerosol processes. The structure for aerosol is similar to the global aerosol-climate model ECHAM5-HAM, for example the aerosol module HAM is coupled with a two-moment stratiform cloud scheme. On the other hand, REMO-HAM does not include an online coupled aerosol-radiation nor a secondary organic aerosol module. In this work, we evaluate the model and compare the results against ECHAM5-HAM and measurements. Four different measurement sites were chosen for the comparison of total number concentrations, size distributions and gas phase sulfur dioxide concentrations: Hyytiälä in Finland, Melpitz in Germany, Mace Head in Ireland and Jungfraujoch in Switzerland. REMO-HAM is run with two different resolutions: 50 × 50 km2 and 10 × 10 km2. Based on our simulations, REMO-HAM is in reasonable agreement with the measured values. The differences in the total number concentrations between REMO-HAM and ECHAM5-HAM can be mainly explained by the difference in the nucleation mode. Since we did not use activation nor kinetic nucleation for the boundary layer, the total number concentrations are somewhat underestimated. From the meteorological point of view, REMO-HAM represents the precipitation fields and 2 m temperature profile very well compared to measurement. Overall, we show that REMO-HAM is a functional aerosol-climate model, which will be used in further studies

A comparison of scavenging and deposition processes in global models: results from the WCRP Cambridge Workshop of 1995

Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/75543/1/j.1600-0889.2000.00980.x.pd

Sources of land-derived runoff to a coral reef-fringed embayment identified using geochemical tracers in nearshore sediment traps

This paper is not subject to U.S. copyright. The definitive version was published in Estuarine, Coastal and Shelf Science 85 (2009): 459-471, doi:10.1016/j.ecss.2009.09.014.Geochemical tracers, including Ba, Co, Th, 7Be, 137Cs and 210Pb, and magnetic properties were used to characterize terrestrial runoff collected in nearshore time-series sediment traps in Hanalei Bay, Kauai, during flood and dry conditions in summer 2006, and to fingerprint possible runoff sources in the lower watershed. In combination, the tracers indicate that runoff during a flood in August could have come from cultivated taro fields bordering the lower reach of the river. Land-based runoff associated with summer floods may have a greater impact on coral reef communities in Hanalei Bay than in winter because sediment persists for several months. During dry periods, sediment carried by the Hanalei River appears to have been mobilized primarily by undercutting of low 7Be, low 137Cs riverbanks composed of soil weathered from tholeiitic basalt with low Ba and Co concentrations. Following a moderate rainfall event in September, high 7Be sediment carried by the Hanalei River was probably mobilized by overland flow in the upper watershed. Ba-desorption in low-salinity coastal water limited its use to a qualitative runoff tracer in nearshore sediment. 210Pb had limited usefulness as a terrestrial tracer in the nearshore due to a large dissolved oceanic source and scavenging onto resuspended bottom sediment. 210Pb-scavenging does, however, illustrate the role resuspension could play in the accumulation of particle-reactive contaminants in nearshore sediment. Co and 137Cs were not affected by desorption or geochemical scavenging and showed the greatest potential as quantitative sediment provenance indicators in material collected in nearshore sediment traps