SOCOL-AERv1 was developed as an aerosol–chemistry–climate model to study the stratospheric sulfur cycle and its influence on climate and the ozone layer. It includes a sectional aerosol model that tracks the sulfate particle size distribution in 40 size bins, between 0.39 nm and 3.2 µm. Sheng et al. (2015) showed that SOCOL-AERv1 successfully matched observable quantities related to stratospheric aerosol. In the meantime, SOCOL-AER has undergone significant improvements and more observational datasets have become available. In producing SOCOL-AERv2 we have implemented several updates to the model: adding interactive deposition schemes, improving the sulfate mass and particle number conservation, and expanding the tropospheric chemistry scheme. We compare the two versions of the model with background stratospheric sulfate aerosol observations, stratospheric aerosol evolution after Pinatubo, and ground-based sulfur deposition networks. SOCOL-AERv2 shows similar levels of agreement as SOCOL-AERv1 with satellite-measured extinctions and in situ optical particle counter (OPC) balloon flights. The volcanically quiescent total stratospheric aerosol burden simulated in SOCOL-AERv2 has increased from 109 Gg of sulfur (S) to 160 Gg S, matching the newly available satellite estimate of 165 Gg S. However, SOCOL-AERv2 simulates too high cross-tropopause transport of tropospheric SO₂ and/or sulfate aerosol, leading to an overestimation of lower stratospheric aerosol. Due to the current lack of upper tropospheric SO₂ measurements and the neglect of organic aerosol in the model, the lower stratospheric bias of SOCOL-AERv2 was not further improved. Model performance under volcanically perturbed conditions has also undergone some changes, resulting in a slightly shorter volcanic aerosol lifetime after the Pinatubo eruption. With the improved deposition schemes of SOCOL-AERv2, simulated sulfur wet deposition fluxes are within a factor of 2 of measured deposition fluxes at 78 % of the measurement stations globally, an agreement which is on par with previous model intercomparison studies. Because of these improvements, SOCOL-AERv2 will be better suited to studying changes in atmospheric sulfur deposition due to variations in climate and emissions.

Atmospheric deposition is a major source of the nutrients sulfur and selenium to agricultural soils. Air pollution control and cleaner energy production have reduced anthropogenic emissions of sulfur and selenium, which has led to lower atmospheric deposition fluxes of these elements. Here, we use a global aerosol-chemistry-climate model to map recent (2005–2009) sulfur and selenium deposition, and project future (2095–2099) changes under two socioeconomic scenarios. Across the Northern Hemisphere, we find substantially decreased deposition to agricultural soils, by 70 to 90% for sulfur and by 55 to 80% for selenium. Recent trends in sulfur and selenium concentrations in USA streams suggest that catchment mass balances of these elements are already changing due to the declining atmospheric supply. Sustainable fertilizer management strategies will need to be developed to offset the decrease in atmospheric nutrient supply and ensure future food security and nutrition, while avoiding consequences for downstream aquatic ecosystems.

This paper features the new atmosphere–ocean–aerosol–chemistry–climate model, SOlar Climate Ozone Links (SOCOL) v4.0, and its validation. The new model was built by interactively coupling the Max Planck Institute Earth System Model version 1.2 (MPI-ESM1.2) (T63, L47) with the chemistry (99 species) and size-resolving (40 bins) sulfate aerosol microphysics modules from the aerosol–chemistry–climate model, SOCOL-AERv2. We evaluate its performance against reanalysis products and observations of atmospheric circulation, temperature, and trace gas distribution, with a focus on stratospheric processes. We show that SOCOLv4.0 captures the low- and midlatitude stratospheric ozone well in terms of the climatological state, variability and evolution. The model provides an accurate representation of climate change, showing a global surface warming trend consistent with observations as well as realistic cooling in the stratosphere caused by greenhouse gas emissions, although, as in previous model versions, a too-fast residual circulation and exaggerated mixing in the surf zone are still present. The stratospheric sulfur budget for moderate volcanic activity is well represented by the model, albeit with slightly underestimated aerosol lifetime after major eruptions. The presence of the interactive ocean and a successful representation of recent climate and ozone layer trends make SOCOLv4.0 ideal for studies devoted to future ozone evolution and effects of greenhouse gases and ozone-destroying substances, as well as the evaluation of potential solar geoengineering measures through sulfur injections. Potential further model improvements could be to increase the vertical resolution, which is expected to allow better meridional transport in the stratosphere, as well as to update the photolysis calculation module and budget of mesospheric odd nitrogen. In summary, this paper demonstrates that SOCOLv4.0 is well suited for applications related to the stratospheric ozone and sulfate aerosol evolution, including its participation in ongoing and future model intercomparison projects.

Mercury (Hg), a neurotoxic heavy metal, is transferred to marine and terrestrial ecosystems through atmospheric transport. Recent studies have highlighted the role of vegetation uptake as a sink for atmospheric elemental mercury (Hg⁰) and a source of Hg to soils. However, the global magnitude of the Hg⁰ vegetation uptake flux is highly uncertain, with estimates ranging 1000–4000 Mg per year. To constrain this sink, we compare simulations in the chemical transport model GEOS-Chem with a compiled database of litterfall, throughfall, and flux tower measurements from 93 forested sites. The prior version of GEOS-Chem predicts median Hg⁰ dry deposition velocities similar to litterfall measurements from Northern hemisphere temperate and boreal forests (∼0.03 cm s⁻¹), yet it underestimates measurements from a flux tower study (0.04 cm s⁻¹vs. 0.07 cm s⁻¹) and Amazon litterfall (0.05 cm s⁻¹vs. 0.17 cm s⁻¹). After revising the Hg⁰ reactivity within the dry deposition parametrization to match flux tower and Amazon measurements, GEOS-Chem displays improved agreement with the seasonality of atmospheric Hg⁰ observations in the Northern midlatitudes. Additionally, the modelled bias in Hg⁰ concentrations in South America decreases from +0.21 ng m⁻³ to +0.05 ng m⁻³. We calculate a global flux of Hg⁰ dry deposition to land of 2276 Mg per year, approximately double previous model estimates. The Amazon rainforest contributes 29% of the total Hg⁰ land sink, yet continued deforestation and climate change threatens the rainforest's stability and thus its role as an important Hg sink. In an illustrative worst-case scenario where the Amazon is completely converted to savannah, GEOS-Chem predicts that an additional 283 Mg Hg per year would deposit to the ocean, where it can bioaccumulate in the marine food chain. Biosphere–atmosphere interactions thus play a crucial role in global Hg cycling and should be considered in assessments of future Hg pollution.

Stratospheric sulfate geoengineering (SSG) could contribute to avoiding some of the adverse impacts of climate change. We used the SOCOL-AER global aerosol–chemistry–climate model to investigate 21 different SSG scenarios, each with 1.83 Mt S yr⁻¹ injected either in the form of accumulation-mode H₂SO₄ droplets (AM H₂SO₄), gas-phase SO₂ or as combinations of both. For most scenarios, the sulfur was continuously emitted at an altitude of 50 hPa (≈20 km) in the tropics and subtropics. We assumed emissions to be zonally and latitudinally symmetric around the Equator. The spread of emissions ranged from 3.75^∘ S–3.75^∘ N to 30^∘ S–30^∘ N. In the SO₂ emission scenarios, continuous production of tiny nucleation-mode particles results in increased coagulation, which together with gaseous H₂SO₄ condensation, produces coarse-mode particles. These large particles are less effective for backscattering solar radiation and have a shorter stratospheric residence time than AM H₂SO₄ particles. On average, the stratospheric aerosol burden and corresponding all-sky shortwave radiative forcing for the AM H₂SO₄ scenarios are about 37 % larger than for the SO₂ scenarios. The simulated stratospheric aerosol burdens show a weak dependence on the latitudinal spread of emissions. Emitting at 30^∘ N–30^∘ S instead of 10^∘ N–10^∘ S only decreases stratospheric burdens by about 10 %. This is because a decrease in coagulation and the resulting smaller particle size is roughly balanced by faster removal through stratosphere-to-troposphere transport via tropopause folds. Increasing the injection altitude is also ineffective, although it generates a larger stratospheric burden, because enhanced condensation and/or coagulation leads to larger particles, which are less effective scatterers. In the case of gaseous SO₂ emissions, limiting the sulfur injections spatially and temporally in the form of point and pulsed emissions reduces the total global annual nucleation, leading to less coagulation and thus smaller particles with increased stratospheric residence times. Pulse or point emissions of AM H₂SO₄ have the opposite effect: they decrease the stratospheric aerosol burden by increasing coagulation and only slightly decrease clear-sky radiative forcing. This study shows that direct emission of AM H₂SO₄ results in higher radiative forcing for the same sulfur equivalent mass injection strength than SO₂ emissions, and that the sensitivity to different injection strategies varies for different forms of injected sulfur.