Atmosphere–ocean–aerosol–chemistry–climate model SOCOLv4.0: description and evaluation

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.

Urban aerosol chemistry at a land–water transition site during summer – Part 1: Impact of agricultural and industrial ammonia emissions

This study characterizes the impact of the Chesapeake Bay and associated meteorological phenomena on aerosol chemistry during the second Ozone Water-Land Environmental Transition Study (OWLETS-2) field campaign, which took place from 4 June to 5 July 2018. Measurements of inorganic PM2.5 composition, gas-phase ammonia (NH3), and an array of meteorological parameters were undertaken at Hart-Miller Island (HMI), a land–water transition site just east of downtown Baltimore on the Chesapeake Bay. The observations at HMI were characterized by abnormally high NH3 concentrations (maximum of 19.3 µg m−3, average of 3.83 µg m−3), which were more than a factor of 3 higher than NH3 levels measured at the closest atmospheric Ammonia Monitoring Network (AMoN) site (approximately 45 km away). While sulfate concentrations at HMI agreed quite well with those measured at a regulatory monitoring station 45 km away, aerosol ammonium and nitrate concentrations were significantly higher, due to the ammonia-rich conditions that resulted from the elevated NH3. The high NH3 concentrations were largely due to regional agricultural emissions, including dairy farms in southeastern Pennsylvania and poultry operations in the Delmarva Peninsula (Delaware–Maryland–Virginia). Reduced NH3 deposition during transport over the Chesapeake Bay likely contributed to enhanced concentrations at HMI compared to the more inland AMoN site. Several peak NH3 events were recorded, including the maximum NH3 observed during OWLETS-2, that appear to originate from a cluster of industrial sources near downtown Baltimore. Such events were all associated with nighttime emissions and advection to HMI under low wind speeds (< 1 m s−1) and stable atmospheric conditions. Our results demonstrate the importance of industrial sources, including several that are not represented in the emissions inventory, on urban air quality. Together with our companion paper, which examines aerosol liquid water and pH during OWLETS-2, we highlight unique processes affecting urban air quality of coastal cities that are distinct from continental locations.

Rapid mass growth and enhanced light extinction of atmospheric aerosols during the heating season haze episodes in Beijing revealed by aerosol–chemistry–radiation–boundary layer interaction

Despite the numerous studies investigating haze formation mechanism in China, it is still puzzling that intensive haze episodes could form within hours directly following relatively clean periods. Haze has been suggested to be initiated by the variation of meteorological parameters and then to be substantially enhanced by aerosol–radiation–boundary layer feedback. However, knowledge on the detailed chemical processes and the driving factors for extensive aerosol mass accumulation during the feedback is still scarce. Here, the dependency of the aerosol number size distribution, mass concentration and chemical composition on the daytime mixing layer height (MLH) in urban Beijing is investigated. The size distribution and chemical composition-resolved dry aerosol light extinction is also explored. The results indicate that the aerosol mass concentration and fraction of nitrate increased dramatically when the MLH decreased from high to low conditions, corresponding to relatively clean and polluted conditions, respectively. Particles having their dry diameters in the size of ∼400–700 nm, and especially particle-phase ammonium nitrate and liquid water, contributed greatly to visibility degradation during the winter haze periods. The dependency of aerosol composition on the MLH revealed that ammonium nitrate and aerosol water content increased the most during low MLH conditions, which may have further triggered enhanced formation of sulfate and organic aerosol via heterogeneous reactions. As a result, more sulfate, nitrate and water-soluble organics were formed, leading to an enhanced water uptake ability and increased light extinction by the aerosols. The results of this study contribute towards a more detailed understanding of the aerosol–chemistry–radiation–boundary layer feedback that is likely to be responsible for explosive aerosol mass growth events in urban Beijing.

Reductions in the deposition of sulfur and selenium to agricultural soils pose risk of future nutrient deficiencies

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.

Urban aerosol chemistry at a land-water transition site during summer – Part 1: Impact of agricultural and industrial ammonia emissions

This study characterizes the impact of the Chesapeake Bay and associated meteorological phenomena on aerosol chemistry during the second Ozone Water-Land Environmental Transition Study (OWLETS-2) field campaign during summer 2018. Measurements of inorganic PM2.5 composition, gas-phase ammonia (NH3), and an array of meteorological parameters were undertaken at Hart-Miller Island (HMI), a land-water transition site just east of downtown Baltimore on the Chesapeake Bay. The observations at HMI were characterized by abnormally high NH3 concentrations (maximum of 19.3 μg m-3, average of 3.83 μg m-3), which were more than a factor of three higher than NH3 levels measured at the closest Atmospheric Ammonia Network (AMoN) site (approximately 45 km away). While sulfate concentrations at HMI agreed quite well with those measured at a regulatory monitoring station 45 km away, aerosol ammonium and nitrate concentrations were significantly higher, due to the ammonia-rich conditions that resulted from the elevated NH3. The high NH3 concentrations were largely due to regional agricultural emissions, including dairy farms in southeastern Pennsylvania and poultry operations in the Delmarva Peninsula (Delaware-Maryland-Virginia). Reduced NH3 deposition during transport over the Chesapeake Bay likely contributed to enhanced concentrations at HMI compared to the more inland AMoN site. Several peak NH3 events were recorded, including the maximum NH3 observed during OWLETS-2, that appear to originate from a cluster of industrial sources near downtown Baltimore. Such events were all associated with nighttime emissions and advection to HMI under low 15 wind speeds (< 1 m s-1) and stable atmospheric conditions. Our results demonstrate the importance of industrial sources, including several that are not represented in the emissions inventory, on urban air quality. Together with our companion paper, which examines aerosol liquid water and pH during OWLETS-2, we highlight unique processes affecting urban air quality of coastal cities that are distinct from continental locations.

Photolytic radical persistence due to anoxia in viscous aerosol particles

In viscous, organic-rich aerosol particles containing iron, sunlight may induce anoxic conditions that stabilize reactive oxygen species (ROS) and carbon-centered radicals (CCRs). In laboratory experiments, we show mass loss, iron oxidation and radical formation and release from photoactive organic particles containing iron. Our results reveal a range of temperature and relative humidity, including ambient conditions, that control ROS build up and CCR persistence in photochemically active, viscous organic particles. We find that radicals can attain high concentrations, altering aerosol chemistry and exacerbating health hazards of aerosol exposure. Our physicochemical kinetic model confirmed these results, implying that oxygen does not penetrate such particles due to the combined effects of fast reaction and slow diffusion near the particle surface, allowing photochemically-produced radicals to be effectively trapped in an anoxic organic matrix.