Globally, carbonyl sulphide (COS) is the most abundant sulphur gas in the atmosphere. Our chemistry-climate model (CCM) of the lower and middle atmosphere with aerosol module realistically simulates ...the background stratospheric sulphur cycle, as observed by satellites in volcanically quiescent periods. The model results indicate that upward transport of COS from the troposphere largely controls the sulphur budget and the aerosol loading of the background stratosphere. This differs from most previous studies which indicated that short-lived sulphur gases are also important. The model realistically simulates the modulation of the particulate and gaseous sulphur abundance in the stratosphere by the quasi-biennial oscillation (QBO). In the lowermost stratosphere organic carbon aerosol contributes significantly to extinction. Further, using a chemical radiative convective model and recent spectra, we compute that the direct radiative forcing efficiency by 1 kg of COS is 724 times that of 1 kg CO2. Considering an anthropogenic fraction of 30% (derived from ice core data), this translates into an overall direct radiative forcing by COS of 0.003 W m−2. The direct global warming potentials of COS over time horizons of 20 and 100 yr are GWP(20 yr) = 97 and GWP(100 yr) = 27, respectively (by mass). Furthermore, stratospheric aerosol particles produced by the photolysis of COS (chemical feedback) contribute to a negative direct solar radiative forcing, which in the CCM amounts to −0.007 W m−2 at the top of the atmosphere for the anthropogenic fraction, more than two times the direct warming forcing of COS. Considering that the lifetime of COS is twice that of stratospheric aerosols the warming and cooling tendencies approximately cancel.
In this study we use the ECHAM/MESSy Atmospheric Chemistry (EMAC) model to simulate global fields of the effective hygroscopicity parameter κ which approximately describes the influence of chemical ...composition on the cloud condensation nucleus (CCN) activity of aerosol particles. The obtained global mean values of κ at the Earth's surface are 0.27±0.21 for continental and 0.72±0.24 for marine regions (arithmetic mean ± standard deviation). These values are the internally mixed κ calculated across the Aitken and accumulation modes. The mean κ values are in good agreement with previous estimates based on observational data, but the model standard deviation for continental regions is higher. Over the continents, the regional distribution appears fairly uniform, with κ values mostly in the range of 0.1–0.4. Lower values over large arid regions and regions of high organic loading lead to reduced continental average values for Africa and South America (0.15–0.17) compared to the other continents (0.21–0.36). Marine regions show greater variability with κ values ranging from 0.9–1.0 in remote regions to 0.4–0.6 in continental outflow regions where the highly hygroscopic sea spray aerosol mixes with less hygroscopic continental aerosol. Marine κ values as low as 0.2–0.3 are simulated in the outflow from the Sahara desert. At the top of the planetary boundary layer the κ values can deviate substantially from those at the surface (up to 30%) – especially in marine and coastal regions. In moving from the surface to the height of the planetary boundary layer, the global average marine κ value reduces by 20%. Thus, surface observations may not always be representative for the altitudes where cloud formation mostly occurs. In a pre-industrial model scenario, the κ values tend to be higher over marine regions and lower over the continents, because the anthropogenic particulate matter is on average less hygroscopic than sea-spray but more hygroscopic than the natural continental background aerosol (dust and organic matter). In regions influenced by desert dust the particle hygroscopicity has increased strongly as the mixing of air pollutants with mineral particles typically enhances the κ values by a factor of 2–3 above the initial value of ≈0.005.
Multiyear simulations with the atmospheric chemistry general circulation model EMAC with a microphysical modal aerosol module at high vertical resolution demonstrate that the sulfur gases COS and ...SO2, the latter from low‐latitude and midlatitude volcanic eruptions, predominantly control the formation of stratospheric aerosol. Marine dimethyl sulfide (DMS) and other SO2 sources, including strong anthropogenic emissions in China, are found to play a minor role except in the lowermost stratosphere. Estimates of volcanic SO2 emissions are based on satellite observations using Total Ozone Mapping Spectrometer and Ozone Monitoring Instrument for total injected mass and Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat or Stratospheric Aerosol and Gases Experiment for the spatial distribution. The 10 year SO2 and COS data set of MIPAS is also used for model evaluation. The calculated radiative forcing of stratospheric background aerosol including sulfate from COS and small contributions by DMS oxidation, and organic aerosol from biomass burning, is about 0.07W/m2. For stratospheric sulfate aerosol from medium and small volcanic eruptions between 2005 and 2011 a global radiative forcing up to 0.2W/m2 is calculated, moderating climate warming, while for the major Pinatubo eruption the simulated forcing reaches 5W/m2, leading to temporary climate cooling. The Pinatubo simulation demonstrates the importance of radiative feedback on dynamics, e.g., enhanced tropical upwelling, for large volcanic eruptions.
Key Points
COS and volcanic injections of SO2 explain most of stratospheric aerosol
Simulated radiative forcing consistent with estimates from observations
All eruptions detected by MIPAS should be considered
In the last decades several convection parameterisations have been developed to consider the impact of small-scale unresolved processes in Earth System Models associated with convective clouds. ...Global model simulations, which have been performed under current climate conditions with different convection schemes, significantly differ among each other in the simulated transport of trace gases and precipitation patterns due to the parameterisation assumptions and formulations, e.g. the computation of convective rainfall rates, calculation of entrainment and detrainment rates etc. Here we address sensitivity studies comparing four different convection schemes under alternative climate conditions (with doubling of the CO2 concentrations) to identify uncertainties related to convective processes. The increase in surface temperature reveals regional differences up to 4 K dependent on the chosen convection parameterisation. These differences are statistically significant almost everywhere in the troposphere of the intertropical convergence zone. The increase in upper tropospheric temperature affects the amount of water vapour transported to the lower stratosphere, leading to enhanced water vapour contents between 40% and 60% at the cold point temperature in the Tropics. Furthermore, the change in transporting short-lived pollutants within the atmosphere is highly ambiguous for the lower and upper troposphere. These results reflect that different approaches to compute mass fluxes, detrainment levels or trigger functions determine the transport of short-lived trace gases from the planetary boundary layer to lower, middle or upper tropospheric levels. Finally, cloud radiative effects have been analysed, uncovering a shift in different cloud types in the Tropics, especially for cirrus and deep convective clouds. These cloud types induce a change in net cloud radiative forcing varying from 0.5 W m−2 to 2.0 W m−2.
The Modular Earth Submodel System (MESSy) is an open, multi-institutional project providing a strategy for developing comprehensive Earth System Models (ESMs) with highly flexible complexity. The ...first version of the MESSy infrastructure and process submodels, mainly focusing on atmospheric chemistry, has been successfully coupled to an atmospheric General Circulation Model (GCM) expanding it into an Atmospheric Chemistry GCM (AC-GCM) for nudged simulations and into a Chemistry Climate Model (CCM) for climate simulations. Here, we present the second development cycle of MESSy, which comprises (1) an improved and extended infrastructure for the basemodel independent coupling of process-submodels, (2) new, highly valuable diagnostic capabilities for the evaluation with observational data and (3) an improved atmospheric chemistry setup. With the infrastructural changes, we place the headstone for further model extensions from a CCM towards a comprehensive ESM. The new diagnostic submodels will be used for regular re-evaluations of the continuously further developing model system. The updates of the chemistry setup are briefly evaluated.
Urban upbringing has consistently been associated with schizophrenia, but which specific environmental exposures are reflected by this epidemiological observation and how they impact the developing ...brain to increase risk is largely unknown. On the basis of prior observations of abnormal functional brain processing of social stress in urban-born humans and preclinical evidence for enduring structural brain effects of early social stress, we investigated a possible morphological correlate of urban upbringing in human brain. In a sample of 110 healthy subjects studied with voxel-based morphometry, we detected a strong inverse correlation between early-life urbanicity and gray matter (GM) volume in the right dorsolateral prefrontal cortex (DLPFC, Brodmann area 9). Furthermore, we detected a negative correlation of early-life urbanicity and GM volumes in the perigenual anterior cingulate cortex (pACC) in men only. Previous work has linked volume reductions in the DLPFC to the exposure to psychosocial stress, including stressful experiences in early life. Besides, anatomical and functional alterations of this region have been identified in schizophrenic patients and high-risk populations. Previous data linking functional hyperactivation of pACC during social stress to urban upbringing suggest that the present interaction effect in brain structure might contribute to an increased risk for schizophrenia in males brought up in cities. Taken together, our results suggest a neural mechanism by which early-life urbanicity could impact brain architecture to increase the risk for schizophrenia.
The new global anthropogenic emission inventory (EDGAR-CIRCE) of gas and aerosol pollutants has been incorporated in the chemistry general circulation model EMAC (ECHAM5/MESSy Atmospheric Chemistry). ...A relatively high horizontal resolution simulation is performed for the years 2005-2008 to evaluate the capability of the model and the emissions to reproduce observed aerosol concentrations and aerosol optical depth (AOD) values. Model output is compared with observations from different measurement networks (CASTNET, EMEP and EANET) and AODs from remote sensing instruments (MODIS and MISR). A good spatial agreement of the distribution of sulfate and ammonium aerosol is found when compared to observations, while calculated nitrate aerosol concentrations show some discrepancies. The simulated temporal development of the inorganic aerosols is in line with measurements of sulfate and nitrate aerosol, while for ammonium aerosol some deviations from observations occur over the USA, due to the wrong temporal distribution of ammonia gas emissions. The calculated AODs agree well with the satellite observations in most regions, while negative biases are found for the equatorial area and in the dust outflow regions (i.e. Central Atlantic and Northern Indian Ocean), due to an underestimation of biomass burning and aeolian dust emissions, respectively. Aerosols and precursors budgets for five different regions (North America, Europe, East Asia, Central Africa and South America) are calculated. Over East-Asia most of the emitted aerosols (precursors) are also deposited within the region, while in North America and Europe transport plays a larger role. Further, it is shown that a simulation with monthly varying anthropogenic emissions typically improves the temporal correlation by 5-10% compared to one with constant annual emissions.
Bacteria are constantly being transported through the atmosphere, which may have implications for human health, agriculture, cloud formation, and the dispersal of bacterial species. We simulate the ...global transport of bacteria, represented as 1 μm and 3 μm diameter spherical solid particle tracers in a general circulation model. We investigate factors influencing residence time and distribution of the particles, including emission region, cloud condensation nucleus activity and removal by ice-phase precipitation. The global distribution depends strongly on the assumptions made about uptake into cloud droplets and ice. The transport is also affected, to a lesser extent, by the emission region, particulate diameter, and season. We find that the seasonal variation in atmospheric residence time is insufficient to explain by itself the observed seasonal variation in concentrations of particulate airborne culturable bacteria, indicating that this variability is mainly driven by seasonal variations in culturability and/or emission strength. We examine the potential for exchange of bacteria between ecosystems and obtain rough estimates of the flux from each ecosystem by using a maximum likelihood estimation technique, together with a new compilation of available observations described in a companion paper. Globally, we estimate the total emissions of bacteria-containing particles to the atmosphere to be 7.6×1023–3.5×1024 a−1, originating mainly from grasslands, shrubs and crops. We estimate the mass of emitted bacteria- to be 40–1800 Gg a−1, depending on the mass fraction of bacterial cells in the particles. In order to improve understanding of this topic, more measurements of the bacterial content of the air and of the rate of surface-atmosphere exchange of bacteria will be necessary. Future observations in wetlands, hot deserts, tundra, remote glacial and coastal regions and over oceans will be of particular interest.
The new Modular Earth Submodel System (MESSy) describes atmospheric chemistry and meteorological processes in a modular framework, following strict coding standards. It has been coupled to the ECHAM5 ...general circulation model, which has been slightly modified for this purpose. A 90-layer model setup up to 0.01 hPa was used at spectral T42 resolution to simulate the lower and middle atmosphere. With the high vertical resolution the model simulates the Quasi-Biennial Oscillation. The model meteorology has been tested to check the influence of the changes to ECHAM5 and the radiation interactions with the new representation of atmospheric composition. In the simulations presented here a Newtonian relaxation technique was applied in the tropospheric part of the domain to weakly nudge the model towards the analysed meteorology during the period 1998–2005. This allows an efficient and direct evaluation with satellite and in-situ data. It is shown that the tropospheric wave forcing of the stratosphere in the model suffices to reproduce major stratospheric warming events leading e.g. to the vortex split over Antarctica in 2002. Characteristic features such as dehydration and denitrification caused by the sedimentation of polar stratospheric cloud particles and ozone depletion during winter and spring are simulated well, although ozone loss in the lower polar stratosphere is slightly underestimated. The model realistically simulates stratosphere-troposphere exchange processes as indicated by comparisons with satellite and in situ measurements. The evaluation of tropospheric chemistry presented here focuses on the distributions of ozone, hydroxyl radicals, carbon monoxide and reactive nitrogen compounds. In spite of minor shortcomings, mostly related to the relatively coarse T42 resolution and the neglect of inter-annual changes in biomass burning emissions, the main characteristics of the trace gas distributions are generally reproduced well. The MESSy submodels and the ECHAM5/MESSy1 model output are available through the internet on request.
The simulation of convection, lightning and consequent NOx emissions with global atmospheric chemistry models is associated with large uncertainties since these processes are heavily parameterised. ...Each parameterisation by itself has deficiencies and the combination of these substantially increases the uncertainties compared to the individual parameterisations. In this study several combinations of state-of-the-art convection and lightning parameterisations are used in simulations with the global atmospheric chemistry general circulation model ECHAM5/MESSy, and are evaluated against lightning observations. A wide range in the spatial and temporal variability of the simulated flash densities is found, attributed to both types of parameterisations. Some combinations perform well, whereas others are hardly applicable. In addition to resolution dependent rescaling parameters, each combination of lightning and convection schemes requires individual scaling to reproduce the observed flash frequencies. The resulting NOx profiles are inter-compared, however definite conclusions about the most realistic profiles can currently not be drawn.
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