The global atmospheric sulfur budget and its emission dependence have been investigated using the coupled aerosol-chemistry-climate model SOCOL-AER. The aerosol module comprises gaseous and aqueous sulfur chemistry and comprehensive microphysics. The particle distribution is resolved by 40 size bins spanning radii from 0.39 nm to 3.2 μm, including size-dependent particle composition. Aerosol radiative properties required by the climate model are calculated online from the aerosol module. The model successfully reproduces main features of stratospheric aerosols under nonvolcanic conditions, including aerosol extinctions compared to Stratospheric Aerosol and Gas Experiment II (SAGE II) and Halogen Occultation Experiment, and size distributions compared to in situ measurements. The calculated stratospheric aerosol burden is 109 Gg of sulfur, matching the SAGE II-based estimate (112 Gg). In terms of fluxes through the tropopause, the stratospheric aerosol layer is due to about 43% primary tropospheric aerosol, 28% SO 2 , 23% carbonyl sulfide (OCS), 4% H 2 S, and 2% dimethyl sulfide (DMS). Turning off emissions of the short-lived species SO 2 , H 2 S, and DMS shows that OCS alone still establishes about 56% of the original stratospheric aerosol burden. Further sensitivity simulations reveal that anticipated increases in anthropogenic SO 2 emissions in China and India have a larger influence on stratospheric aerosols than the same increase in Western Europe or the U.S., due to deep convection in the western Pacific region. However, even a doubling of Chinese and Indian emissions is predicted to increase the stratospheric background aerosol burden only by 9%. In contrast, small to moderate volcanic eruptions, such as that of Nabro in 2011, may easily double the stratospheric aerosol loading.

We investigate the effects of a recently proposed 21st century Dalton minimum like decline of solar activity on the evolution of Earth's climate and ozone layer. Three sets of two member ensemble simulations, radiatively forced by a midlevel emission scenario (Intergovernmental Panel on Climate Change RCP4.5), are performed with the atmosphere‐ocean chemistry‐climate model AOCCM SOCOL3‐MPIOM, one with constant solar activity, the other two with reduced solar activity and different strength of the solar irradiance forcing. A future grand solar minimum will reduce the global mean surface warming of 2 K between 1986–2005 and 2081–2100 by 0.2 to 0.3 K. Furthermore, the decrease in solar UV radiation leads to a significant delay of stratospheric ozone recovery by 10 years and longer. Therefore, the effects of a solar activity minimum, should it occur, may interfere with international efforts for the protection of global climate and the ozone layer.

Abstract. The aim of this work is to elucidate the impact of changes in solar irradiance and energetic particles versus volcanic eruptions on tropospheric global climate during the Dalton Minimum (DM, AD 1780–1840). Separate variations in the (i) solar irradiance in the UV-C with wavelengths λ < 250 nm, (ii) irradiance at wavelengths λ > 250 nm, (iii) in energetic particle spectrum, and (iv) volcanic aerosol forcing were analyzed separately, and (v) in combination, by means of small ensemble calculations using a coupled atmosphere–ocean chemistry–climate model. Global and hemispheric mean surface temperatures show a significant dependence on solar irradiance at λ > 250 nm. Also, powerful volcanic eruptions in 1809, 1815, 1831 and 1835 significantly decreased global mean temperature by up to 0.5 K for 2–3 years after the eruption. However, while the volcanic effect is clearly discernible in the Southern Hemispheric mean temperature, it is less significant in the Northern Hemisphere, partly because the two largest volcanic eruptions occurred in the SH tropics and during seasons when the aerosols were mainly transported southward, partly because of the higher northern internal variability. In the simulation including all forcings, temperatures are in reasonable agreement with the tree ring-based temperature anomalies of the Northern Hemisphere. Interestingly, the model suggests that solar irradiance changes at λ < 250 nm and in energetic particle spectra have only an insignificant impact on the climate during the Dalton Minimum. This downscales the importance of top–down processes (stemming from changes at λ < 250 nm) relative to bottom–up processes (from λ > 250 nm). Reduction of irradiance at λ > 250 nm leads to a significant (up to 2%) decrease in the ocean heat content (OHC) between 0 and 300 m in depth, whereas the changes in irradiance at λ < 250 nm or in energetic particles have virtually no effect. Also, volcanic aerosol yields a very strong response, reducing the OHC of the upper ocean by up to 1.5%. In the simulation with all forcings, the OHC of the uppermost levels recovers after 8–15 years after volcanic eruption, while the solar signal and the different volcanic eruptions dominate the OHC changes in the deeper ocean and prevent its recovery during the DM. Finally, the simulations suggest that the volcanic eruptions during the DM had a significant impact on the precipitation patterns caused by a widening of the Hadley cell and a shift in the intertropical convergence zone.

Abstract. The newly developed atmosphere-oceanchemistry-climate model SOCOL-MPIOM is presented by demonstrating the influence of chemistry-climate interactions on the climate state and the variability. Therefore, we compare pre-industrial control simulations with (CHEM) and without (NOCHEM) interactive chemistry. In general, the influence of the chemistry on the mean state and the variability is small and mainly restricted to the stratosphere and mesosphere. The atmospheric dynamics mainly differ in polar regions, with slightly stronger polar vortices in the austral and boreal winter, respectively. The strengthening of the vortex is related to larger stratospheric temperature gradients, which are attributed to a parameterisation of the absorption of ozone and oxygen in different wavelength intervals, which is considered in the version with interactive chemistry only. A second reason for the temperature differences between CHEM and NOCHEM is related to diurnal variations in the ozone concentrations in the higher atmosphere, which are missing in NOCHEM. Furthermore, stratospheric water vapour concentrations substantially differ between the two experiments, but their effect on temperature is small. In both setups, the simulated intensity and variability of the northern polar vortex is inside the range of present-day observations. Additionally, the performance of SOCOL-MPIOM under changing external forcings is assessed for the period 1600-2000 using an ensemble of simulations. In the industrial period from 1850 onward SOCOL-MPIOM overestimates the global mean surface air temperature increase in comparison to observational data sets. Sensitivity simulations show that this overestimation can be attributed to a combination of factors: the solar forcing reconstruction, the simulated ozone changes, and incomplete aerosol effects and land use changes.