Anthropogenic greenhouse gas emissions are warming the global climate at an unprecedented rate. Significant emission reductions will be required soon to avoid a rapid temperature rise. As a potential interim measure to avoid extreme temperature increase, it has been suggested that Earth's albedo be increased by artificially enhancing stratospheric sulfate aerosols. We use a 3D chemistry climate model, fed by aerosol size distributions from a zonal mean aerosol model, to simulate continuous injection of 1-10 Mt/a into the lower tropical stratosphere. In contrast to the case for all previous work, the particles are predicted to grow to larger sizes than are observed after volcanic eruptions. The reason is the continuous supply of sulfuric acid and hence freshly formed small aerosol particles, which enhance the formation of large aerosol particles by coagulation and, to a lesser extent, by condensation. Owing to their large size, these particles have a reduced albedo. Furthermore, their sedimentation results in a non-linear relationship between stratospheric aerosol burden and annual injection, leading to a reduction of the targeted cooling. More importantly, the sedimenting particles heat the tropical cold point tropopause and, hence, the stratospheric entry mixing ratio of H 2 O increases. Therefore, geoengineering by means of sulfate aerosols is predicted to accelerate the hydroxyl catalyzed ozone destruction cycles and cause a significant depletion of the ozone layer even though future halogen concentrations will be significantly reduced.

[1] Measurements of BrO suggest that inorganic bromine (Br y ) at and above the tropopause is 4 to 8 ppt greater than assumed in models used in past ozone trend assessment studies. This additional bromine is likely carried to the stratosphere by short-lived biogenic compounds and their decomposition products, including tropospheric BrO. Including this additional bromine in an ozone trend simulation increases the computed ozone depletion over the past $25 years, leading to better agreement between measured and modeled ozone trends. This additional Br y (assumed constant over time) causes more ozone depletion because associated BrO provides a reaction partner for ClO, which increases due to anthropogenic sources. Enhanced Br y causes photochemical loss of ozone below $14 km to change from being controlled by HO x catalytic cycles (primarily HO 2 +O 3 ) to a situation where loss by the BrO+HO 2 cycle is also important. Citation: Salawitch, R. J.,

[1] The large solar storms in October-November 2003 caused solar proton events (SPEs) at the Earth and impacted the middle atmospheric polar cap regions. Although occurring near the end of the maximum of solar cycle 23, the fourth largest period of SPEs measured in the past 40 years happened 28-31 October 2003. The highly energetic protons associated with the SPEs produced ionizations, excitations, dissociations, and dissociative ionizations of the background constituents, which led to the production of odd hydrogen (HO x ) and odd nitrogen (NO y ). NO x (NO + NO 2 ) was observed by the UARS HALOE instrument to increase over 20 ppbv throughout the Southern Hemisphere polar lower mesosphere. The NOAA 16 SBUV/2 instrument measured a short-term ozone depletion of 40% in the Southern Hemisphere polar lower mesosphere, probably a result of the HO x increases. SBUV/2 observations showed ozone depletions of 5-8% in the southern polar upper stratosphere lasting days beyond the events, most likely a result of the NO y enhancements. Longer-term Northern Hemisphere polar total ozone decreases of >0.5% were predicted to last for over 8 months past the events with the Goddard Space Flight Center two-dimensional model. Although the production of NO y constituents is the same in both hemispheres, the NO y constituents have a much larger impact in the northern than the southern polar latitudes because of the seasonal differences between the two hemispheres. These observations and model computations illustrate the substantial impact of solar protons on the polar neutral middle atmosphere.

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Recent analysis suggests that the effectiveness of stratospheric aerosol climate engineering through emission of non‐condensable vapors such as SO2 is limited because the slow conversion to H2SO4 tends to produce aerosol particles that are too large; SO2 injection may be so inefficient that it is difficult to counteract the radiative forcing due to a CO2 doubling. Here we describe an alternate method in which aerosol is formed rapidly in the plume following injection of H2SO4, a condensable vapor, from an aircraft. This method gives better control of particle size and can produce larger radiative forcing with lower sulfur loadings than SO2 injection. Relative to SO2 injection, it may reduce some of the adverse effects of geoengineering such as radiative heating of the lower stratosphere. This method does not, however, alter the fact that such a geoengineered radiative forcing can, at best, only partially compensate for the climate changes produced by CO2.

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.

Abstract. A two-dimensional model of sulfate aerosols has been developed. The model includes the sulfate precursor species H2S, CS2, DMS, OCS, and S02. Microphysical processes simulated are homogeneous nucleation, condensation and evaporation, coagulation, and sedimentation. Tropospheric aerosols are removed by washout processes and by surface deposition. We assume that all aerosols are strictly binary water-sulfuric acid solutions without solid cores. The main source of condensation nuclei for the stratosphere is new particle formation by homogeneous nucleation in the upper tropical troposphere. A signficant finding is that the stratospheric aerosol mass may be strongly influenced by deep convection in the troposphere. This process, which could transport gas-phase sulfate precursors into the upper troposphere and lead to elevated levels of S02 there, could potentially double the stratospheric aerosol mass relative to that due to OCS photooxidation alone. Our model is successful at reproducing the magnitude of stratospheric aerosol loading following the Mount Pinatubo eruption, but the calculated rate of decay of aerosols from the stratosphere is faster than that derived from observations.

Abstract. We report here on the details of the first, in situ, real-time measurements of H-1211 (CBrC1F2) and sulfur hexafluoride (SF6) mixing ratios in the stratosphere up to 20 km. Stratospheric air was analyzed for these gases and others with a new gas chromatograph, flown aboard a National Aeronautics and Space Administration ER-2 aircraft as part of the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft mission conducted in 1994. The mixing ratio of $F6, with its nearly linear increase in the troposphere, was used to estimate the mean age of stratospheric air parcels along the ER-2 flight path. Measurements of H-1211 and mean age estimates were then combined with simultaneous measurements of CFC-11 (CC13F), measurements of brominated compounds in stratospheric whole air samples, and records of tropospheric organic bromine mixing ratios to calculate the dry mixing ratio of total bromine in the lower stratosphere and its partitioning between organic and inorganic forms. We estimate that the organic bromine-containing species were almost completely photolyzed to inorganic species in the oldest air parcels sampled. Our results for inorganic bromine are consistent with those obtained from a photochemical, steady state model for stratospheric air parcels with CFC-11 mixing ratios greater than 150 ppt. For stratospheric air parcels with CFC-11 mixing ratios less than 50 ppt (mean age >5 years) we calculate inorganic bromine mixing ratios that are approximately 20% less than the photochemical, steady state model. There is a 20% reduction in calculated ozone loss resulting from bromine chemistry in old air relative to some previous estimates as a result of the lower bromine