Interest in stratospheric aerosol and its role in climate have increased over the last decade due to the observed increase in stratospheric aerosol since 2000 and the potential for changes in the sulfur cycle induced by climate change. This review provides an overview about the advances in stratospheric aerosol research since the last comprehensive assessment of stratospheric aerosol was published in 2006. A crucial development since 2006 is the substantial improvement in the agreement between in situ and space-based inferences of stratospheric aerosol properties during volcanically quiescent periods. Furthermore, new measurement systems and techniques, both in situ and space based, have been developed for measuring physical aerosol properties with greater accuracy and for characterizing aerosol composition. However, these changes induce challenges to constructing a long-term stratospheric aerosol climatology. Currently, changes in stratospheric aerosol levels less than 20% cannot be confidently quantified. The volcanic signals tend to mask any nonvolcanically driven change, making them difficult to understand. While the role of carbonyl sulfide as a substantial and relatively constant source of stratospheric sulfur has been confirmed by new observations and model simulations, large uncertainties remain with respect to the contribution from anthropogenic sulfur dioxide emissions. New evidence has been provided that stratospheric aerosol can also contain small amounts of nonsulfate matter such as black carbon and organics. Chemistry-climate models have substantially increased in quantity and sophistication. In many models the implementation of stratospheric aerosol processes is coupled to radiation and/or stratospheric chemistry modules to account for relevant feedback processes.

[1] In June 2009 the Sarychev volcano located in the Kuril Islands to the northeast of Japan erupted explosively, injecting ash and an estimated 1.2 ± 0.2 Tg of sulfur dioxide into the upper troposphere and lower stratosphere, making it arguably one of the 10 largest stratospheric injections in the last 50 years. During the period immediately after the eruption, we show that the sulfur dioxide (SO 2 ) cloud was clearly detected by retrievals developed for the Infrared Atmospheric Sounding Interferometer (IASI) satellite instrument and that the resultant stratospheric sulfate aerosol was detected by the Optical Spectrograph and Infrared Imaging System (OSIRIS) limb sounder and CALIPSO lidar. Additional surface-based instrumentation allows assessment of the impact of the eruption on the stratospheric aerosol optical depth. We use a nudged version of the HadGEM2 climate model to investigate how well this state-of-the-science climate model can replicate the distributions of SO 2 and sulfate aerosol. The model simulations and OSIRIS measurements suggest that in the Northern Hemisphere the stratospheric aerosol optical depth was enhanced by around a factor of 3 (0.01 at 550 nm), with resultant impacts upon the radiation budget. The simulations indicate that, in the Northern Hemisphere for July 2009, the magnitude of the mean radiative impact from the volcanic aerosols is more than 60% of the direct radiative forcing of all anthropogenic aerosols put together. While the cooling induced by the eruption will likely not be detectable in the observational record, the combination of modeling and measurements would provide an ideal framework for simulating future larger volcanic eruptions.Citation: Haywood, J. M., et al. (2010), Observations of the eruption of the Sarychev volcano and simulations using the HadGEM2 climate model,

Dissociation of ozone in the Chappuis bands has been used as an O atom source to study isotope effects occurring in the O(3P)+O2(3∑g) recombination reaction. The ozone produced was found to be enriched in both of its heavy isotopes. The pressure dependence (5–1000 torr) and temperature dependence (127–360 K) of this isotope effect have been investigated. The enrichment is approximately constant from 5 torr to 100 torr and decreases at higher pressures. It increases with temperature, with 50O3 showing a slightly faster rate of increase than 49O3. The results of this experiment have clearly isolated the source of the isotope effect to the gas phase O(3P) + O2(3∑g) recombination reaction. For comparison, we also present isotope ratios of ozone formed in an electric discharge. None of the results, however, have shown the large enhancement of 40% or more in mass 50 observed in some stratospheric measurements.

Understanding the cooling effect of recent volcanoes is of particular interest in the context of the post-2000 slowing of the rate of global warming. Satellite observations of aerosol optical depth above 15 km have demonstrated that small-magnitude volcanic eruptions substantially perturb incoming solar radiation. Here we use lidar, Aerosol Robotic Network, and balloon-borne observations to provide evidence that currently available satellite databases neglect substantial amounts of volcanic aerosol between the tropopause and 15 km at middle to high latitudes and therefore underestimate total radiative forcing resulting from the recent eruptions. Incorporating these estimates into a simple climate model, we determine the global volcanic aerosol forcing since 2000 to be À0.19 ± 0.09 Wm À2 . This translates into an estimated global cooling of 0.05 to 0.12°C. We conclude that recent volcanic events are responsible for more post-2000 cooling than is implied by satellite databases that neglect volcanic aerosol effects below 15 km.

The stratospheric aerosol layer has been monitored with lidars at Mauna Loa Observatory in Hawaii and Boulder in Colorado since 1975 and 2000, respectively. Following the Pinatubo volcanic eruption in June 1991, the global stratosphere has not been perturbed by a major volcanic eruption providing an unprecedented opportunity to study the background aerosol. Since about 2000, an increase of 4–7% per year in the aerosol backscatter in the altitude range 20–30 km has been detected at both Mauna Loa and Boulder. This increase is superimposed on a seasonal cycle with a winter maximum that is modulated by the quasi‐biennial oscillation (QBO) in tropical winds. Of the three major causes for a stratospheric aerosol increase: volcanic emissions to the stratosphere, increased tropical upwelling, and an increase in anthropogenic sulfur gas emissions in the troposphere, it appears that a large increase in coal burning since 2002, mainly in China, is the likely source of sulfur dioxide that ultimately ends up as the sulfate aerosol responsible for the increased backscatter from the stratospheric aerosol layer. The results are consistent with 0.6–0.8% of tropospheric sulfur entering the stratosphere.

[1] Water vapor in the subtropical troposphere plays an important role in the radiative balance, the distribution of precipitation, and the chemistry of the Earth's atmosphere. Measurements of the water vapor mixing ratio paired with stable isotope ratios provide unique information on transport processes and moisture sources that is not available with mixing ratio data alone. Measurements of the D/H isotope ratio of water vapor from Mauna Loa Observatory over 4 weeks in October-November 2008 were used to identify components of the regional hydrological cycle. A mixing model exploits the isotope information to identify water fluxes from time series data. Mixing is associated with exchange between marine boundary layer air and tropospheric air on diurnal time scales and between different tropospheric air masses with characteristics that evolve on the synoptic time scale. Diurnal variations are associated with upslope flow and the transition from nighttime air above the marine trade inversion to marine boundary layer air during daytime. During easterly trade wind conditions, growth and decay of the boundary layer are largely conservative in a regional context but contribute ∼12% of the nighttime water vapor at Mauna Loa. Tropospheric moisture is associated with convective outflow and exchange with drier air originating from higher latitude or higher altitude. During the passage of a moist filament, boundary layer exchange is enhanced. Isotopic data reflect the combination of processes that control the water balance, which highlights the utility for baseline measurements of water vapor isotopologues in monitoring the response of the hydrological cycle to climate change. Citation: Noone, D., et al. (2011), Properties of air mass mixing and humidity in the subtropics from measurements of the D/H isotope ratio of water vapor at the Mauna Loa Observatory,

[1] Here we present extensive observations of stratospheric and upper tropospheric water vapor using the balloon-borne Cryogenic Frost point Hygrometer (CFH) in support of the Aura Microwave Limb Sounder (MLS) satellite instrument. Coincident measurements were used for the validation of MLS version 1.5 and for a limited validation of MLS version 2.2 water vapor. The sensitivity of MLS is on average 30% lower than that of CFH, which is fully compensated by a constant offset at stratospheric levels but only partially compensated at tropospheric levels, leading to an upper tropospheric dry bias. The sensitivity of MLS observations may be adjusted using the correlation parameters provided here. For version 1.5 stratospheric observations at pressures of 68 hPa and smaller MLS retrievals and CFH in situ observations agree on average to within 2.3% ± 11.8%. At 100 hPa the agreement is to within 6.4% ± 22% and at upper tropospheric pressures to within 23% ± 37%. In the tropical stratosphere during the boreal winter the agreement is not as good. The ''tape recorder'' amplitude in MLS observations depends on the vertical profile of water vapor mixing ratio and shows a significant interannual variation. The agreement between stratospheric observations by MLS version 2.2 and CFH is comparable to the agreement using MLS version 1.5. The variability in the difference between observations by MLS version 2.2 and CFH at tropospheric levels is significantly reduced, but a tropospheric dry bias and a reduced sensitivity remain in this version. In the validation data set a dry bias at 177.8 hPa of À24.1% ± 16.0% is statistically significant.

Australian wildfires burning from December 2019 to January 2020 injected approximately 0.9 Tg of smoke into the stratosphere; this is the largest amount observed in the satellite era. A comparison of numerical simulations to satellite observations of the plume rise suggests that the smoke mass contained 2.5% black carbon. Model calculations project a 1 K warming in the stratosphere of the Southern Hemisphere midlatitudes for more than 6 months following the injection of black‐carbon containing smoke. The 2020 average global mean clear sky effective radiative forcing at top of atmosphere is estimated to be −0.03 W m−2 with a surface value of −0.32 W m−2. Assuming that smoke particles coat with sulfuric acid in the stratosphere and have similar heterogeneous reaction rates as sulfate aerosol, we estimate a smoke‐induced chemical decrease in total column ozone of 10–20 Dobson units from August to December in mid‐high southern latitudes.