East Asian summer monsoon delivers large abundances of very-short-lived organic chlorine substances to the lower stratosphere.

Deep convection in the Asian summer monsoon is a significant transport process for lifting pollutants from the planetary boundary layer to the tropopause level. This process enables efficient injection into the stratosphere of reactive species such as chlorinated very-short-lived substances (Cl-VSLSs) that deplete ozone. Past studies of convective transport associated with the Asian summer monsoon have focused mostly on the south Asian summer monsoon. Airborne observations reported in this work identify the East Asian summer monsoon convection as an effective transport pathway that carried record-breaking levels of ozone-depleting Cl-VSLSs (mean organic chlorine from these VSLSs ~500 ppt) to the base of the stratosphere. These unique observations show total organic chlorine from VSLSs in the lower stratosphere over the Asian monsoon tropopause to be more than twice that previously reported over the tropical tropopause. Considering the recently observed increase in Cl-VSLS emissions and the ongoing strengthening of the East Asian summer monsoon under global warming, our results highlight that a reevaluation of the contribution of Cl-VSLS injection via the Asian monsoon to the total stratospheric chlorine budget is warranted.

Rapid ozone depletion after humidification of the stratosphere by the Hunga Tonga Eruption.

The eruption of the Hunga Tonga-Hunga Ha'apai volcano on 15 January 2022 offered a good opportunity to explore the early impacts of tropical volcanic eruptions on stratospheric composition. Balloon-borne observations near Réunion Island revealed the unprecedented amount of water vapor injected by the volcano. The enhanced stratospheric humidity, radiative cooling, and expanded aerosol surface area in the volcanic plume created the ideal conditions for swift ozone depletion of 5% in the tropical stratosphere in just 1 week. The decrease in hydrogen chloride by 0.4 parts per million by volume (ppbv) and the increase in chlorine monoxide by 0.4 ppbv provided compelling evidence for chlorine activation within the volcanic plume. This study enhances our understanding of the effect of this unusual volcanic eruption on stratospheric chemistry and provides insights into possible chemistry changes that may occur in a changing climate.

Reanalysis comparisons of upper tropospheric/lower stratospheric jets and multiple tropopauses.

The representation of upper tropospheric/lower stratospheric (UTLS) jet and tropopause characteristics is compared in five modern high-resolution reanalyses for 1980 through 2014. Climatologies of upper tropospheric jet, subvortex jet (the lowermost part of the stratospheric vortex), and multiple tropopause frequency distributions in MERRA (Modern Era Retrospective Analysis for Research and Applications), ERA-I (the ECMWF interim reanalysis), JRA-55 (the Japanese 55-year Reanalysis), and CFSR (the Climate Forecast System Reanalysis) are compared with those in MERRA-2. Differences between alternate products from individual reanalysis systems are assessed; in particular, a comparison of CFSR data on model and pressure levels highlights the importance of vertical grid spacing. Most of the differences in distributions of UTLS jets and multiple tropopauses are consistent with the differences in assimilation model grids and resolution: For example, ERA-I (with coarsest native horizontal resolution) typically shows a significant low bias in upper tropospheric jets with respect to MERRA-2, and JRA-55 a more modest one, while CFSR (with finest native horizontal resolution) shows a high bias with respect to MERRA-2 in both upper tropospheric jets and multiple tropopauses. Vertical temperature structure and grid spacing are especially important for multiple tropopause characterization. Substantial differences between MERRA and MERRA-2 are seen in mid- to high-latitude southern hemisphere winter upper tropospheric jets and multiple tropopauses, and in the upper tropospheric jets associated with tropical circulations during the solstice seasons; some of the largest differences from the other reanalyses are seen in the same times and places. Very good qualitative agreement among the reanalyses is seen between the large scale climatological features in UTLS jet and multiple tropopause distributions. Quantitative differences may, however, have important consequences for transport and variability studies. Our results highlight the importance of considering reanalyses differences in UTLS studies, especially in relation to resolution and model grids; this is particularly critical when using high-resolution reanalyses as an observational reference for evaluating global chemistry climate models.

Midlatitude atmospheric OH response to the most recent 11-y solar cycle.

The hydroxyl radical (OH) plays an important role in middle atmospheric photochemistry, particularly in ozone (O(3)) chemistry. Because it is mainly produced through photolysis and has a short chemical lifetime, OH is expected to show rapid responses to solar forcing [e.g., the 11-y solar cycle (SC)], resulting in variabilities in related middle atmospheric O(3) chemistry. Here, we present an effort to investigate such OH variability using long-term observations (from space and the surface) and model simulations. Ground-based measurements and data from the Microwave Limb Sounder on the National Aeronautics and Space Administration's Aura satellite suggest an ∼7-10% decrease in OH column abundance from solar maximum to solar minimum that is highly correlated with changes in total solar irradiance, solar Mg-II index, and Lyman-α index during SC 23. However, model simulations using a commonly accepted solar UV variability parameterization give much smaller OH variability (∼3%). Although this discrepancy could result partially from the limitations in our current understanding of middle atmospheric chemistry, recently published solar spectral irradiance data from the Solar Radiation and Climate Experiment suggest a solar UV variability that is much larger than previously believed. With a solar forcing derived from the Solar Radiation and Climate Experiment data, modeled OH variability (∼6-7%) agrees much better with observations. Model simulations reveal the detailed chemical mechanisms, suggesting that such OH variability and the corresponding catalytic chemistry may dominate the O(3) SC signal in the upper stratosphere. Continuing measurements through SC 24 are required to understand this OH variability and its impacts on O(3) further.

Unprecedented Arctic ozone loss in 2011.

Chemical ozone destruction occurs over both polar regions in local winter-spring. In the Antarctic, essentially complete removal of lower-stratospheric ozone currently results in an ozone hole every year, whereas in the Arctic, ozone loss is highly variable and has until now been much more limited. Here we demonstrate that chemical ozone destruction over the Arctic in early 2011 was--for the first time in the observational record--comparable to that in the Antarctic ozone hole. Unusually long-lasting cold conditions in the Arctic lower stratosphere led to persistent enhancement in ozone-destroying forms of chlorine and to unprecedented ozone loss, which exceeded 80 per cent over 18-20 kilometres altitude. Our results show that Arctic ozone holes are possible even with temperatures much milder than those in the Antarctic. We cannot at present predict when such severe Arctic ozone depletion may be matched or exceeded.

Constraining the chlorine monoxide (ClO)/chlorine peroxide (ClOOCl) equilibrium constant from Aura Microwave Limb Sounder measurements of nighttime ClO.

The primary ozone loss process in the cold polar lower stratosphere hinges on chlorine monoxide (ClO) and one of its dimers, chlorine peroxide (ClOOCl). Recently, analyses of atmospheric observations have suggested that the equilibrium constant, K(eq), governing the balance between ClOOCl formation and thermal decomposition in darkness is lower than that in the current evaluation of kinetics data. Measurements of ClO at night, when ClOOCl is unaffected by photolysis, provide a useful means of testing quantitative understanding of the ClO/ClOOCl relationship. Here we analyze nighttime ClO measurements from the National Aeronautics and Space Administration Aura Microwave Limb Sounder (MLS) to infer an expression for K(eq). Although the observed temperature dependence of the nighttime ClO is in line with the theoretical ClO/ClOOCl equilibrium relationship, none of the previously published expressions for K(eq) consistently produces ClO abundances that match the MLS observations well under all conditions. Employing a standard expression for K(eq), A x exp(B/T), we constrain the parameter A to currently recommended values and estimate B using a nonlinear weighted least squares analysis of nighttime MLS ClO data. ClO measurements at multiple pressure levels throughout the periods of peak chlorine activation in three Arctic and four Antarctic winters are used to estimate B. Our derived B leads to values of K(eq) that are approximately 1.4 times smaller at stratospherically relevant temperatures than currently recommended, consistent with earlier studies. Our results are in better agreement with the newly updated (2009) kinetics evaluation than with the previous (2006) recommendation.