Description: During the summer monsoon, the western tropical Indian Ocean is predicted to be a hot spot for dimethylsulfide emissions, the major marine sulfur source to the atmosphere, and an important aerosol precursor. Other aerosol relevant fluxes, such as isoprene and sea spray, should also be enhanced, due to the steady strong winds during the monsoon. Marine air masses dominate the area during the summer monsoon, excluding the influence of continentally derived pollutants. During the SO234-2/235 cruise in the western tropical Indian Ocean from July to August 2014, directly measured eddy covariance DMS fluxes confirm that the area is a large source of sulfur to the atmosphere (cruise average 9.1 μmol m−2 d−1). The directly measured fluxes, as well as computed isoprene and sea spray fluxes, were combined with FLEXPART backward and forward trajectories to track the emissions in space and time. The fluxes show a significant positive correlation with aerosol data from the Terra and Suomi-NPP satellites, indicating a local influence of marine emissions on atmospheric aerosol numbers.

Description: Halogen- and sulfur-containing compounds are supersaturated in the surface ocean, which results in their emission to the atmosphere. These compounds can be transported to the stratosphere, where they impact ozone, the background aerosol layer, and climate. In this study we calculate the seasonal and interannual variability of transport from the West Indian Ocean (WIO) surface to the stratosphere for 2000-2016 with the Lagrangian transport model FLEXPART using ERA-Interim meteorological fields. We investigate the transport relevant for very short lived substances (VSLS) with tropospheric lifetimes corresponding to dimethylsulfide (1 day), methyl iodide (CH3I, 3.5 days), bromoform (CHBr3, 17 days), and dibromomethane (CH2Br2, 150 days). The stratospheric source gas injection of VSLS tracers from the WIO shows a distinct annual cycle associated with the Asian monsoon. Over the 16-year time series, a slight increase in source gas injection from the WIO to the stratosphere is found for all VSLS tracers and during all seasons. The interannual variability shows a relationship with sea surface temperatures in the WIO as well as the El Niño-Southern Oscillation. During boreal spring of El Niño, enhanced stratospheric injection of VSLS from the tropical WIO is caused by positive sea surface temperature anomalies and enhanced vertical uplift above the WIO. During boreal fall of La Niña, strong injection is related to enhanced atmospheric upward motion over the East Indian Ocean and a prolonged Indian summer monsoon season. Related physical mechanisms and uncertainties are discussed in this study

Description: Reconstructions of the atmospheric sulfate aerosol burdens resulting from past volcanic eruptions are based on ice core-derived estimates of volcanic sulfate deposition and the assumption that the two quantities are directly proportional. We test this assumption within simulations of tropical volcanic stratospheric sulfur injections with the MAECHAM5-HAM aerosol-climate model. An ensemble of 70 simulations is analyzed, with SO2 injections ranging from 8.5 to 700 Tg, with eruptions in January and July. Modeled sulfate deposition flux to Antarctica shows excellent spatial correlation with ice core-derived estimates for Pinatubo and Tambora, although the comparison suggests the modeled flux to the ice sheets is 4–5 times too large. We find that Greenland and Antarctic deposition efficiencies (the ratio of sulfate flux to each ice sheet to the maximum hemispheric stratospheric sulfate aerosol burden) vary as a function of the magnitude and season of stratospheric sulfur injection. Changes in simulated sulfate deposition for large SO2 injections are connected to increases in aerosol particle size, which impact aerosol sedimentation velocity and radiative properties, the latter leading to strong dynamical changes including strengthening of the winter polar vortices, which inhibits the transport of stratospheric aerosols to high latitudes. The resulting relationship between Antarctic and Greenland volcanic sulfate deposition is nonlinear for very large eruptions, with significantly less sulfate deposition to Antarctica than to Greenland. These model results suggest that variability of deposition efficiency may be an important consideration in the interpretation of ice core sulfate signals for eruptions of Tambora-magnitude and larger.

Description: A comprehensive quality assessment of the ozone products from 18 limb-viewing satellite instruments is provided by means of a detailed inter-comparison. The ozone climatologies in the form of monthly zonal mean time series covering the upper troposphere to lower mesosphere are obtained from LIMS, SAGE I, SAGE II, UARS-MLS, HALOE, POAM II, POAM III, SMR, OSIRIS, SAGE III, MIPAS, GOMOS, SCIAMACHY, ACE-FTS, ACE-MAESTRO, Aura-MLS, HIRDLS, and SMILES within 1978-2010. The inter-comparisons focus on mean biases based on monthly and annual zonal mean fields, on inter-annual variability and on seasonal cycles. Additionally, the physical consistency of the data sets is tested through diagnostics of the quasi-biennial oscillation and the Antarctic ozone hole. The comprehensive evaluations reveal that the uncertainty in our knowledge of the atmospheric ozone mean state is smallest in the tropical middle stratosphere and in the midlatitude lower/middle stratosphere, where we find a 1σ multi-instrument spread of less than ±5%. While the overall agreement among the climatological data sets is very good for large parts of the stratosphere, individual discrepancies have been identified including unrealistic month-to-month fluctuations, large biases in particular atmospheric regions, or inconsistencies in the seasonal cycle. Notable differences between the data sets exist in the tropical lower stratosphere and at high latitudes, with a multi-instrument spread of ±30% at the tropical tropopause and ±15% at polar latitudes. In particular, large relative differences are identified in the Antarctic polar cap during the time of the ozone hole, with a spread between the monthly zonal mean fields of ±50%. Differences between the climatological data sets are suggested to be partially related to inter-instrumental differences in vertical resolution and geographical sampling. The evaluations as a whole provide guidance on what data sets are the most reliable for applications such as studies of ozone variability, model-measurement comparisons and detection of long-term trends. A detailed comparison versus SAGE II data is presented, which can help identify suitable candidates for long-term data merging studies.

Description: Monthly zonal mean climatologies of atmospheric measurements from satellite instruments can have biases due to the non-uniform sampling of the atmosphere by the instruments. We characterize potential sampling biases in stratospheric trace gas climatologies of the Stratospheric Processes and their Role in Climate (SPARC) Data Initiative using chemical fields from a chemistry climate model simulation and sampling patterns from 16 satellite-borne instruments. The exercise is performed for the long-lived stratospheric trace gases O3 and H2O. Monthly sample biases for O3 exceed 10% for many instruments in the high latitude stratosphere and in the upper troposphere/lower stratosphere, while annual mean sampling biases reach values of up to 20% in the same regions for some instruments. Sampling biases for H2O are generally smaller than for O3, although still notable in the upper troposphere/lower stratosphere and Southern Hemisphere high latitudes. The most important mechanism leading to monthly sampling bias is the non-uniform temporal sampling of many instruments, i.e., the fact that for many instruments, monthly means are produced from measurements which span less than the full month in question. Similarly, annual mean sampling biases are well explained by non-uniformity in the month-to-month sampling by different instruments. Non-uniform sampling in latitude and longitude are shown to also lead to non-negligible sampling biases, which are most relevant for climatologies which are otherwise free of sampling biases due to non-uniform temporal sampling.

Description: The current generation of Earth system models that participate in the Coupled Model Intercomparison Project phase 5 (CMIP5) does not, on average, produce a strengthened Northern Hemisphere (NH) polar vortex after large tropical volcanic eruptions as suggested by observational records. Here we investigate the impact of volcanic eruptions on the NH winter stratosphere with an ensemble of 20 model simulations of the Max Planck Institute Earth system model. We compare the dynamical impact in simulations of the very large 1815 Tambora eruption with the averaged dynamical response to the two largest eruptions of the CMIP5 historical simulations (the 1883 Krakatau and the 1991 Pinatubo eruptions). We find that for both the Tambora and the averaged Krakatau-Pinatubo eruptions the radiative perturbation only weakly affects the polar vortex directly. The position of the maximum temperature anomaly gradient is located at approximately 30°N, where we obtain significant westerly zonal wind anomalies between 10hPa and 30hPa. Under the very strong forcing of the Tambora eruption, the NH polar vortex is significantly strengthened because the subtropical westerly wind anomalies are sufficiently strong to robustly alter the propagation of planetary waves. The average response to the eruptions of Krakatau and Pinatubo reveals a slight strengthening of the polar vortex, but individual ensemble members differ substantially, indicating that internal variability plays a dominant role. For the Tambora eruption the ensemble variability of the zonal mean temperature and zonal wind anomalies during midwinter and late winter is significantly reduced compared to the volcanically unperturbed period.

Description: The Los Chocoyos (14.6°N, 91.2°W) supereruption happened ∼75,000 years ago in Guatemala and was one of the largest eruptions of the past 100,000 years. It emitted enormous amounts of sulfur, chlorine, and bromine, with multi‐decadal consequences for the global climate and environment. Here, we simulate the impact of a Los Chocoyos‐like eruption on the quasi‐biennial oscillation (QBO), an oscillation of zonal winds in the tropical stratosphere, with a comprehensive aerosol chemistry Earth System Model. We find a ∼10‐year disruption of the QBO starting 4 months post eruption, with anomalous easterly winds lasting ∼5 years, followed by westerlies, before returning to QBO conditions with a slightly prolonged periodicity. Volcanic aerosol heating and ozone depletion cooling leads to the QBO disruption and anomalous wind regimes through radiative changes and wave‐mean flow interactions. Different model ensembles, volcanic forcing scenarios and results of a second model back up the robustness of our results.