Aerosol microphysics simulations of the Mt.~Pinatubo eruption with the UM-UKCA composition-climate model

We use a stratosphere–troposphere composition–climate model with interactive sulfur chemistry and aerosol microphysics, to investigate the effect of the 1991 Mount Pinatubo eruption on stratospheric aerosol properties. Satellite measurements indicate that shortly after the eruption, between 14 and 23 Tg of SO2 (7 to 11.5 Tg of sulfur) was present in the tropical stratosphere. Best estimates of the peak global stratospheric aerosol burden are in the range 19 to 26 Tg, or 3.7 to 6.7 Tg of sulfur assuming a composition of between 59 and 77 % H2SO4. In light of this large uncertainty range, we performed two main simulations with 10 and 20 Tg of SO2 injected into the tropical lower stratosphere. Simulated stratospheric aerosol properties through the 1991 to 1995 period are compared against a range of available satellite and in situ measurements. Stratospheric aerosol optical depth (sAOD) and effective radius from both simulations show good qualitative agreement with the observations, with the timing of peak sAOD and decay timescale matching well with the observations in the tropics and mid-latitudes. However, injecting 20 Tg gives a factor of 2 too high stratospheric aerosol mass burden compared to the satellite data, with consequent strong high biases in simulated sAOD and surface area density, with the 10 Tg injection in much better agreement. Our model cannot explain the large fraction of the injected sulfur that the satellite-derived SO2 and aerosol burdens indicate was removed within the first few months after the eruption. We suggest that either there is an additional alternative loss pathway for the SO2 not included in our model (e.g. via accommodation into ash or ice in the volcanic cloud) or that a larger proportion of the injected sulfur was removed via cross-tropopause transport than in our simulations. We also critically evaluate the simulated evolution of the particle size distribution, comparing in detail to balloon-borne optical particle counter (OPC) measurements from Laramie, Wyoming, USA (41° N). Overall, the model captures remarkably well the complex variations in particle concentration profiles across the different OPC size channels. However, for the 19 to 27 km injection height-range used here, both runs have a modest high bias in the lowermost stratosphere for the finest particles (radii less than 250 nm), and the decay timescale is longer in the model for these particles, with a much later return to background conditions. Also, whereas the 10 Tg run compared best to the satellite measurements, a significant low bias is apparent in the coarser size channels in the volcanically perturbed lower stratosphere. Overall, our results suggest that, with appropriate calibration, aerosol microphysics models are capable of capturing the observed variation in particle size distribution in the stratosphere across both volcanically perturbed and quiescent conditions. Furthermore, additional sensitivity simulations suggest that predictions with the models are robust to uncertainties in sub-grid particle formation and nucleation rates in the stratosphere

Validation of ACE-FTS version 3.5 NOy species profiles using correlative satellite measurements

The ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) instrument on the Canadian SCISAT satellite, which has been in operation for over 12 years, has the capability of deriving stratospheric profiles of many of the NO$_{γ}$ (N+ NO+ NO$_{2}$+ NO$_{3}$+ 2×N$_{2}$O$_{5}$+HNO$_{3}$+HNO$_{4}$+ClONO$_{2}$+BrONO$_{2}$) species. Version 2.2 of ACE-FTS NO, NO$_{2}$, HNO$_{3}$, N$_{2}$O$_{5}$, and ClONO$_{2}$ has previously been validated, and this study compares the most recent version (v3.5) of these five ACE-FTS products to spatially and temporally coincident measurements from other satellite instruments – GOMOS, HALOE, MAESTRO, MIPAS, MLS, OSIRIS, POAM III, SAGE III, SCIAMACHY, SMILES, and SMR. For each ACE-FTS measurement, a photochemical box model was used to simulate the diurnal variations of the NO$_{γ}$ species and the ACE-FTS measurements were scaled to the local times of the coincident measurements. The comparisons for all five species show good agreement with correlative satellite measurements. For NO in the altitude range of 25–50 km, ACE-FTS typically agrees with correlative data to within -10 %. Instrumentaveraged mean relative differences are approximately 10% at 30–40 km for NO$_{2}$, within ±7% at 8–30 km for HNO$_{3}$, better than -7% at 21–34 km for local morning N$_{2}$O$_{5}$, and better than -8% at 21–34 km for ClONO$_{2}$. Where possible, the variations in the mean differences due to changes in the comparison local time and latitude are also discussed

The SPARC water vapour assessment II: Profile-to-profile comparisons of stratospheric and lower mesospheric water vapour data sets obtained from satellites

This work is distributed under the Creative Commons Attribution 4.0 License. Within the framework of the second SPARC (Stratosphere-troposphere Processes And their Role in Climate) water vapour assessment (WAVAS-II), profile-to-profile comparisons of stratospheric and lower mesospheric water vapour were performed by considering 33 data sets derived from satellite observations of 15 different instruments. These comparisons aimed to provide a picture of the typical biases and drifts in the observational database and to identify data-set-specific problems. The observational database typically exhibits the largest biases below 70 hPa, both in absolute and relative terms. The smallest biases are often found between 50 and 5 hPa. Typically, they range from 0.25 to 0.5 ppmv (5 % to 10 %) in this altitude region, based on the 50 % percentile over the different comparison results. Higher up, the biases increase with altitude overall but this general behaviour is accompanied by considerable variations. Characteristic values vary between 0.3 and 1 ppmv (4 % to 20 %). Obvious data-set-specific bias issues are found for a number of data sets. In our work we performed a drift analysis for data sets overlapping for a period of at least 36 months. This assessment shows a wide range of drifts among the different data sets that are statistically significant at the 2σ uncertainty level. In general, the smallest drifts are found in the altitude range between about 30 and 10 hPa. Histograms considering results from all altitudes indicate the largest occurrence for drifts between 0.05 and 0.3 ppmv decade-1. Comparisons of our drift estimates to those derived from comparisons of zonal mean time series only exhibit statistically significant differences in slightly more than 3 % of the comparisons. Hence, drift estimates from profile-to-profile and zonal mean time series comparisons are largely interchangeable. As for the biases, a number of data sets exhibit prominent drift issues. In our analyses we found that the large number of MIPAS data sets included in the assessment affects our general results as well as the bias summaries we provide for the individual data sets. This is because these data sets exhibit a relative similarity with respect to the remaining data sets, despite the fact that they are based on different measurement modes and different processors implementing different retrieval choices. Because of that, we have by default considered an aggregation of the comparison results obtained from MIPAS data sets. Results without this aggregation are provided on multiple occasions to characterise the effects due to the numerous MIPAS data sets. Among other effects, they cause a reduction of the typical biases in the observational database

Stratospheric effects of energetic particle precipitation in 2003-2004

Upper stratospheric enhancements in NOx (NO and NO2) were observed at high northern latitudes from March through at least July of 2004. Multi-satellite data analysis is used to examine the temporal evolution of the enhancements, to place them in historical context, and to investigate their origin. The enhancements were a factor of 4 higher than nominal at some locations, and are unprecedented in the northern hemisphere since at least 1985. They were accompanied by reductions in O-3 of more than 60% in some cases. The analysis suggests that energetic particle precipitation led to substantial NOx production in the upper atmosphere beginning with the remarkable solar storms in late October 2003 and possibly persisting through January. Downward transport of the excess NOx, facilitated by unique meteorological conditions in 2004 that led to an unusually strong upper stratospheric vortex from late January through March, caused the enhancements

Validation of ACE-FTS version 3.5 NO<i>y</i> species profiles using correlative satellite measurements

The ACE-FTS (Atmospheric Chemistry Experiment-Fourier Transform Spectrometer) instrument on the Canadian SCISAT satellite, which has been in operation for over 12 years, has the capability of deriving stratospheric profiles of many of the NO (N+NO+NO+NO+2×NO+HNO+HNO+ClONO+BrONO) species. Version 2.2 of ACE-FTS NO, NO, HNO, NO, and ClONO has previously been validated, and this study compares the most recent version (v3.5) of these five ACE-FTS products to spatially and temporally coincident measurements from other satellite instruments-GOMOS, HALOE, MAESTRO, MIPAS, MLS, OSIRIS, POAM III, SAGE III, SCIAMACHY, SMILES, and SMR. For each ACE-FTS measurement, a photochemical box model was used to simulate the diurnal variations of the NOy species and the ACE-FTS measurements were scaled to the local times of the coincident measurements. The comparisons for all five species show good agreement with correlative satellite measurements. For NO in the altitude range of 25-50 km, ACE-FTS typically agrees with correlative data to within .10 %. Instrumentaveraged mean relative differences are approximately.10% at 30-40 km for NO, within-7% at 8-30 km for HNO, better than.7% at 21-34 km for local morning NO, and better than.8% at 21-34 km for ClONO. Where possible, the variations in the mean differences due to changes in the comparison local time and latitude are also discussed.©2016 Author(s).The Atmospheric Chemistry Experiment is a Canadian-led mission mainly supported by the CSA. Odin is a Swedish-led satellite project funded jointly by Sweden (Swedish National Space Board), Canada (CSA), France (Centre National d'Etudes Spatiales), and Finland (Tekes), with support by the third-party mission programme of the European Space Agency (ESA). Coauthor CER was funded by NASA grant NNX14AH54G. The University of Bremen team was funded in parts by the DLR Space Agency (Germany) and by the University and State of Bremen.Peer Reviewe

Long-term evolution of upper stratospheric ozone at selected stations of the Network for the Detection of Stratospheric Change (NDSC)

The long-term evolution of upper stratospheric ozone has been recorded by lidars and microwave radiometers within the ground-based Network for the Detection of Stratospheric Change (NDSC), and by the space-borne Solar Backscatter Ultra-Violet instruments (SBUV), Stratospheric Aerosol and Gas Experiment (SAGE), and Halogen Occultation Experiment (HALOE). Climatological mean differences between these instruments are typically smaller than 5% between 25 and 50 km. Ozone anomaly time series from all instruments, averaged from 35 to 45 km altitude, track each other very well and typically agree within 3 to 5%. SBUV seems to have a slight positive drift against the other instruments. The corresponding 1979 to 1999 period from a transient simulation by the fully coupled MAECHAM4-CHEM chemistry climate model reproduces many features of the observed anomalies. However, in the upper stratosphere the model shows too low ozone values and too negative ozone trends, probably due to an underestimation of methane and a consequent overestimation of ClO. The combination of all observational data sets provides a very consistent picture, with a long-term stability of 2% or better. Upper stratospheric ozone shows three main features: (1) a decline by 10 to 15% since 1980, due to chemical destruction by chlorine; (2) two to three year fluctuations by 5 to 10%, due to the Quasi-Biennial Oscillation (QBO); (3) an 11-year oscillation by about 5%, due to the 11-year solar cycle. The 1979 to 1997 ozone trends are larger at the southern mid-latitude station Lauder (45°S), reaching ?8%/decade, compared to only about ?6%/decade at Table Mountain (35°N), Haute Provence/Bordeaux (?45°N), and Hohenpeissenberg/Bern(?47°N). At Lauder, Hawaii (20°N), Table Mountain, and Haute Provence, ozone residuals after subtraction of QBO- and solar cycle effects have levelled off in recent years, or are even increasing. Assuming a turning point in January 1997, the change of trend is largest at southern mid-latitude Lauder, +11%/decade, compared to +7%/decade at northern mid-latitudes. This points to a beginning recovery of upper stratospheric ozone. However, chlorine levels are still very high and ozone will remain vulnerable. At this point the most northerly mid-latitude station, Hohenpeissenberg/Bern differs from the other stations, and shows much less clear evidence for a beginning recovery, with a change of trend in 1997 by only +3%/decade. In fact, record low upper stratospheric ozone values were observed at Hohenpeissenberg/Bern, and to a lesser degree at Table Mountain and Haute Provence, in the winters 2003/2004 and 2004/2005