Seasonal persistence of midlatitude total ozone anomalies

Temporal autocorrelations of monthly mean total ozone anomalies over the 35–60°S and 35–60°N latitude bands reveal that anomalies established in the wintertime midlatitude ozone buildup persist (with photochemical decay) until the end of the following autumn, and then are rapidly erased once the next winter's buildup begins. The photochemical decay rate is found to be identical between the two hemispheres. High predictability of ozone through late summer exists based on the late-spring values. In the northern hemisphere, extending the 1979–2001 springtime ozone trend to other months through regression based on the seasonal persistence of anomalies captures the seasonality of the ozone trends remarkably well. In the southern hemisphere, the springtime trend only accounts for part of the summertime trends. There is a strong correlation between the ozone anomalies in northern hemisphere spring and those in the subsequent southern hemisphere spring, but not the converse

Summertime total ozone variations over middle and polar latitudes

The statistical relationship between springtime and summertime ozone over middle and polar latitudes is analyzed using zonally averaged total ozone data. Shortterm variations in springtime midlatitude ozone demonstrate only a modest correlation with springtime polar ozone variations. However by early summer, ozone variations throughout the extratropics are highly correlated. Analysis of correlation functions indicates that springtime midlatitude ozone, not polar ozone, is the best predictor for summertime polar ozone. Long-term total ozone trends at middle and high latitudes are also different for spring and nearly identical for summer. About 39% of the observed southern midlatitude ozone decline in December can be attributed to the polar ozone depletion up to November. In the Northern Hemisphere, the corresponding contribution is about 15%, but the error bars are too large to make an accurate estimate

On ozone correlation with meteofields in the Northern Hemisphere

The correlation coefficients of temperature and geopotential heights at various levels with total ozone and its vertical distribution have been analyzed, using the ground based and ozone sounding data. Two independent groups of factors affect total ozone. The first group - the geopotential values of the troposphere - stratosphere border (100-500 mb) manifest themselves most of all in the middle latitudes. Pertaining to this group is the total ozone correlation with the tropopause height and temperature at 500 mb. The correlation coefficients are negative (-0.55 -0.65) and little depend on the season. Related to this factor is a high (up to 0.8) correlation of ozone partial pressure with the temperature in the lower stratosphere. The second group is the geopotential and temperature values at the 10-30 mb coefficients (up to 0.6) are observed in winter in the subpolar latitudes. In summer they are substantially lower - about 0.1

Estimation of anthropogenic and volcanic SO2 emissions from satellite data in the presence of snow/ice on the ground

Early versions of satellite nadir-viewing UV SO2 data products did not explicitly account for the effects of snow/ice on retrievals. Snow-covered terrain, with its high reflectance in the UV, typically enhances satellite sensitivity to boundary layer pollution. However, a significant fraction of high-quality cloud-free measurements over snow is currently excluded from analyses. This leads to increased uncertainties of satellite emission estimates and potential seasonal biases due to the lack of data in winter months for some high-latitudinal sources. In this study, we investigated how Ozone Monitoring Instrument (OMI) and TROPOspheric Monitoring Instrument (TROPOMI) satellite SO2 measurements over snow-covered surfaces can be used to improve the annual emissions reported in our SO2 emissions catalogue (version 2; Fioletov et al., 2023). Only 100 out of 759 sources listed in the catalogue have 10 % or more of the observations over snow. However, for 40 high-latitude sources, more than 30 % of measurements suitable for emission calculations were made over snow-covered surfaces. For example, in the case of Norilsk, the world's largest SO2 point-source, annual emission estimates in the SO2 catalogue were based only on 3–4 summer months, while the addition of data for snow conditions extends that period to 7 months. Emissions in the SO2 catalogue were based on satellite measurements of SO2 slant column densities (SCDs) that were converted to vertical column densities (VCDs) using site-specific clear-sky air mass factors (AMFs), calculated for snow-free conditions. The same approach was applied to measurements with snow on the ground whereby a new set of constant, site-specific, clear sky with snow AMFs was created, and these were applied to the measured SCDs. Annual emissions were then estimated for each source considering (i) only clear-sky and snow-free days, (ii) only clear-sky with snow days, and (iii) a merged dataset (snow and snow-free conditions). For individual sources, the difference between emissions estimated for snow and snow-free conditions is within ±20 % for three-quarters of smelters and oil and gas sources and with practically no systematic bias. This is excellent consistency given that there is typically a factor of 3–5 difference between AMFs for snow and snow-free conditions. For coal-fired power plants, however, emissions estimated for snow conditions are on average 25 % higher than for snow-free conditions; this difference is likely real and due to larger production (consumption of coal) and emissions in wintertime.</p

Version 2 of the global catalogue of large anthropogenic and volcanic SO2 sources and emissions derived from satellite measurements

Sulfur dioxide (SO2) measurements from the Ozone Monitoring Instrument (OMI), Ozone Mapping and Profiler Suite (OMPS), and TROPOspheric Monitoring Instrument (TROPOMI) satellite spectrometers were used to update and extend the previously developed global catalogue of large SO2 emission sources. This version 2 of the global catalogue covers the period of 2005-2021 and includes a total of 759 continuously emitting point sources releasing from about 10 ktyr-1 to more than 4000 ktyr-1 of SO2, that have been identified and grouped by country and primary source origin: volcanoes (106 sources); power plants (477); smelters (74); and sources related to the oil and gas industry (102). There are several major improvements compared to the original catalogue: it combines emissions estimates from three satellite instruments instead of just OMI, uses a new version 2 of the OMI and OMPS SO2 dataset, and updated consistent site-specific air mass factors (AMFs) are used to calculate SO2 vertical column densities (VCDs). The newest TROPOMI SO2 data processed with the Covariance-Based Retrieval Algorithm (COBRA), used in the catalogue, can detect sources with emissions as low as 8 ktyr-1 (in 2018-2021) compared to the 30 ktyr-1 limit for OMI. In general, there is an overall agreement within ±12 % in total emissions estimated from the three satellite instruments for large regions. For individual emission sources, the spread is larger: the annual emissions estimated from OMI and TROPOMI agree within ±13 % in 50 % of cases and within ±28 % in 90 % of cases. The version 2 catalogue emissions were calculated as a weighted average of emission estimates from the three satellite instruments using an inverse-variance weighting method. OMI, OMPS, and TROPOMI data contribute 7 %, 5 %, and 88 % to the average, respectively, for small (\u3c30 \u3ektyr-1) sources and 33 %, 20 %, and 47 %, respectively, for large (\u3e300 ktyr-1) sources. The catalogue data show an approximate 50 % decline in global SO2 emissions between 2005 and 2021, although emissions were relatively stable during the last 3 years. The version 2 of the global catalogue has been posted at the NASA global SO2 monitoring website (10.5067/MEASURES/SO2/DATA406, Fioletov et al., 2022)

The evolution of synoptic ozone anomalies during the European Arctic Stratospheric Ozone Experiment in winter 1991/1992

The evolution of ozone anomalies over the middle and high latitudes of the Northern Hemisphere during the winter 1991-1992 is studied in this work. The largest monthly mean negative deviations in the middle latitudes of the Northern Hemisphere were about 10 percent in November and December, and up to 20 percent in January, February, and March over Eurasian territories, and much smaller over the Canadian sector. At the end of January, on individual days, total ozone values of 190-210 D.U. were observed over Eastern Europe and European part of Russia, that is 40-45 percent below normal. On the whole, the 1991-1992 winter was one of the most anomalous over all the period of ozone observations. Finally, an attempt is made to quantify the contribution of transport in the ozone layer changes over Europe during this period

Global total ozone recovery trends attributed to ozone-depleting substance (ODS) changes derived from five merged ozone datasets

We report on updated trends using different merged zonal mean total ozone datasets from satellite and ground-based observations for the period from 1979 to 2020. This work is an update of the trends reported in Weber et al. (2018) using the same datasets up to 2016. Merged datasets used in this study include NASA MOD v8.7 and NOAA Cohesive Data (COH) v8.6, both based on data from the series of Solar Backscatter Ultraviolet (SBUV), SBUV-2, and Ozone Mapping and Profiler Suite (OMPS) satellite instruments (1978–present), as well as the Global Ozone Monitoring Experiment (GOME)-type Total Ozone – Essential Climate Variable (GTO-ECV) and GOME-SCIAMACHY-GOME-2 (GSG) merged datasets (both 1995–present), mainly comprising satellite data from GOME, SCIAMACHY, OMI, GOME-2A, GOME-2B, and TROPOMI. The fifth dataset consists of the annual mean zonal mean data from ground-based measurements collected at the World Ozone and Ultraviolet Radiation Data Centre (WOUDC). Trends were determined by applying a multiple linear regression (MLR) to annual mean zonal mean data. The addition of 4 more years consolidated the fact that total ozone is indeed slowly recovering in both hemispheres as a result of phasing out ozone-depleting substances (ODSs) as mandated by the Montreal Protocol. The near-global (60∘ S–60∘ N) ODS-related ozone trend of the median of all datasets after 1995 was 0.4 ± 0.2 (2σ) %/decade, which is roughly a third of the decreasing rate of 1.5 ± 0.6 %/decade from 1978 until 1995. The ratio of decline and increase is nearly identical to that of the EESC (equivalent effective stratospheric chlorine or stratospheric halogen) change rates before and after 1995, confirming the success of the Montreal Protocol. The observed total ozone time series are also in very good agreement with the median of 17 chemistry climate models from CCMI-1 (Chemistry-Climate Model Initiative Phase 1) with current ODS and GHG (greenhouse gas) scenarios (REF-C2 scenario). The positive ODS-related trends in the Northern Hemisphere (NH) after 1995 are only obtained with a sufficient number of terms in the MLR accounting properly for dynamical ozone changes (Brewer–Dobson circulation, Arctic Oscillation (AO), and Antarctic Oscillation (AAO)). A standard MLR (limited to solar, Quasi-Biennial Oscillation (QBO), volcanic, and El Niño–Southern Oscillation (ENSO)) leads to zero trends, showing that the small positive ODS-related trends have been balanced by negative trend contributions from atmospheric dynamics, resulting in nearly constant total ozone levels since 2000

A New Global Anthropogenic SO2 Emission Inventory for the Last Decade: A Mosaic of Satellite-Derived and Bottom-Up Emissions

Sulfur dioxide (SO2) measurements from the Ozone Monitoring Instrument (OMI) satellite sensor have been used to detect emissions from large point sources. Emissions from over 400 sources have been quantified individually based on OMI observations, accounting for about a half of total reported anthropogenic SO2 emissions. Here we report a newly developed emission inventory, OMI-HTAP, by combining these OMI-based emission estimates and the conventional bottom-up inventory, HTAP, for smaller sources that OMI is not able to detect. OMI-HTAP includes emissions from OMI-detected sources that are not captured in previous leading bottom-up inventories, enabling more accurate emission estimates for regions with such missing sources. In addition, our approach offers the possibility of rapid updates to emissions from large point sources that can be detected by satellites. Our methodology applied to OMI-HTAP can also be used to merge improved satellite-derived estimates with other multi-year bottom-up inventories, which may further improve the accuracy of the emission trends. OMI-HTAP SO2 emissions estimates for Persian Gulf, Mexico, and Russia are 59%, 65%, and 56% larger than HTAP estimates, respectively, in year 2010. We have evaluated the OMI-HTAP inventory by performing simulations with the Goddard Earth Observing System version 5 (GEOS-5) model. The GEOS-5 simulated SO2 concentrations driven by both HTAP and OMI-HTAP were compared against in situ measurements. We focus for the validation on year 2010 for which HTAP is most valid and for which a relatively large number of in situ measurements are available. Results show that the OMI-HTAP inventory improves the agreement between the model and observations, in particular over the US, with the normalized mean bias decreasing from 0.41 (HTAP) to -0.03 (OMI-HTAP) for year 2010. Simulations with the OMI-HTAP inventory capture the worldwide major trends of large anthropogenic SO2 emissions that are observed with OMI. Correlation coefficients of the observed and modelled surface SO2 in 2014 increase from 0.16 (HTAP) to 0.59 (OMI-HTAP) and the normalized mean bias dropped from 0.29 (HTAP) to 0.05 (OMI-HTAP), when we updated 2010 HTAP emissions with 2014 OMI-HTAP emissions in the model

Impact of long-range correlations on trend detection in total ozone

Total ozone trends are typically studied using linear regression models that assume a first-order autoregression of the residuals [so-called AR(1) models]. We consider total ozone time series over 60°S–60°N from 1979 to 2005 and show that most latitude bands exhibit long-range correlated (LRC) behavior, meaning that ozone autocorrelation functions decay by a power law rather than exponentially as in AR(1). At such latitudes the uncertainties of total ozone trends are greater than those obtained from AR(1) models and the expected time required to detect ozone recovery correspondingly longer. We find no evidence of LRC behavior in southern middle-and high-subpolar latitudes (45°–60°S), where the long-term ozone decline attributable to anthropogenic chlorine is the greatest. We thus confirm an earlier prediction based on an AR(1) analysis that this region (especially the highest latitudes, and especially the South Atlantic) is the optimal location for the detection of ozone recovery, with a statistically significant ozone increase attributable to chlorine likely to be detectable by the end of the next decade. In northern middle and high latitudes, on the other hand, there is clear evidence of LRC behavior. This increases the uncertainties on the long-term trend attributable to anthropogenic chlorine by about a factor of 1.5 and lengthens the expected time to detect ozone recovery by a similar amount (from ∼2030 to ∼2045). If the long-term changes in ozone are instead fit by a piecewise-linear trend rather than by stratospheric chlorine loading, then the strong decrease of northern middle- and high-latitude ozone during the first half of the 1990s and its subsequent increase in the second half of the 1990s projects more strongly on the trend and makes a smaller contribution to the noise. This both increases the trend and weakens the LRC behavior at these latitudes, to the extent that ozone recovery (according to this model, and in the sense of a statistically significant ozone increase) is already on the verge of being detected. The implications of this rather controversial interpretation are discussed

Satellite Monitoring Over the Canadian Oil Sands: Highlights from Aura OMI and TES

Satellite remote sensing provides a unique perspective for air quality monitoring in and around the Canadian Oil Sands as a result of its spatial and temporal coverage. Presented are Aura satellite observations of key pollutants including nitrogen dioxide (NO2), sulfur dioxide (SO2), carbon monoxide (CO), ammonia (NH3), methanol (CH3OH), and formic acid (HCOOH) over the Canadian Oil Sands. Some of the highlights include: (i) the evolution of NO2 and SO2 from the Ozone Monitoring Instrument (OMI), including comparisons with other nearby sources, (ii) two years of ammonia, carbon monoxide, methanol, and formic acid observations from 240 km North-South Tropospheric Emission Spectrometer (TES) transects through the oils sands, and (iii) preliminary insights into emissions derived from these observations