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

Seasonal persistence of northern low- and middle-latitude anomalies of ozone and other trace gases in the upper stratosphere

Analysis of observed ozone profiles in Northern Hemisphere low and middle latitudes reveals the seasonal persistence of ozone anomalies in both the lower and upper stratosphere. Principal component analysis is used to detect that above 16 hPa the persistence is strongest in the latitude band 15–45°N, while below 16 hPa the strongest persistence is found over 45–60°N. In both cases, ozone anomalies persist through the entire year from November to October. The persistence of ozone anomalies in the lower stratosphere is presumably related to the wintertime ozone buildup with subsequent photochemical relaxation through summer, as previously found for total ozone. The persistence in the upper stratosphere is more surprising, given the short lifetime of Ox at these altitudes. It is hypothesized that this “seasonal memory” in the upper stratospheric ozone anomalies arises from the seasonal persistence of transport-induced wintertime NOy anomalies, which then perturb the ozone chemistry throughout the rest of the year. This hypothesis is confirmed by analysis of observations of NO2, NOx, and various long-lived trace gases in the upper stratosphere, which are found to exhibit the same seasonal persistence. Previous studies have attributed much of the year-to-year variability in wintertime extratropical upper stratospheric ozone to the Quasi-Biennial Oscillation (QBO) through transport-induced NOy (and hence NO2) anomalies but have not identified any statistical connection between the QBO and summertime ozone variability. Our results imply that through this “seasonal memory,” the QBO has an asynchronous effect on ozone in the low to midlatitude upper stratosphere during summer and early autumn

Trend and variability in ozone in the tropical lower stratosphere over 2.5 solar cycles observed by SAGE II and OSIRIS

We have extended the satellite-based ozone anomaly time series to the present (December 2012) by merging SAGE II (Stratospheric Aerosol and Gas Experiment II) with OSIRIS (Optical Spectrograph and Infrared Imager System) and correcting for the small bias (~0.5%) between them, determined using their temporal overlap of 4 years. Analysis of the merged data set (1984–2012) shows a statistically significant negative trend at all altitudes in the 18–25 km range, including a trend of (−4.6 ± 2.6)% decade⁻¹ at 19.5 km where the relative standard error is a minimum. We are also able to replicate previously reported decadal trends in the tropical lower-stratospheric ozone anomaly based on SAGE II observations. Uncertainties are smaller on the merged trend than the SAGE II trend at all altitudes. Underlying strong fluctuations in ozone anomaly due to El Niño–Southern Oscillation (ENSO), the altitude-dependent quasi-biennial oscillation, and tropopause pressure need to be taken into account to reduce trend uncertainties and, in the case of ENSO, to accurately determine the linear trend just above the tropopause. We also compare the observed ozone trend with a calculated trend that uses information on tropical upwelling and its temporal trend from model simulations, tropopause pressure trend information derived from reanalysis data, and vertical profiles from SAGE II and OSIRIS to determine the vertical gradient of ozone and its trend. We show that the observed trend agrees with the calculated trend and that the magnitude of the calculated trend is dominated by increased tropical upwelling, with minor but increasing contribution from the vertical ozone gradient trend as the tropical tropopause is approached. Improvements are suggested for future regression modelling efforts which could reduce trend uncertainties and biases in trend magnitudes, thereby allowing accurate trend detection to extend below 18 km

A global catalogue of large SO \u3c inf\u3e 2 sources and emissions derived from the Ozone Monitoring Instrument

Sulfur dioxide (SO2) measurements from the Ozone Monitoring Instrument (OMI) satellite sensor processed with the new principal component analysis (PCA) algorithm were used to detect large point emission sources or clusters of sources. The total of 491 continuously emitting point sources releasing from about 30 kt yr-1 to more than 4000 kt yr-1 of SO2 per year have been identified and grouped by country and by primary source origin: volcanoes (76 sources); power plants (297); smelters (53); and sources related to the oil and gas industry (65). The sources were identified using different methods, including through OMI measurements themselves applied to a new emission detection algorithm, and their evolution during the 2005-2014 period was traced by estimating annual emissions from each source. For volcanic sources, the study focused on continuous degassing, and emissions from explosive eruptions were excluded. Emissions from degassing volcanic sources were measured, many for the first time, and collectively they account for about 30 % of total SO2 emissions estimated from OMI measurements, but that fraction has increased in recent years given that cumulative global emissions from power plants and smelters are declining while emissions from oil and gas industry remained nearly constant. Anthropogenic emissions from the USA declined by 80 % over the 2005-2014 period as did emissions from western and central Europe, whereas emissions from India nearly doubled, and emissions from other large SO2-emitting regions (South Africa, Russia, Mexico, and the Middle East) remained fairly constant. In total, OMI-based estimates account for about a half of total reported anthropogenic SO2 emissions; the remaining half is likely related to sources emitting less than 30 kt yr-1 and not detected by OMI

On the statistical modeling of persistence in total ozone anomalies

Geophysical time series sometimes exhibit serial correlations that are stronger than can be captured by the commonly used first‐order autoregressive model. In this study we demonstrate that a power law statistical model serves as a useful upper bound for the persistence of total ozone anomalies on monthly to interannual timescales. Such a model is usually characterized by the Hurst exponent. We show that the estimation of the Hurst exponent in time series of total ozone is sensitive to various choices made in the statistical analysis, especially whether and how the deterministic (including periodic) signals are filtered from the time series, and the frequency range over which the estimation is made. In particular, care must be taken to ensure that the estimate of the Hurst exponent accurately represents the low‐frequency limit of the spectrum, which is the part that is relevant to long‐term correlations and the uncertainty of estimated trends. Otherwise, spurious results can be obtained. Based on this analysis, and using an updated equivalent effective stratospheric chlorine (EESC) function, we predict that an increase in total ozone attributable to EESC should be detectable at the 95% confidence level by 2015 at the latest in southern midlatitudes, and by 2020–2025 at the latest over 30°–45°N, with the time to detection increasing rapidly with latitude north of this range

A Global Ozone Climatology from Ozone Soundings via Trajectory Mapping: A Stratospheric Perspective

This study explores a domain-filling trajectory approach to generate a global ozone climatology from sparse ozonesonde data. Global ozone soundings of 51,898 profiles at 116 stations over 44 years (1965-2008) are used, from which forward and backward trajectories are performed for 4 days, driven by a set of meteorological reanalysis data. Ozone mixing ratios of each sounding from the surface to 26 km altitude are assigned to the entire path along the trajectory. The resulting global ozone climatology is archived monthly for five decades from the 1960s to the 2000s with grids of 5 degree 5 degree 1 km (latitude, longitude, and altitude). It is also archived yearly from 1965 to 2008. This climatology is validated at 20 ozonesonde stations by comparing the actual ozone sounding profile with that found through the trajectories, using the ozone soundings at all the stations except one being tested. The two sets of profiles are in good agreement, both individually with correlation coefficients between 0.975 and 0.998 and root mean square (RMS) differences of 87 to 482 ppbv, and overall with a correlation coefficient of 0.991 and an RMS of 224 ppbv. The ozone climatology is also compared with two sets of satellite data, from the Satellite Aerosol and Gas Experiment (SAGE) and the Optical Spectrography and InfraRed Imager System (OSIRIS). Overall, the ozone climatology compares well with SAGE and OSIRIS data by both seasonal and zonal means. The mean difference is generally under 20 above 15 km. The comparison is better in the northern hemisphere, where there are more ozonesonde stations, than in the southern hemisphere; it is also better in the middle and high latitudes than in the tropics, where assimilated winds are imperfect in some regions. This ozone climatology can capture known features in the stratosphere, as well as seasonal and decadal variations of these features. Furthermore, it provides a wealth of detail about longitudinal variations in the stratosphere such as the spring ozone maximum over the Canadian Arctic. It also covers higher latitudes than current satellite data. The climatology shows clearly the depletion of ozone from the 1970s to the mid 1990s and ozone recovery in the 2000s. When this climatology is used as the upper boundary condition in an Environment Canada operational chemical forecast model, the forecast is improved in the vicinity of the upper tropospherelower stratosphere region. As this ozone climatology is neither dependent on a priori data or photochemical modeling, it provides independent information and insight that can supplement satellite data and model simulations and enhance our understanding of stratospheric ozone

Performance of the ground-based total ozone network assessed using satellite data

Dobson and Brewer spectrophotometer and filter ozonometer data available from the World Ozone and Ultraviolet Data Centre (WOUDC) were compared with satellite total ozone measurements from TOMS (onboard Nimbus 7, Meteor 3, and Earth Probe satellites), OMI (AURA satellite) and GOME (ERS-2 satellite) instruments. Five characteristics of the difference with satellite data were calculated for each site and instrument type: the mean difference, the standard deviation of daily differences, the standard deviation of monthly differences, the amplitude of the seasonal component of the difference, and the range of annual values. All these characteristics were calculated for five 5-year-long bins and for each site separately for direct sun (DS) and zenith sky (ZS) ozone measurements. The main percentiles were estimated for the five characteristics of the difference and then used to establish criteria for “suspect” or “outlier” sites for each characteristic. About 61% of Dobson, 46% of Brewer, and 28% of filter stations located between 60°S and 60°N have no “suspect” or “outlier” characteristics. In nearly 90% of all cases, Dobson and Brewer sites demonstrated 5-year mean differences with satellites to be within ±3% (for DS observations). The seasonal median difference between all Brewer DS measurements at 25°–60°N and GOME and OMI overpasses remained within ±0.5% over a period of more than 10 years (...

Dynamics, stratospheric ozone, and climate change

Dynamics affects the distribution and abundance of stratospheric ozone directly through transport of ozone itself and indirectly through its effect on ozone chemistry via temperature and transport of other chemical species. Dynamical processes must be considered in order to understand past ozone changes, especially in the northern hemisphere where there appears to be significant low-frequency variability which can look “trend-like” on decadal time scales. A major challenge is to quantify the predictable, or deterministic, component of past ozone changes. Over the coming century, changes in climate will affect the expected recovery of ozone. For policy reasons it is important to be able to distinguish and separately attribute the effects of ozone-depleting substances and greenhouse gases on both ozone and climate. While the radiative-chemical effects can be relatively easily identified, this is not so evident for dynamics — yet dynamical changes (e.g., changes in the Brewer-Dobson circulation) could have a first-order effect on ozone over particular regions. Understanding the predictability and robustness of such dynamical changes represents another major challenge. Chemistry-climate models have recently emerged as useful tools for addressing these questions, as they provide a self-consistent representation of dynamical aspects of climate and their coupling to ozone chemistry. We can expect such models to play an increasingly central role in the study of ozone and climate in the future, analogous to the central role of global climate models in the study of tropospheric climate change

Reconciliation of halogen-induced ozone loss with the total-column ozone record

The observed depletion of the ozone layer from the 1980s onwards is attributed to halogen source gases emitted by human activities. However, the precision of this attribution is complicated by year-to-year variations in meteorology, that is, dynamical variability, and by changes in tropospheric ozone concentrations. As such, key aspects of the total-column ozone record, which combines changes in both tropospheric and stratospheric ozone, remain unexplained, such as the apparent absence of a decline in total-column ozone levels before 1980, and of any long-term decline in total-column ozone levels in the tropics. Here we use a chemistry–climate model to estimate changes in halogen-induced ozone loss between 1960 and 2010; the model is constrained by observed meteorology to remove the effects of dynamical variability, and driven by emissions of tropospheric ozone precursors to separate out changes in tropospheric ozone. We show that halogen-induced ozone loss closely followed stratospheric halogen loading over the studied period. Pronounced enhancements in ozone loss were apparent in both hemispheres following the volcanic eruptions of El Chichon and, in particular, Mount Pinatubo, which significantly enhanced stratospheric aerosol loads. We further show that approximately 40% of the long-term non-volcanic ozone loss occurred before 1980, and that long-term ozone loss also occurred in the tropical stratosphere. Finally, we show that halogen-induced ozone loss has declined by over 10% since stratospheric halogen loading peaked in the late 1990s, indicating that the recovery of the ozone layer is well underway