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

Satellite Estimation of Spectral Surface UV Irradiance

The local variability of UV irradiance at the Earth's surface is mostly caused by clouds in addition to the seasonal variability. Parametric representations of radiative transfer RT calculations are presented for the convenient solution of the transmission T of ultraviolet radiation through plane parallel clouds over a surface with reflectivity R(sub s). The calculations are intended for use with the Total Ozone Mapping Spectrometer (TOMS) measured radiances to obtain the calculated Lambert equivalent scene reflectivity R for scenes with and without clouds. The purpose is to extend the theoretical analysis of the estimation of UV irradiance from satellite data for a cloudy atmosphere. Results are presented for a range of cloud optical depths and solar zenith angles for the cases of clouds over a low reflectivity surface R(sub s) less than 0.1, over a snow or ice surface R(sub s) greater than 0.3, and for transmission through a non-conservative scattering cloud with single scattering albedo omega(sub 0) = 0.999. The key finding for conservative scattering is that the cloud-transmission function C(sub T), the ratio of cloudy-to clear-sky transmission, is roughly C(sub T) = 1 - R(sub c) with an error of less than 20% for nearly overhead sun and snow-free surfaces. For TOMS estimates of UV irradiance in the presence of both snow and clouds, independent information about snow albedo is needed for conservative cloud scattering. For non-conservative scattering with R(sub s) greater than 0.5 (snow) the satellite measured scene reflectance cannot be used to estimate surface irradiance. The cloud transmission function has been applied to the calculation of UV irradiance at the Earth's surface and compared with ground-based measurements

Technical Note: A SAGE-corrected SBUV zonal-mean ozone data set

A stratospheric vertically resolved, monthly, zonal-mean ozone data set based on Satellite Aerosol and Gas Experiment (SAGE) and Solar Backscatter UltraViolet (SBUV) data spanning 1979–2005 is presented. Drifts in individual SBUV instruments and inter-SBUV biases are corrected using SAGE I and II by calculating differences between coincident SAGE-SBUV measurements. In this way the daily, near-global coverage of SBUV(/2) is combined with the stability and precision of SAGE to provide a homogeneous ozone record suitable for trend analysis. The resultant SAGE-corrected SBUV data set, shows, for example, a more realistic Quasi-Biennial Oscillation signal compared to the one derived from SBUV data alone. Furthermore, this methodology can be used to extend the present data set beyond the lifetime of SAGE II

Lessons Learned from OMI Observations of Point Source SO2 Pollution

The Ozone Monitoring Instrument (OMI) on NASA Aura satellite makes global daily measurements of the total column of sulfur dioxide (SO2), a short-lived trace gas produced by fossil fuel combustion, smelting, and volcanoes. Although anthropogenic SO2 signals may not be detectable in a single OMI pixel, it is possible to see the source and determine its exact location by averaging a large number of individual measurements. We describe new techniques for spatial and temporal averaging that have been applied to the OMI SO2 data to determine the spatial distributions or "fingerprints" of SO2 burdens from top 100 pollution sources in North America. The technique requires averaging of several years of OMI daily measurements to observe SO2 pollution from typical anthropogenic sources. We found that the largest point sources of SO2 in the U.S. produce elevated SO2 values over a relatively small area - within 20-30 km radius. Therefore, one needs higher than OMI spatial resolution to monitor typical SO2 sources. TROPOMI instrument on the ESA Sentinel 5 precursor mission will have improved ground resolution (approximately 7 km at nadir), but is limited to once a day measurement. A pointable geostationary UVB spectrometer with variable spatial resolution and flexible sampling frequency could potentially achieve the goal of daily monitoring of SO2 point sources and resolve downwind plumes. This concept of taking the measurements at high frequency to enhance weak signals needs to be demonstrated with a GEOCAPE precursor mission before 2020, which will help formulating GEOCAPE measurement requirements

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

Improved Satellite Retrievals of NO2 and SO2 over the Canadian Oil Sands and Comparisons with Surface Measurements

Satellite remote sensing is increasingly being used to monitor air quality over localized sources such as the Canadian oil sands. Following an initial study, significantly low biases have been identified in current NO2 and SO2 retrieval products from the Ozone Monitoring Instrument (OMI) satellite sensor over this location resulting from a combination of its rapid development and small spatial scale. Air mass factors (AMFs) used to convert line-of-sight "slant" columns to vertical columns were re-calculated for this region based on updated and higher resolution input information including absorber profiles from a regional-scale (15 km 15 km resolution) air quality model, higher spatial and temporal resolution surface reflectivity, and an improved treatment of snow. The overall impact of these new Environment Canada (EC) AMFs led to substantial increases in the peak NO2 and SO2 average vertical column density (VCD), occurring over an area of intensive surface mining, by factors of 2 and 1.4, respectively, relative to estimates made with previous AMFs. Comparisons are made with long-term averages of NO2 and SO2 (2005-2011) from in situ surface monitors by using the air quality model to map the OMI VCDs to surface concentrations. This new OMI-EC product is able to capture the spatial distribution of the in situ instruments (slopes of 0.65 to 1.0, correlation coefficients of greater than 0.9). The concentration absolute values from surface network observations were in reasonable agreement, with OMI-EC NO2 and SO2 biased low by roughly 30%. Several complications were addressed including correction for the interference effect in the surface NO2 instruments and smoothing and clear-sky biases in the OMI measurements. Overall these results highlight the importance of using input information that accounts for the spatial and temporal variability of the location of interest when performing retrievals

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