ALBERT

Description: The electrochemical concentration cell (ECC) ozonesonde has been the main instrument for in situ profiling of ozone worldwide; yet, some details of its operation, which contribute to the ozone uncertainty budget, are not well understood. Here, we investigate the time response of the chemical reactions inside the ECC and how corrections can be used to remove some systematic biases. The analysis is based on the understanding that two reaction pathways involving ozone occur inside the ECC that generate electrical currents on two very different timescales. The main fast-reaction pathway with a time constant of about 20 s is due the conversion of iodide to molecular iodine and the generation of two free electrons per ozone molecule. A secondary slow-reaction pathway involving the buffer generates an excess current of about 2 %–10 % with a time constant of about 25 min. This excess current can be interpreted as what has conventionally been considered the “background current”. This contribution can be calculated and removed from the measured current instead of the background current. Here we provide an algorithm to calculate and remove the contribution of the slow-reaction pathway and to correct for the time lag of the fast-reaction pathway. This processing algorithm has been applied to ozonesonde profiles at Costa Rica and during the Central Equatorial Pacific Experiment (CEPEX) as well as to laboratory experiments evaluating the performance of ECC ozonesondes. At Costa Rica, where a 1 % KI, 1/10th buffer solution is used, there is no change in the derived total ozone column; however, in the upper troposphere and lower stratosphere, average reported ozone concentrations increase by up to 7 % and above 30 km decrease by up to 7 %. During CEPEX, where a 1 % KI, full-buffer solution was used, ozone concentrations are increased mostly in the upper troposphere, with no change near the top of the profile. In the laboratory measurements, the processing algorithms have been applied to measurements using the majority of current sensing solutions and using only the stronger pump efficiency correction reported by Johnson et al. (2002). This improves the accuracy of the ECC sonde ozone profiles, especially for low ozone concentrations or large ozone gradients and removes systematic biases relative to the reference instruments. In the surface layer, operational procedures prior to launch, in particular the use of filters, influence how typical gradients above the surface are detected. The correction algorithm may report gradients that are steeper than originally reported, but their uncertainty is strongly influenced by the prelaunch procedures.

Description: Ozone plays a significant role in the chemical and radiative state of the atmosphere. For this reason there are many instruments used to measure ozone from the ground, from space, and from balloons. Balloon-borne electrochemical cell ozonesondes provide some of the best measurements of the ozone profile up to the mid-stratosphere, providing high vertical resolution, high precision, and a wide geographic distribution. From the mid-1990s to the late 2000s the consistency of long-term records from balloon-borne ozonesondes has been compromised by differences in manufacturers, Science Pump (SP) and ENSCI (EN), and differences in recommended sensor solution concentrations, 1.0 % potassium iodide (KI) and the one-half dilution: 0.5 %. To investigate these differences, a number of organizations have independently undertaken comparisons of the various ozonesonde types and solution concentrations, resulting in 197 ozonesonde comparison profiles. The goal of this study is to derive transfer functions to allow measurements outside of standard recommendations, for sensor composition and ozonesonde type, to be converted to a standard measurement and thus homogenize the data to the expected accuracy of 5 % (10 %) in the stratosphere (troposphere). Subsets of these data have been analyzed previously and intermediate transfer functions derived. Here all the comparison data are analyzed to compare (1) differences in sensor solution composition for a single ozonesonde type, (2) differences in ozonesonde type for a single sensor solution composition, and (3) the World Meteorological Organization's (WMO) and manufacturers' recommendations of 1.0 % KI solution for Science Pump and 0.5 % KI for ENSCI. From the recommendations it is clear that ENSCI ozonesondes and 1.0 % KI solution result in higher amounts of ozone sensed. The results indicate that differences in solution composition and in ozonesonde type display little pressure dependence at pressures  ≥  30 hPa, and thus the transfer function can be characterized as a simple ratio of the less sensitive to the more sensitive method. This ratio is 0.96 for both solution concentration and ozonesonde type. The ratios differ at pressures

Description: We validate the Ozone Monitoring Instrument (OMI) Ozone Profile (PROFOZ) product from October 2004 through December 2014 retrieved by the Smithsonian Astrophysical Observatory (SAO) algorithm against ozonesonde observations. We also evaluate the effects of OMI row anomaly (RA) on the retrieval by dividing the dataset into before and after the occurrence of serious OMI RA, i.e., pre-RA (2004–2008) and post-RA (2009–2014). The retrieval shows good agreement with ozonesondes in the tropics and midlatitudes and for pressure  

Description: Atmospheric ozone plays a key role in air quality and the radiation budget of the Earth, both directly and through its chemical influence on other trace gases. Assessments of the atmospheric ozone distribution and associated climate change therefore demand accurate vertically resolved ozone observations with both stratospheric and tropospheric sensitivity, on both global and regional scales, and both in the long term and at shorter timescales. Such observations have been acquired by two series of European nadir-viewing ozone profilers, namely the scattered-light UV–visible spectrometers of the GOME family, launched regularly since 1995 (GOME, SCIAMACHY, OMI, GOME-2A/B, TROPOMI, and the upcoming Sentinel-5 series), and the thermal infrared emission sounders of the IASI type, launched regularly since 2006 (IASI on Metop platforms and the upcoming IASI-NG on Metop-SG). In particular, several Level-2 retrieved, Level-3 monthly gridded, and Level-4 assimilated nadir ozone profile data products have been improved and harmonized in the context of the ozone project of the European Space Agency's Climate Change Initiative (ESA Ozone_cci). To verify their fitness for purpose, these ozone datasets must undergo a comprehensive quality assessment (QA), including (a) detailed identification of their geographical, vertical, and temporal domains of validity; (b) quantification of their potential bias, noise, and drift and their dependences on major influence quantities; and (c) assessment of the mutual consistency of data from different sounders. For this purpose we have applied to the Ozone_cci Climate Research Data Package (CRDP) released in 2017 the versatile QA and validation system Multi-TASTE, which has been developed in the context of several heritage projects (ESA's Multi-TASTE, EUMETSAT's O3M-SAF, and the European Commission's FP6 GEOmon and FP7 QA4ECV). This work, as the second in a series of four Ozone_cci validation papers, reports for the first time on data content studies, information content studies and ground-based validation for both the GOME- and IASI-type climate data records combined. The ground-based reference measurements have been provided by the Network for the Detection of Atmospheric Composition Change (NDACC), NASA's Southern Hemisphere Additional Ozonesonde programme (SHADOZ), and other ozonesonde and lidar stations contributing to the World Meteorological Organisation's Global Atmosphere Watch (WMO GAW). The nadir ozone profile CRDP quality assessment reveals that all nadir ozone profile products under study fulfil the GCOS user requirements in terms of observation frequency and horizontal and vertical resolution. Yet all L2 observations also show sensitivity outliers in the UTLS and are strongly correlated vertically due to substantial averaging kernel fluctuations that extend far beyond the kernel's 15 km FWHM. The CRDP typically does not comply with the GCOS user requirements in terms of total uncertainty and decadal drift, except for the UV–visible L4 dataset. The drift values of the L2 GOME and OMI, the L3 IASI, and the L4 assimilated products are found to be overall insignificant, however, and applying appropriate altitude-dependent bias and drift corrections make the data fit for climate and atmospheric composition monitoring and modelling purposes. Dependence of the Ozone_cci data quality on major influence quantities – resulting in data screening suggestions to users – and perspectives for the Copernicus Sentinel missions are additionally discussed.

Description: This study examines the adequacy of the existing Brewer network to supplement other networks from the ground and space to detect SO2 plumes of volcanic origin. It was found that large volcanic eruptions of the last decade in the Northern Hemisphere have a positive columnar SO2 signal seen by the Brewer instruments located under the plume. It is shown that a few days after the eruption the Brewer instrument is capable of detecting significant columnar SO2 increases, exceeding on average 2 DU relative to an unperturbed pre-volcanic 10-day baseline, with a mean close to 0 and σ = 0.46, as calculated from the 32 Brewer stations under study. Intercomparisons with independent measurements from the ground and space as well as theoretical calculations corroborate the capability of the Brewer network to detect volcanic plumes. For instance, the comparison with OMI (Ozone Monitoring Instrument) and GOME-2 (Global Ozone Monitoring Experiment-2) SO2 space-borne retrievals shows statistically significant agreement between the Brewer network data and the collocated satellite overpasses in the case of the Kasatochi eruption. Unfortunately, due to sparsity of satellite data, the significant positive departures seen in the Brewer and other ground networks following the Eyjafjallajökull, Bárðarbunga and Nabro eruptions could not be statistically confirmed by the data from satellite overpasses. A model exercise from the MACC (Monitoring Atmospheric Composition and Climate) project shows that the large increases in SO2 over Europe following the Bárðarbunga eruption in Iceland were not caused by local pollution sources or ship emissions but were clearly linked to the volcanic eruption. Sulfur dioxide positive departures in Europe following Bárðarbunga could be traced by other networks from the free troposphere down to the surface (AirBase (European air quality database) and EARLINET (European Aerosol Research Lidar Network)). We propose that by combining Brewer data with that from other networks and satellites, a useful tool aided by trajectory analyses and modelling could be created which can also be used to forecast high SO2 values both at ground level and in air flight corridors following future eruptions.

Description: The Arosa site is well known in the ozone community for its continuous total ozone column observations that have been recorded since 1926. Originally based on Dobson sun spectrophotometers, the site has been gradually complemented by three automatic Brewer instruments, in operation since 1998. To secure the long-term ozone monitoring in this Alpine region and to benefit from synergies with the World Radiation Center, the feasibility of moving this activity to the nearby site at Davos (aerial distance of 13 km) has been explored. Concerns about a possible rupture of the 90-year-long record has motivated a careful comparison of the two sites, since great attention to the data continuity and quality has always been central to the operations of the observatory at Arosa. To this end, one element of the Arosa Brewer triad has been set up at the Davos site since November 2011 to realize a campaign of parallel measurements and to study the deviations between the three Brewer instruments. The analysis of the coincident measurement shows that the differences between Arosa and Davos remain within the range of the long-term stability of the Brewer instruments. A nonsignificant seasonal cycle is observed, which could possibly be induced by a stray-light bias and the altitude difference between the two sites. These differences are shown to be lower than the short-term variability of the time series and the overall uncertainty from individual Brewer instruments and therefore are not statistically significant. It is therefore concluded that the world's longest time series of the total ozone column obtained at Arosa site could be safely extended and continued with measurements taken from instruments located at the nearby Davos site without introducing a bias to this unique record.

Description: Ozone forms in the Earth's atmosphere from the photodissociation of molecular oxygen, primarily in the tropical stratosphere. It is then transported to the extratropics by the Brewer–Dobson circulation (BDC), forming a protective ozone layer around the globe. Human emissions of halogen-containing ozone-depleting substances (hODSs) led to a decline in stratospheric ozone until they were banned by the Montreal Protocol, and since 1998 ozone in the upper stratosphere is rising again, likely the recovery from halogen-induced losses. Total column measurements of ozone between the Earth's surface and the top of the atmosphere indicate that the ozone layer has stopped declining across the globe, but no clear increase has been observed at latitudes between 60° S and 60° N outside the polar regions (60–90°). Here we report evidence from multiple satellite measurements that ozone in the lower stratosphere between 60° S and 60° N has indeed continued to decline since 1998. We find that, even though upper stratospheric ozone is recovering, the continuing downward trend in the lower stratosphere prevails, resulting in a downward trend in stratospheric column ozone between 60° S and 60° N. We find that total column ozone between 60° S and 60° N appears not to have decreased only because of increases in tropospheric column ozone that compensate for the stratospheric decreases. The reasons for the continued reduction of lower stratospheric ozone are not clear; models do not reproduce these trends, and thus the causes now urgently need to be established.

Description: Observing stratospheric ozone is essential to assess whether the Montreal Protocol has succeeded in saving the ozone layer by banning ozone depleting substances. Recent studies have reported positive trends, indicating that ozone is recovering in the upper stratosphere at mid-latitudes, but the trend magnitudes differ, and uncertainties are still high. Trends and their uncertainties are influenced by factors such as instrumental drifts, sampling patterns, discontinuities, biases, or short-term anomalies that may all mask a potential ozone recovery. The present study investigates how anomalies, temporal measurement sampling rates, and trend period lengths influence resulting trends. We present an approach for handling suspicious anomalies in trend estimations. For this, we analysed multiple ground-based stratospheric ozone records in central Europe to identify anomalous periods in data from the GROund-based Millimetre-wave Ozone Spectrometer (GROMOS) located in Bern, Switzerland. The detected anomalies were then used to estimate ozone trends from the GROMOS time series by considering the anomalous observations in the regression. We compare our improved GROMOS trend estimate with results derived from the other ground-based ozone records (lidars, ozonesondes, and microwave radiometers), that are all part of the Network for the Detection of Atmospheric Composition Change (NDACC). The data indicate positive trends of 1 % decade−1 to 3 % decade−1 at an altitude of about 39 km (3 hPa), providing a confirmation of ozone recovery in the upper stratosphere in agreement with satellite observations. At lower altitudes, the ground station data show inconsistent trend results, which emphasize the importance of ongoing research on ozone trends in the lower stratosphere. Our presented method of a combined analysis of ground station data provides a useful approach to recognize and to reduce uncertainties in stratospheric ozone trends by considering anomalies in the trend estimation. We conclude that stratospheric trend estimations still need improvement and that our approach provides a tool that can also be useful for other data sets.

Description: Climatic Observatory (LKO) in Arosa (Switzerland), marking the beginning of the world's longest series of total (or column) ozone measurements. They were driven by the recognition that atmospheric ozone is important for human health, as well as by scientific curiosity about what was, at the time, an ill characterised atmospheric trace gas. From around the mid-1950s to the beginning of the 1970s studies of high atmosphere circulation patterns that could improve weather forecasting was justification for studying stratospheric ozone. In the mid-1970s, a paradigm shift occurred when it became clear that the damaging effects of anthropogenic ozone-depleting substances (ODSs), such as long-lived chlorofluorocarbons, needed to be documented. This justified continuing the ground-based measurements of stratospheric ozone. Levels of ODSs peaked around the mid-1990s as a result of a global environmental policy to protect the ozone layer, implemented through the 1987 Montreal Protocol and its subsequent amendments and adjustments. Consequently, chemical destruction of stratospheric ozone started to slow around the mid-1990s. To some extent, this raises the question as to whether continued ozone observation is indeed necessary. In the last decade there has been a tendency to reduce the costs associated with making ozone measurements globally including at Arosa. However, the large natural variability in ozone on diurnal, seasonal, and interannual scales complicates the capacity for demonstrating the success of the Montreal Protocol. Chemistry-climate models also predict a super-recovery of the ozone layer at mid-latitudes in the second half of this century, i.e. an increase of ozone concentrations beyond pre-1970 levels, as a consequence of ongoing climate change. These factors, and identifying potentially unexpected stratospheric responses to climate change, support the continued need to document stratospheric ozone changes. This is particularly valuable at the Arosa site, due to the unique length of the observational record. This paper presents the evolution of the ozone layer, the history of international ozone research, and discusses the justification for the measurements in the past, present and into future.

Description: This paper demonstrates that SO2 columnar amounts have significantly increased following the five largest volcanic eruptions of the past decade in the Northern Hemisphere. A strong positive signal was detected by all the existing networks either ground based (Brewer, EARLINET, AirBase) or from satellites (OMI, GOME-2). The study particularly examines the adequacy of the existing Brewer network to detect SO2 plumes of volcanic origin in comparison to other networks and satellite platforms. The comparison with OMI and GOME-2 SO2 space-borne retrievals shows statistically significant agreement between the Brewer network data and the collocated satellite overpasses. It is shown that the Brewer instrument is capable of detecting significant columnar SO2 increases following large volcanic eruptions, when SO2 levels rise well above the instrumental noise of daily observations, estimated to be of the order of 2 DU. A model exercise from the MACC project shows that the large increases of SO2 over Europe following the Bárðarbunga eruption in Iceland were not caused by local sources or ship emissions but are clearly linked to the eruption. We propose that by combining Brewer data with that from other networks and satellites, a useful tool aided by trajectory analyses and modeling could be created which can be used to forecast high SO2 values both at ground level and in air flight corridors following future eruptions.