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This study analyses the variability and trends of ultraviolet-B (UV-B, wavelength 280–320 nm) radiation that can cause DNA damage. The variability and trends caused by climate change due to enhanced greenhouse gas (GHG) concentrations. The analysis is based on DNA-active irradiance, total ozone, total cloud cover, and surface albedo calculations with the European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) chemistry–climate model (CCM) free-running simulations following the RCP 6.0 climate scenario for the period 1960–2100. The model output is evaluated with DNA-active irradiance ground-based measurements, satellite SBUV (v8.7) total-ozone measurements, and satellite MODerate-resolution Imaging Spectroradiometer (MODIS) Terra cloud cover data. The results show that the model reproduces the observed variability and change in total ozone, DNA-active irradiance, and cloud cover for the period 2000–2018 quite well according to the statistical comparisons. Between 50∘ N–50∘ S, the DNA-damaging UV radiation is expected to decrease until 2050 and to increase thereafter, as was shown previously by Eleftheratos et al. (2020). This change is associated with decreases in the model total cloud cover and negative trends in total ozone after about 2050 due to increasing GHGs. The new study confirms the previous work by adding more stations over low latitudes and mid-latitudes (13 instead of 5 stations). In addition, we include estimates from high-latitude stations with long-term measurements of UV irradiance (three stations in the northern high latitudes and four stations in the southern high latitudes greater than 55∘). In contrast to the predictions for 50∘ N–50∘ S, it is shown that DNA-active irradiance will continue to decrease after the year 2050 over high latitudes because of upward ozone trends. At latitudes poleward of 55∘ N, we estimate that DNA-active irradiance will decrease by 8.2 %±3.8 % from 2050 to 2100. Similarly, at latitudes poleward of 55∘ S, DNA-active irradiance will decrease by 4.8 % ± 2.9 % after 2050. The results for the high latitudes refer to the summer period and not to the seasons when ozone depletion occurs, i.e. in late winter and spring. The contributions of ozone, cloud, and albedo trends to the DNA-active irradiance trends are estimated and discussed.

Within the framework of the UV-Indien network, nine ground stations have been equipped with ultraviolet broadband radiometers, five of them have also been equipped with an all-sky camera, and the main station in Saint-Denis de la Réunion is also equipped with a spectroradiometer. These stations are spatially distributed to cover a wide range of latitudes, longitudes, altitudes, and environmental conditions in five countries of the western Indian Ocean region (Comoros, France, Madagascar, Mauritius, and Seychelles), a part of the world where almost no measurements have been made so far. The distribution of the stations is based on the scientific interest of studying ultraviolet radiation not only in relation to atmospheric processes but also in order to provide data relevant to fields such as biology, health (prevention of skin cancer), and agriculture. The main scientific objectives of this network are to study the annual and inter-annual variability in the ultraviolet (UV) radiation in this area, to validate the output of numerical models and satellite estimates of ground-based UV measurements, and to monitor UV radiation in the context of climate change and projected ozone depletion in this region. A calibration procedure including three types of calibrations responding to the various constraints of sustaining the network has been put in place, and a data processing chain has been set up to control the quality and the format of the files sent to the various data centres. A method of clear-sky filtering of the data is also applied. Here, we present an intercomparison with other datasets, as well as several daily or monthly representations of the UV index (UVI) and cloud fraction data, to discuss the quality of the data and their range of values for the older stations (Antananarivo, Anse Quitor, Mahé, and Saint-Denis). Ground-based measurements of the UVI are used to validate satellite estimates – Ozone Monitoring Instrument (OMI), the TROPOspheric Monitoring Instrument (TROPOMI), and the Global Ozone Monitoring Experiment (GOME) – and model forecasts of UVI – Tropospheric Emission Monitoring Internet Service (TEMIS) and Copernicus Atmospheric Monitoring Service (CAMS). The median relative differences between satellite or model estimates and ground-based measurements of clear-sky UVI range between −34.5 % and 15.8 %. Under clear skies, the smallest UVI median difference between the satellite or model estimates and the measurements made by ground-based instruments is found to be 0.02 (TROPOMI), 0.04 (OMI), −0.1 (CAMS), and −0.4 (CAMS) at Saint-Denis, Antananarivo, Anse Quitor, and Mahé, respectively. The diurnal variability in UVI and cloud fraction, as well as the monthly variability in UVI, is evaluated to ensure the quality of the dataset. The data used in this study are available at https://doi.org/10.5281/zenodo.4811488 (Lamy and Portafaix, 2021a).

The TROPOspheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5 Precursor (S5P) satellite was launched on 13 October 2017 to provide the atmospheric composition for atmosphere and climate research. The S5P is a Sun-synchronous polar-orbiting satellite providing global daily coverage. The TROPOMI swath is 2600 km wide, and the ground resolution for most data products is 7.2×3.5 km2 (5.6×3.5 km2 since 6 August 2019) at nadir. The Finnish Meteorological Institute (FMI) is responsible for the development of the TROPOMI UV algorithm and the processing of the TROPOMI surface ultraviolet (UV) radiation product which includes 36 UV parameters in total. Ground-based data from 25 sites located in arctic, subarctic, temperate, equatorial and Antarctic areas were used for validation of the TROPOMI overpass irradiance at 305, 310, 324 and 380 nm, overpass erythemally weighted dose rate/UV index, and erythemally weighted daily dose for the period from 1 January 2018 to 31 August 2019. The validation results showed that for most sites 60 %–80 % of TROPOMI data was within ±20 % of ground-based data for snow-free surface conditions. The median relative differences to ground-based measurements of TROPOMI snow-free surface daily doses were within ±10 % and ±5 % at two-thirds and at half of the sites, respectively. At several sites more than 90 % of cloud-free TROPOMI data was within ±20 % of ground-based measurements. Generally median relative differences between TROPOMI data and ground-based measurements were a little biased towards negative values (i.e. satellite data < ground-based measurement), but at high latitudes where non-homogeneous topography and albedo or snow conditions occurred, the negative bias was exceptionally high: from −30 % to −65 %. Positive biases of 10 %–15 % were also found for mountainous sites due to challenging topography. The TROPOMI surface UV radiation product includes quality flags to detect increased uncertainties in the data due to heterogeneous surface albedo and rough terrain, which can be used to filter the data retrieved under challenging conditions.

Volcanic sulfate aerosols play a key role in air quality and climate. However, the rate of oxidation of sulfur dioxide (SO2) precursor gas to sulfate aerosols (SO42-) in volcanic plumes is poorly known, especially in the troposphere. Here we determine the chemical speciation as well as the intensity and temporal persistence of the impact on air quality of sulfate aerosols from the 2014–2015 Holuhraun flood lava eruption of Icelandic volcano Bárðarbunga. To do so, we jointly analyse a set of SO2 observations from satellite (OMPS and IASI) and ground-level measurements from air quality monitoring stations together with high temporal resolution mass spectrometry measurements of an Aerosol Chemical Speciation Monitor (ACSM) performed far from the volcanic source. We explore month/year long ACSM data in France from stations in contrasting environments, close and far from industrial sulfur-rich activities. We demonstrate that volcanic sulfate aerosols exhibit a distinct chemical signature in urban/rural conditions, with NO3:SO4 mass concentration ratios lower than for non-volcanic background aerosols. These results are supported by thermodynamic simulations of aerosol composition, using the ISORROPIA II model, which show that ammonium sulfate aerosols are preferentially formed at a high concentration of sulfate, leading to a decrease in the production of particulate ammonium nitrate. Such a chemical signature is however more difficult to identify at heavily polluted industrial sites due to a high level of background noise in sulfur. Nevertheless, aged volcanic sulfates can be distinguished from freshly emitted industrial sulfates according to their contrasting degree of anion neutralization. Combining AERONET (AErosol RObotic NETwork) sunphotometric data with ACSM observations, we also show a long persistence over weeks of pollution in volcanic sulfate aerosols, while SO2 pollution disappears in a few days at most. Finally, gathering 6-month long datasets from 27 sulfur monitoring stations of the EMEP (European Monitoring and Evaluation Programme) network allows us to demonstrate a much broader large-scale European pollution, in both SO2 and SO4, associated with the Holuhraun eruption, from Scandinavia to France. While widespread SO2 anomalies, with ground-level mass concentrations far exceeding background values, almost entirely result from the volcanic source, the origin of sulfate aerosols is more complex. Using a multi-site concentration-weighted trajectory analysis, emissions from the Holuhraun eruption are shown to be one of the main sources of SO4 at all EMEP sites across Europe and can be distinguished from anthropogenic emissions from eastern Europe but also from Great Britain. A wide variability in SO2:SO4 mass concentration ratios, ranging from 0.8 to 8.0, is shown at several stations geographically dispersed at thousands of kilometres from the eruption site. Despite this apparent spatial complexity, we demonstrate that these mass oxidation ratios can be explained by a simple linear dependency on the age of the plume, with a SO2-to-SO4 oxidation rate of 0.23 h−1. Most current studies generally focus on SO2, an unambiguous and more readily measured marker of the volcanic plume. However, the long persistence of the chemical fingerprint of volcanic sulfate aerosols at continental scale, as shown for the Holuhraun eruption here, casts light on the impact of tropospheric eruptions and passive degassing activities on air quality, health, atmospheric chemistry and climate.

We have derived values of the ultraviolet index (UVI) at solar noon using the Tropospheric Ultraviolet Model (TUV) driven by ozone, temperature and aerosol fields from climate simulations of the first phase of the Chemistry-Climate Model Initiative (CCMI-1). Since clouds remain one of the largest uncertainties in climate projections, we simulated only the clear-sky UVI. We compared the modelled UVI climatologies against present-day climatological values of UVI derived from both satellite data (the OMI-Aura OMUVBd product) and ground-based measurements (from the NDACC network). Depending on the region, relative differences between the UVI obtained from CCMI/TUV calculations and the ground-based measurements ranged between −5.9 % and 10.6 %. We then calculated the UVI evolution throughout the 21st century for the four Representative Concentration Pathways (RCPs 2.6, 4.5, 6.0 and 8.5). Compared to 1960s values, we found an average increase in the UVI in 2100 (of 2 %–4 %) in the tropical belt (30∘ N–30∘ S). For the mid-latitudes, we observed a 1.8 % to 3.4 % increase in the Southern Hemisphere for RCPs 2.6, 4.5 and 6.0 and found a 2.3 % decrease in RCP 8.5. Higher increases in UVI are projected in the Northern Hemisphere except for RCP 8.5. At high latitudes, ozone recovery is well identified and induces a complete return of mean UVI levels to 1960 values for RCP 8.5 in the Southern Hemisphere. In the Northern Hemisphere, UVI levels in 2100 are higher by 0.5 % to 5.5 % for RCPs 2.6, 4.5 and 6.0 and they are lower by 7.9 % for RCP 8.5. We analysed the impacts of greenhouse gases (GHGs) and ozone-depleting substances (ODSs) on UVI from 1960 by comparing CCMI sensitivity simulations (1960–2100) with fixed GHGs or ODSs at their respective 1960 levels. As expected with ODS fixed at their 1960 levels, there is no large decrease in ozone levels and consequently no sudden increase in UVI levels. With fixed GHG, we observed a delayed return of ozone to 1960 values, with a corresponding pattern of change observed on UVI, and looking at the UVI difference between 2090s values and 1960s values, we found an 8 % increase in the tropical belt during the summer of each hemisphere. Finally we show that, while in the Southern Hemisphere the UVI is mainly driven by total ozone column, in the Northern Hemisphere both total ozone column and aerosol optical depth drive UVI levels, with aerosol optical depth having twice as much influence on the UVI as total ozone column does.

Volcanic eruptions impact climate through the injection of sulfur dioxide (SO2), which is oxidized to form sulfuric acid aerosol particles that can enhance the stratospheric aerosol optical depth (SAOD). Besides large-magnitude eruptions, moderate-magnitude eruptions such as Kasatochi in 2008 and Sarychev Peak in 2009 can have a significant impact on stratospheric aerosol and hence climate. However, uncertainties remain in quantifying the atmospheric and climatic impacts of the 2009 Sarychev Peak eruption due to limitations in previous model representations of volcanic aerosol microphysics and particle size, whilst biases have been identified in satellite estimates of post-eruption SAOD. In addition, the 2009 Sarychev Peak eruption co-injected hydrogen chloride (HCl) alongside SO2, whose potential stratospheric chemistry impacts have not been investigated to date. We present a study of the stratospheric SO2–particle–HCl processing and impacts following Sarychev Peak eruption, using the Community Earth System Model version 1.0 (CESM1) Whole Atmosphere Community Climate Model (WACCM) – Community Aerosol and Radiation Model for Atmospheres (CARMA) sectional aerosol microphysics model (with no a priori assumption on particle size). The Sarychev Peak 2009 eruption injected 0.9 Tg of SO2 into the upper troposphere and lower stratosphere (UTLS), enhancing the aerosol load in the Northern Hemisphere. The post-eruption evolution of the volcanic SO2 in space and time are well reproduced by the model when compared to Infrared Atmospheric Sounding Interferometer (IASI) satellite data. Co-injection of 27 Gg HCl causes a lengthening of the SO2 lifetime and a slight delay in the formation of aerosols, and acts to enhance the destruction of stratospheric ozone and mono-nitrogen oxides (NOx) compared to the simulation with volcanic SO2 only. We therefore highlight the need to account for volcanic halogen chemistry when simulating the impact of eruptions such as Sarychev on stratospheric chemistry. The model-simulated evolution of effective radius (reff) reflects new particle formation followed by particle growth that enhances reff to reach up to 0.2 µm on zonal average. Comparisons of the model-simulated particle number and size distributions to balloon-borne in situ stratospheric observations over Kiruna, Sweden, in August and September 2009, and over Laramie, USA, in June and November 2009 show good agreement and quantitatively confirm the post-eruption particle enhancement. We show that the model-simulated SAOD is consistent with that derived from the Optical Spectrograph and InfraRed Imager System (OSIRIS) when both the saturation bias of OSIRIS and the fact that extinction profiles may terminate well above the tropopause are taken into account. Previous modelling studies (involving assumptions on particle size) that reported agreement with (biased) post-eruption estimates of SAOD derived from OSIRIS likely underestimated the climate impact of the 2009 Sarychev Peak eruption.

Surface ultraviolet radiation (SUR) is not an increasing concern after the implementation of the Montreal Protocol and the recovery of the ozone layer Morgenstern et al.(2008). However, large uncertainties remain in the prediction of future changes of SUR Bais et al.(2015). Several studies pointed out that UV-B impacts the biosphere Erickson et al.(2015), especially the aquatic system, which plays a central part in the biogeochemical cycle Hader et al.(2007). It can affect phytoplankton productivity Smith and Cullen(1995). This influence can result in either positive or negative feedback on climate (Zepp et al., 2007). Global circulation model simulations predict an acceleration of the Brewer-Dobson circulation over the next century (Butchart, 2014), which would lead to a decrease in ozone levels in the tropics and an enhancement at higher latitudes (Hegglin and Shepherd, 2009). Reunion Island is located in the tropics (21° S, 55° E), in a part of the world where the amount of ozone in the ozone column is naturally low. In addition, this island is mountainous and the marine atmosphere is often clean with low aerosol concentrations. Thus, measurements show much higher SUR than at other sites at the same latitude or at midlatitudes. Ground-based measurements of SUR have been taken on Reunion Island by a Bentham DTMc300 spectroradiometer since 2009. This instrument is affiliated with the Network for the Detection of Atmospheric Composition Change (NDACC). In order to quantify the future evolution of SUR in the tropics, it is necessary to validate a model against present observations. This study is designed to be a preliminary parametric and sensitivity study of SUR modelling in the tropics. We developed a local parameterisation using the Tropospheric Ultraviolet and Visible Model (TUV; Madronich, 1993) and compared the output of TUV to multiple years of Bentham spectral measurements. This comparison started in early 2009 and continued until 2016. Only clear-sky SUR was modelled, so we needed to sort out the clear-sky measurements. We used two methods to detect cloudy conditions: the first was based on an observer's hourly report on the sky cover, while the second was based on applying Long and Ackerman(2000)'s algorithm to broadband pyranometer data to obtain the cloud fraction and then discriminating clear-sky windows on SUR measurements. Long et al. (2006)'s algorithm, with the co-located pyranometer data, gave better results for clear-sky filtering than the observer's report. Multiple model inputs were tested to evaluate the model sensitivity to different parameters such as total ozone column, aerosol optical properties, extraterrestrial spectrum or ozone cross section. For total column ozone, we used ground-based measurements from the SAOZ (Système d'Analyse par Observation Zénithale) spectrometer and satellite measurements from the OMI and SBUV instruments, while ozone profiles were derived from radio-soundings and the MLS ozone product. Aerosol optical properties came from a local aerosol climatology established using a Cimel photometer. Since the mean difference between various inputs of total ozone column was small, the corresponding response on UVI modelling was also quite small, at about 1 %. The radiative amplification factor of total ozone column on UVI was also compared for observations and the model. Finally, we were able to estimate UVI on Reunion Island with, at best, a mean relative difference of about 0.5 %, compared to clear-sky observations.

The major volcanic eruption of Mount Pinatubo in 1991 has been shown to have significant effects on stratospheric chemistry and ozone depletion even at midlatitudes. Since then, only moderate but recurrent volcanic eruptions have modulated the stratospheric aerosol loading and are assumed to be one cause for the reported increase in the global aerosol content over the past 15 years. This particularly enhanced aerosol context raises questions about the effects on stratospheric chemistry which depend on the latitude, altitude and season of injection. In this study, we focus on the midlatitude Sarychev volcano eruption in June 2009, which injected 0.9 Tg of sulfur dioxide (about 20 times less than Pinatubo) into a lower stratosphere mainly governed by high-stratospheric temperatures. Together with in situ measurements of aerosol amounts, we analyse high-resolution in situ and/or remote-sensing observations of NO2, HNO3 and BrO from balloon-borne infrared and UV–visible spectrometers launched in Sweden in August–September 2009. It is shown that differences between observations and three-dimensional (3-D) chemistry-transport model (CTM) outputs are not due to transport calculation issues but rather reflect the chemical impact of the volcanic plume below 19 km altitude. Good measurement–model agreement is obtained when the CTM is driven by volcanic aerosol loadings derived from in situ or space-borne data. As a result of enhanced N2O5 hydrolysis in the Sarychev volcanic aerosol conditions, the model calculates reductions of ∼ 45 % and increases of ∼ 11 % in NO2 and HNO3 amounts respectively over the August–September 2009 period. The decrease in NOx abundances is limited due to the expected saturation effect for high aerosol loadings. The links between the various chemical catalytic cycles involving chlorine, bromine, nitrogen and HOx compounds in the lower stratosphere are discussed. The increased BrO amounts (∼ 22 %) compare rather well with the balloon-borne observations when volcanic aerosol levels are accounted for in the CTM and appear to be mainly controlled by the coupling with nitrogen chemistry rather than by enhanced BrONO2 hydrolysis. We show that the chlorine partitioning is significantly controlled by enhanced BrONO2 hydrolysis. However, simulated effects of the Sarychev eruption on chlorine activation are very limited in the high-temperature conditions in the stratosphere in the period considered, inhibiting the effect of ClONO2 hydrolysis. As a consequence, the simulated chemical ozone loss due to the Sarychev aerosols is low with a reduction of −22 ppbv (−1.5 %) of the ozone budget around 16 km. This is at least 10 times lower than the maximum ozone depletion from chemical processes (up to −20 %) reported in the Northern Hemisphere lower stratosphere over the first year following the Pinatubo eruption. This study suggests that moderate volcanic eruptions have limited chemical effects when occurring at midlatitudes (restricted residence times) and outside winter periods (high-temperature conditions). However, it would be of interest to investigate longer-lasting tropical volcanic plumes or sulfur injections in the wintertime low-temperature conditions.

Spectral solar UV radiation measurements are performed in France using three spectroradiometers located at very different sites. One is installed in Villeneuve d'Ascq, in the north of France (VDA). It is an urban site in a topographically flat region. Another instrument is installed in Observatoire de Haute-Provence, located in the southern French Alps (OHP). It is a rural mountainous site. The third instrument is installed in Saint-Denis, Réunion Island (SDR). It is a coastal urban site on a small mountainous island in the southern tropics. The three instruments are affiliated with the Network for the Detection of Atmospheric Composition Change (NDACC) and carry out routine measurements to monitor the spectral solar UV radiation and enable derivation of UV index (UVI). The ground-based UVI values observed at solar noon are compared to similar quantities derived from the Ozone Monitoring Instrument (OMI, onboard the Aura satellite) and the second Global Ozone Monitoring Experiment (GOME-2, onboard the Metop-A satellite) measurements for validation of these satellite-based products. The present study concerns the period 2009–September 2012, date of the implementation of a new OMI processing tool. The new version (v1.3) introduces a correction for absorbing aerosols that were not considered in the old version (v1.2). Both versions of the OMI UVI products were available before September 2012 and are used to assess the improvement of the new processing tool. On average, estimates from satellite instruments always overestimate surface UVI at solar noon. Under cloudless conditions, the satellite-derived estimates of UVI compare satisfactorily with ground-based data: the median relative bias is less than 8 % at VDA and 4 % at SDR for both OMI v1.3 and GOME-2, and about 6 % for OMI v1.3 and 2 % for GOME-2 at OHP. The correlation between satellite-based and ground-based data is better at VDA and OHP (about 0.99) than at SDR (0.96) for both space-borne instruments. For all sky conditions, the median relative biases are much larger, with large dispersion for both instruments at all sites (VDA: about 12 %; OHP: 9 %; SDR: 11 %). Correlation between satellite-based and ground-based data is still better at VDA and OHP (about 0.95) than at SDR (about 0.73) for both satellite instruments. These results are explained considering the time of overpass of the two satellites, which is far from solar noon, preventing a good estimation of the cloud cover necessary for a good modelling of the UVI. Site topography and environment are shown to have a non-significant influence. At VDA and OHP, OMI v1.3 shows a significant improvement with respect to v1.2, which did not account for absorbing aerosols.

The 2014–2015 Holuhraun lava-flood eruption of Bárðarbunga volcano (Iceland) emitted prodigious amounts of sulfur dioxide into the atmosphere. This eruption caused a large-scale episode of air pollution throughout Western Europe in September 2014, the first event of this magnitude recorded in the modern era. We gathered chemistry-transport simulations and a wealth of complementary observations from satellite sensors (OMI, IASI), ground-based remote sensing (lidar, sunphotometry, differential optical absorption spectroscopy) and ground-level air quality monitoring networks to characterize both the spatial-temporal distributions of volcanic SO2 and sulfate aerosols as well as the dynamics of the planetary boundary layer. Time variations of dynamical and microphysical properties of sulfate aerosols in the aged low-tropospheric volcanic cloud, including loading, vertical distribution, size distribution and single scattering albedo, are provided. Retrospective chemistry-transport simulations at low horizontal resolution (25 km × 25 km) capture the correct temporal dynamics of this far-range air pollution event but fail to reproduce the correct magnitude of SO2 concentration at ground-level. Simulations at higher spatial resolution, relying on two nested domains with finest resolution of 7.3 km × 7.3 km, improve substantially the far-range vertical distribution of the volcanic cloud and subsequently the description of ground-level SO2 concentrations. However, remaining discrepancies between model and observations are shown to result from an inaccurate representation of the planetary boundary layer (PBL) dynamics. Comparison with lidar observations points out a systematic under-estimation of the PBL height by the model, whichever the PBL parameterization scheme. Such a shortcoming impedes the capture of the overlying Bárðarbunga cloud into the PBL at the right time and in sufficient quantities. This study therefore demonstrates the key role played by the PBL dynamics in accurately modelling large-scale volcanogenic air pollution.

Aerosols from the Sarychev volcano eruption (Kuril Islands, northeast of Japan) were observed in the Arctic lower stratosphere a few days after the strongest SO2 injection which occurred on 15 and 16 June 2009. From the observations provided by the Infrared Atmospheric Sounding Interferometer (IASI) an estimated 0.9 Tg of sulphur dioxide was injected into the upper troposphere and lower stratosphere (UTLS). The resultant stratospheric sulphate aerosols were detected from satellites by the Optical Spectrograph and Infrared Imaging System (OSIRIS) limb sounder and by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and from the surface by the Network for the Detection of Atmospheric Composition Changes (NDACC) lidar deployed at OHP (Observatoire de Haute-Provence, France). By the first week of July the aerosol plume had spread out over the entire Arctic region. The Sarychev-induced stratospheric aerosol over the Kiruna region (north of Sweden) was measured by the Stratospheric and Tropospheric Aerosol Counter (STAC) during eight balloon flights planned in August and September 2009. During this balloon campaign the Micro Radiomètre Ballon (MicroRADIBAL) and the Spectroscopie d'Absorption Lunaire pour l'Observation des Minoritaires Ozone et NOx (SALOMON) remote-sensing instruments also observed these aerosols. Aerosol concentrations returned to near-background levels by spring 2010. The effective radius, the surface area density (SAD), the aerosol extinction, and the total sulphur mass from STAC in situ measurements are enhanced with mean values in the range 0.15–0.21 μm, 5.5–14.7 μm2 cm−3, 5.5–29.5 × 10−4 km−1, and 4.9–12.6 × 10−10 kg[S] kg−1[air], respectively, between 14 km and 18 km. The observed and modelled e-folding time of sulphate aerosols from the Sarychev eruption is around 70–80 days, a value much shorter than the 12–14 months calculated for aerosols from the 1991 eruption of Mt Pinatubo. The OSIRIS stratospheric aerosol optical depth (AOD) at 750 nm is enhanced by a factor of 6, with a value of 0.02 in late July compared to 0.0035 before the eruption. The HadGEM2 and MIMOSA model outputs indicate that aerosol layers in polar region up to 14–15 km are largely modulated by stratosphere–troposphere exchange processes. The spatial extent of the Sarychev plume is well represented in the HadGEM2 model with lower altitudes of the plume being controlled by upper tropospheric troughs which displace the plume downward and upper altitudes around 18–20 km, in agreement with lidar observations. Good consistency is found between the HadGEM2 sulphur mass density and the value inferred from the STAC observations, with a maximum located about 1 km above the tropopause ranging from 1 to 2 × 10−9 kg[S] kg−1[air], which is one order of magnitude higher than the background level.

In order to test the validity of ultraviolet index (UVI) satellite products and UVI model simulations for general public information, intercomparison involving three satellite instruments (SCIAMACHY, OMI and GOME-2), the Chemistry and Transport Model, Modélisation de la Chimie Atmosphérique Grande Echelle (MOCAGE), and ground-based instruments was performed in 2008 and 2009. The intercomparison highlighted a systematic high bias of ~1 UVI in the OMI clear-sky products compared to the SCIAMACHY and TUV model clear-sky products. The OMI and GOME-2 all-sky products are close to the ground-based observations with a low 6 % positive bias, comparable to the results found during the satellite validation campaigns. This result shows that OMI and GOME-2 all-sky products are well appropriate to evaluate the UV-risk on health. The study has pointed out the difficulty to take into account either in the retrieval algorithms or in the models, the large spatial and temporal cloud modification effect on UV radiation. This factor is crucial to provide good quality UV information. OMI and GOME-2 show a realistic UV variability as a function of the cloud cover. Nevertheless these satellite products do not sufficiently take into account the radiation reflected by clouds. MOCAGE numerical forecasts show good results during periods with low cloud covers, but are actually not adequate for overcast conditions; this is why Météo-France currently uses human-expertised cloudiness (rather than direct outputs from Numerical Prediction Models) together with MOCAGE clear-sky UV indices for its operational forecasts. From now on, the UV monitoring could be done using free satellite products (OMI, GOME-2) and operational forecast for general public by using modelling, as long as cloud forecasts and the parametrisation of the impact of cloudiness on UV radiation are adequate.

Estimates of Aerosol Single Scattering Albedo (SSA) from ground-based spectral measurements in the UV-visible are conducted at Villeneuve d'Ascq (VdA) in France. In order to estimate this parameter, measurements of global and diffuse UV-visible solar irradiances performed under cloud-free conditions since 2003 with a spectroradiometer operated by the Laboratoire d'Optique Atmosphérique (LOA) are used. The technique consists in comparing the measured irradiance values to modelled irradiances computed for various SSA. The retrieval is restricted to the 330–450 nm range to avoid ozone influence. For validation purpose, the retrieved values of SSA at 440 nm are compared to the ones obtained from sunphotometer measurements of the AERONET/PHOTONS network available on the LOA site. The results are rather satisfying: for the period 2003–2006 the Root Mean Square (RMS) of the differences is about 0.05, this value is within the uncertainty domain of retrieval of both products. Distinction between days characterized by different aerosol content, by means of the aerosol optical thickness (AOT) retrieved from ground-based measurements at the same wavelength, shows that the comparisons between both products are better when AOT are higher. Indeed in case AOT are greater than 0.2, the RMS is 0.031 compared to 0.060 for days with an AOT lower than 0.2. The SSA estimated at 340 and 380 nm from ground-based spectra are also studied, though no validation can be carried out with sunphotometer data (440 nm is the shortest wavelength at which the SSA is provided by the network). The good comparisons observed at 440 nm can let assume that the SSA retrieved from spectroradiometer measurements at the two other wavelengths are also obtained with a good confidence level. Thus these values in the UV range can be used to complete aerosol data provided by AERONET/PHOTONS at VdA. Moreover they can be used for a best knowledge of the aerosol absorption that is necessary to quantify the error on surface UV irradiances estimated from satellites.

The aerosol Single Scattering Albedo (SSA) and Absorbing Aerosol Optical Depth (AAOD) at 320.1 nm are derived at Rome site by the comparison between Brewer and modelled spectra. The UVSPEC radiative transfer model is used to calculate the UV irradiances for different SSA values, taking into account as input data total ozone and Aerosol Optical Depth (AOD) obtained from Brewer spectral measurements. The accuracy in determining SSA depends on the aerosol amount and on Solar Zenith Angle (SZA) value: SSA uncertainty increases when AOD and SZA decrease. The monthly mean values of SSA and AAOD during the period January 2005–June 2008 are analysed, showing a monthly and seasonal variability. It is found that the SSA and AAOD averages are 0.80±0.08 and 0.056±0.028, respectively. AAOD retrievals are also used to quantify the error in the Ozone Monitoring Instrument (OMI) surface UV products due to absorbing aerosols, not included in the current OMI UV algorithm. OMI and Brewer UV irradiances at 324.1 nm and Erythemal Dose Rates (EDRs) under clear sky conditions, are compared as a function of AAOD. Three methods are considered to investigate on the applicability of an absorbing aerosol correction on OMI UV data at Rome site. Depending on the correction methodology, the bias value decreases from 18% to 2% for spectral irradiance at 324.1 nm and from 25% to 8% for EDR.

This paper presents extensive {bias determination} analyses of ozone observations from the Atmospheric Chemistry Experiment (ACE) satellite instruments: the ACE Fourier Transform Spectrometer (ACE-FTS) and the Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (ACE-MAESTRO) instrument. Here we compare the latest ozone data products from ACE-FTS and ACE-MAESTRO with coincident observations from nearly 20 satellite-borne, airborne, balloon-borne and ground-based instruments, by analysing volume mixing ratio profiles and partial column densities. The ACE-FTS version 2.2 Ozone Update product reports more ozone than most correlative measurements from the upper troposphere to the lower mesosphere. At altitude levels from 16 to 44 km, the average values of the mean relative differences are nearly all within +1 to +8%. At higher altitudes (45–60 km), the ACE-FTS ozone amounts are significantly larger than those of the comparison instruments, with mean relative differences of up to +40% (about +20% on average). For the ACE-MAESTRO version 1.2 ozone data product, mean relative differences are within ±10% (average values within ±6%) between 18 and 40 km for both the sunrise and sunset measurements. At higher altitudes (~35–55 km), systematic biases of opposite sign are found between the ACE-MAESTRO sunrise and sunset observations. While ozone amounts derived from the ACE-MAESTRO sunrise occultation data are often smaller than the coincident observations (with mean relative differences down to −10%), the sunset occultation profiles for ACE-MAESTRO show results that are qualitatively similar to ACE-FTS, indicating a large positive bias (mean relative differences within +10 to +30%) in the 45–55 km altitude range. In contrast, there is no significant systematic difference in bias found for the ACE-FTS sunrise and sunset measurements.

Routine measurements of global and diffuse UV irradiances at Briançon station (1310 m a.s.l.) are used to retrieve the direct solar irradiance and the aerosol optical depth (AOD), for cloudless days. Data of three years (2003, 2004, 2005) are analyzed; the results confirm those of a preliminary analysis for 2001, 2002. The atmosphere is very clear in winter, with AODs between 0.05 and 0.1. The turbidity increases slowly in spring, starting end of February, with AODs around 0.2–0.3 in mid summer, some values reaching 0.4. A similar behaviour is observed for all years, with somewhat higher values in late summer for the year 2003.

Vertical profiles of NO2 and NO have been obtained from solar occultation measurements by the Atmospheric Chemistry Experiment (ACE), using an infrared Fourier Transform Spectrometer (ACE-FTS) and (for NO2) an ultraviolet-visible-near-infrared spectrometer, MAESTRO (Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation). In this paper, the quality of the ACE-FTS version 2.2 NO2 and NO and the MAESTRO version 1.2 NO2 data are assessed using other solar occultation measurements (HALOE, SAGE II, SAGE III, POAM III, SCIAMACHY), stellar occultation measurements (GOMOS), limb measurements (MIPAS, OSIRIS), nadir measurements (SCIAMACHY), balloon-borne measurements (SPIRALE, SAOZ) and ground-based measurements (UV-VIS, FTIR). Time differences between the comparison measurements were reduced using either a tight coincidence criterion, or where possible, chemical box models. ACE-FTS NO2 and NO and the MAESTRO NO2 are generally consistent with the correlative data. The ACE-FTS and MAESTRO NO2 volume mixing ratio (VMR) profiles agree with the profiles from other satellite data sets to within about 20% between 25 and 40 km, with the exception of MIPAS ESA (for ACE-FTS) and SAGE II (for ACE-FTS (sunrise) and MAESTRO) and suggest a negative bias between 23 and 40 km of about 10%. MAESTRO reports larger VMR values than the ACE-FTS. In comparisons with HALOE, ACE-FTS NO VMRs typically (on average) agree to ±8% from 22 to 64 km and to +10% from 93 to 105 km, with maxima of 21% and 36%, respectively. Partial column comparisons for NO2 show that there is quite good agreement between the ACE instruments and the FTIRs, with a mean difference of +7.3% for ACE-FTS and +12.8% for MAESTRO.

Global and diffuse UV-visible solar irradiances are routinely measured since 2003 with a spectroradiometer operated by the Laboratoire d'Optique Atmosphérique (LOA) located in Villeneuve d'Ascq, France. The analysis of the direct irradiance derived by cloudless conditions enables retrieving the aerosol optical thickness (AOT) spectrum in the 330–450 nm range. The site hosts also sunphotometers from the AERONET/PHOTONS network performing routinely measurements of the AOT at several wavelengths. On one hand, comparisons between the spectroradiometer and the sunphotometer AOT at 440 nm as well as, when available, at 340 and 380 nm, show good agreement: in 2003–2005 at 440 nm the correlation coefficient, the slope and the intercept of the regression line are [0.97, 0.95, 0.025], and in 2006 at 440, 380 and 340 nm they are [0.97, 1.00, −0.013], [0.97, 0.98, −0.007], and [0.98, 0.98, −0.002] respectively. On the other hand, the AOT's spectral variations have been compared using the Angström exponents derived from AOT data at 340 and 440 nm for both instruments. The comparisons show that this parameter is difficult to retrieve accurately due to the small wavelength range and due to the weak AOT values. Thus, AOT derived at wavelengths outside the spectroradiometer range by means of an extrapolation using the Angström parameter would have large uncertainties, whereas spectroradiometer's spectral AOT could be used for direct validation of other AOT, such as those provided by satellite instruments.

Ozone Monitoring Instrument (OMI), launched in July 2004, is dedicated to the monitoring of the Earth's ozone, air quality and climate. OMI is the successor of the Total Ozone Mapping Spectrometer (TOMS) instruments and provides among other atmospheric and radiometric quantities the total column of ozone (TOC), the surface ultraviolet (UV) irradiance at several wavelengths, the erythemal dose rates and the erythemal daily doses. The main objective of this work is to compare OMI data with data from ground-based instruments in order to use OMI products (collection 2) for scientific studies. The Laboratoire d'Optique Atmosphérique (LOA) located in Villeneuve d'Ascq (VdA) in the north of France performs solar UV measurements using a spectroradiometer. The site of Briançon in the French Southern Alps is also equipped with a spectroradiometer operated by Interaction Rayonnement Solaire Atmosphère (IRSA). The OMI total ozone column data is obtained from the OMI-TOMS and OMI-DOAS algorithms. The comparison between the TOC retrieved with ground-based measurements and OMI-TOMS data shows good agreement at both sites for all sky conditions with a relative difference for most of points better than 5%. For OMI-DOAS data, the agreement is generally better than 7% and these data show a significant dependence on solar zenith angle. Comparisons of spectral UV on clear sky conditions are also satisfying with relative differences smaller than 10% except at solar zenith angles larger than 65°. On the contrary, results of comparisons of the erythemal dose rates and erythemal daily doses for clear sky show that OMI overestimates surface UV doses at VdA by about 15% and that on cloudy skies, the bias increases. At Briançon, such a bias is observed if data corresponding to snow-covered surface are excluded.

The ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) solar occultation instrument that was launched onboard the Canadian SCISAT-1 satellite in August 2003 is measuring vertical profiles from the upper troposphere to the lower mesosphere for a large number of atmospheric constituents. Methane is one of the key species. The version v2.2 data of the ACE-FTS CH4 data have been compared to correlative satellite, balloon-borne and ground-based Fourier transform infrared remote sensing data to assess their quality. The comparison results indicate that the accuracy of the data is within 10% in the upper troposphere – lower stratosphere, and within 25% in the middle and higher stratosphere up to the lower mesosphere (

The Canadian ACE (Atmospheric Chemistry Experiment) mission is dedicated to the retrieval of a large number of atmospheric trace gas species using the solar occultation technique in the infrared and UV/visible spectral domain. However, two additional solar disk imagers (at 525 nm and 1020 nm) were added for a number of reasons, including the retrieval of aerosol and cloud products. In this paper, we present first comparison results for these imager aerosol/cloud optical extinction coefficient profiles, with the ones derived from measurements performed by 3 solar occultation instruments (SAGE II, SAGE III, POAM III), one stellar occultation instrument (GOMOS) and one limb sounder (OSIRIS). The results indicate that the ACE imager profiles are of good quality in the upper troposphere/lower stratosphere, although the aerosol extinction for the visible channel at 525 nm contains a significant negative bias at higher altitudes, while the relative differences indicate that ACE profiles are almost always too high at 1020 nm. Both problems are probably related to ACE imager instrumental issues.