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Detection of climate change requires a network of stable ground-based long-term measurements. Building upon earlier work, we first explore requirements of such measurements (such as maximum random uncertainty and sampling frequency) to ensure a minimum random uncertainty in monthly mean temperatures and to ensure effective detection of trends. In agreement with previous work we find that only for individual measurement random uncertainties >0.2K does the measurement random uncertainty start to contribute significantly to the random uncertainty in the monthly mean. For trend analysis, we find that the quality of the trend determination is only compromised when the measurement random uncertainty exceeds 2K and measurements are made just once or twice a month. In the second part of the study we provide guidance on how to most effectively design a measurement network. To this end we developed a method to objectively identify the optimal location of sites for detecting projected trends in upper-air temperatures and total column ozone in the shortest possible time. This is done by first estimating the spatial distribution of the minimum length of time during which measurements have to be made in order to detect projected trends in temperature and ozone. This quantity is calculated from the unforced variance in the signal and the degree of autocorrelation, both estimated from historical data sets and assumed not to change in the future, and the projected trends as estimated from chemistry-climate models. The optimal site locations are then selected by an iterative procedure based on the minimum time required to detect a trend and a minimal distance between different measurement sites. While the optimal sites identified here result from our use of only one of a wide range of objective strategies, these results provide additional incentives for initiating measurement programmes at these sites or, if already in operation, to continue to be supported. [ABSTRACT FROM AUTHOR]

Denitrification within the stratospheric vortex is a crucial process for Antarctic ozone hole formation, resulting in an analogous stratospheric "nitrogen hole". Sedimentation of large nitric acid trihydrate polar stratospheric cloud particles within the Antarctic polar stratospheric vortex that form during winter depletes the inner vortex of nitrogen oxides. Here, 2018–2021 daily TROPOspheric Monitoring Instrument (TROPOMI) measurements are used for the first time for a detailed characterization of this nitrogen hole. Nitrogen dioxide total columns exhibit strong spatiotemporal and seasonal variations associated with photochemistry as well as transport and mixing processes. Combined with total ozone column data two main regimes are identified: inner-vortex ozone- and nitrogen-dioxide-depleted air and outer-vortex air enhanced in ozone and nitrogen dioxide. Within the vortex total ozone and total stratospheric nitrogen dioxide are strongly correlated, which is much less evident outside of the vortex. Connecting the two main regimes is a third regime of coherent patterns in the total nitrogen dioxide column–total ozone column phase space – defined here as "mixing lines". These mixing lines exist because of differences in three-dimensional variations of nitrogen dioxide and ozone, thereby providing information about vortex dynamics and cross-vortex edge mixing. On the other hand, interannual variability of nitrogen dioxide–total ozone characteristics is rather small except in 2019 when the vortex was unusually unstable. Overall, the results show that daily stratospheric nitrogen dioxide column satellite measurements provide an innovative means for characterizing polar stratospheric denitrification processes, vortex dynamics, and long-term monitoring of Antarctic ozone hole conditions. [ABSTRACT FROM AUTHOR]

Observations of nitrogen dioxide (NO 2) and nitrogen oxide (NO) in the stratosphere are relevant to understand long-term changes and variabilities in stratospheric nitrogen oxide (NO x) and ozone (O 3) concentrations. Due to the versatile role of NO 2 and NO in stratospheric O 3 photochemistry, they are important for recovery and build-up of O 3 holes in the stratosphere and therefore can indirectly affect human life. Thus, we present in this work the evaluation of NO 2 and NO stratospheric partial columns (> 16 km altitude) retrieved from ground-based Fourier-transform infrared (FTIR) measurements of over 25 years at Zugspitze (47.42° N, 10.98° E; 2964 m a.s.l.) and 18 years at Garmisch (47.47° N, 11.06° E; 745 m a.s.l.), Germany. The obtained stratospheric columns are only weakly influenced by tropospheric pollution and show only a very small bias of 2.5 ± 0.2 % when comparing NO 2 above Zugspitze and Garmisch. Stratospheric columns of both NO 2 and NO show a diurnal increase that depends on local solar time (LST). We quantified this behavior by calculating diurnal increasing rates. Here, we find mean values for the NO 2 diurnal increasing rate of (0.89 ± 0.14) × 10 14 and (0.94 ± 0.14) × 10 14 cm -2 h -1 at Zugspitze and Garmisch, respectively. The mean NO morning diurnal increasing rate above Zugspitze is found to be (1.42 ± 0.12) × 10 14 cm -2 h -1. Regarding the seasonal dependency of these increasing rates, for the first time, we were able to experimentally detect a significant seasonal variation in both NO 2 diurnal increasing rates and NO morning diurnal increasing rates with a maximum of (1.13 ± 0.04) × 10 14 cm -1 h -1 for NO 2 and (1.76 ± 0.25) × 10 14 cm -1 h -1 for NO in September and a minimum of (0.71 ± 0.18) × 10 14 cm -1 h -1 in December for NO 2 and a minimum of (1.18 ± 0.41) × 10 14 cm -1 h -1 in November for NO. This similar behavior may be explained by the interconnection of both species in stratospheric photochemistry. The outcome of this work is a retrieval and analysis strategy of FTIR data for NO x stratospheric columns, which can help to further validate photochemical models or improve satellite validations. The first use of this data set is shown in the companion paper (Nürnberg et al., 2023) wherein experiment-based NO x scaling factors describing the diurnal increase in the retrieved partial columns are extracted and recently published model-based scaling factors are validated. [ABSTRACT FROM AUTHOR]

Heatwaves are a substantial health threat in the UK, exacerbated by co-occurrence of ozone pollution episodes. Here we report on the first use of retrieved vertical profiles of nitrogen dioxide (NO2) and formaldehyde (HCHO) over Central London from a newly installed multi-axis differential optical absorption spectroscopy (MAX-DOAS) instrument coincident with two of three heatwaves for the hottest summer on record. We evaluate space-based sensor observations routinely used to quantify temporal changes in air pollution and precursor emissions over London. Collocated daily mean tropospheric column densities from the high-spatial-resolution space-based TROPOspheric Monitoring Instrument (TROPOMI) and MAX-DOAS, after accounting for differences in vertical sensitivities, are temporally consistent for NO2 and HCHO (both R = 0.71). TROPOMI NO2 is 27 %–31 % less than MAX-DOAS NO2 , as expected from horizontal dilution of NO2 by TROPOMI pixels in polluted cities. TROPOMI HCHO is 20 % more than MAX-DOAS HCHO , greater than differences in past validation studies but within the range of systematic errors in the MAX-DOAS retrieval. The MAX-DOAS near-surface (0–110 m) retrievals have similar day-to-day and hourly variability to the surface sites for comparison of NO2 (R ≥ 0.7) and for MAX-DOAS HCHO versus surface site isoprene (R ≥ 0.7) that oxidises to HCHO in prompt and high yields. Daytime ozone production, diagnosed with MAX-DOAS HCHO -to- NO2 tropospheric vertical column ratios, is mostly limited by availability of volatile organic compounds (VOCs), except on heatwave days. Temperature-dependent biogenic VOC emissions of isoprene increase exponentially, resulting in ozone concentrations that exceed the regulatory standard for ozone and cause non-compliance at urban background sites in Central London. Locations in Central London heavily influenced by traffic remain in compliance, but this is likely to change with stricter controls on vehicle emissions of NOx and higher likelihood of heatwave frequency, severity, and persistence due to anthropogenic climate change. [ABSTRACT FROM AUTHOR]

A new technique was used to directly measure O 3 response to changes in precursor NO x and volatile organic compound (VOC) concentrations in the atmosphere using three identical Teflon smog chambers equipped with UV lights. One chamber served as the baseline measurement for O 3 formation, one chamber added NO x , and one chamber added surrogate VOCs (ethylene, m -xylene, n -hexane). Comparing the O 3 formation between chambers over a 3-hour UV cycle provides a direct measurement of O 3 sensitivity to precursor concentrations. Measurements made with this system at Sacramento, California, between April–December 2020 revealed that the atmospheric chemical regime followed a seasonal cycle. O 3 formation was VOC-limited (NO x -rich) during the early spring, transitioned to NO x -limited during the summer due to increased concentrations of ambient VOCs with high O 3 formation potential, and then returned to VOC-limited (NO x -rich) during the fall season as the concentrations of ambient VOCs decreased and NO x increased. This seasonal pattern of O 3 sensitivity is consistent with the cycle of biogenic emissions in California. The direct chamber O 3 sensitivity measurements matched semi-direct measurements of HCHO/NO2 ratios from the TROPOspheric Monitoring Instrument (TROPOMI) aboard the Sentinel-5 Precursor (Sentinel-5P) satellite. Furthermore, the satellite observations showed that the same seasonal cycle in O 3 sensitivity occurred over most of the entire state of California, with only the urban cores of the very large cities remaining VOC-limited across all seasons. The O 3 -nonattainment days (MDA8 O 3>70 ppb) have O 3 sensitivity in the NO x -limited regime, suggesting that a NO x emissions control strategy would be most effective at reducing these peak O 3 concentrations. In contrast, a large portion of the days with MDA8 O 3 concentrations below 55 ppb were in the VOC-limited regime, suggesting that an emissions control strategy focusing on NO x reduction would increase O 3 concentrations. This challenging situation suggests that emissions control programs that focus on NO x reductions will immediately lower peak O 3 concentrations but slightly increase intermediate O 3 concentrations until NO x levels fall far enough to re-enter the NO x -limited regime. The spatial pattern of increasing and decreasing O 3 concentrations in response to a NO x emissions control strategy should be carefully mapped in order to fully understand the public health implications. [ABSTRACT FROM AUTHOR]

Nitrogen oxides (NO x , NO + NO 2) are potent air pollutants which directly impact on human health and which aid the formation of other hazardous pollutants such as ozone (O 3) and particulate matter. In this study, we use satellite tropospheric column nitrogen dioxide (TCNO 2) data to evaluate the spatiotemporal variability and magnitude of the United Kingdom (UK) bottom-up National Atmospheric Emissions Inventory (NAEI) NO x emissions. Although emissions and TCNO 2 represent different quantities, for UK city sources we find a spatial correlation of ∼0.5 between the NAEI NO x emissions and TCNO 2 from the high-spatial-resolution TROPOspheric Monitoring Instrument (TROPOMI), suggesting a good spatial distribution of emission sources in the inventory. Between 2005 and 2015, the NAEI total UK NO x emissions and long-term TCNO 2 record from the Ozone Monitoring Instrument (OMI), averaged over England, show annually decreasing trends of 4.4 % and 2.2 %, respectively. Top-down NO x emissions were derived in this study by applying a simple mass balance approach to TROPOMI-observed downwind NO 2 plumes from city sources. Overall, these top-down estimates were consistent with the NAEI, but for larger cities such as London and Birmingham the inventory is significantly (>25 %) less than the top-down emissions. [ABSTRACT FROM AUTHOR]

The occurrence of tropospheric ozone depletion events (ODEs) in the Antarctic can be influenced by many factors, such as the total ozone column (TOC). In this study, we analyzed the observational data obtained from ground observation stations and used two numerical models (TUV and KINAL), to discover the relationship between the TOC and the occurrence of ODEs in the Antarctic. A sensitivity analysis was also performed on ozone and major bromine species (BrO , HOBr and HBr) to find out key photolysis reactions determining the impact on the occurrence of tropospheric ODEs brought by TOC. From the analysis of the observational data and the numerical results, we suggest that the occurrence frequency of ODEs in the Antarctic is negatively associated with TOC, after screening out the impact on ODEs caused by the solar zenith angle (SZA). This negative impact of TOC on the occurrence of ODEs was suggested to be exerted through altering the solar radiation reaching the ground surface and changing the rates of photolysis reactions. Moreover, major ODE accelerating reactions (i.e., photolysis of tropospheric ozone, H2O2 and HCHO) and decelerating reactions (i.e., photolysis of BrO and HOBr), which heavily control the start of ODEs, were also identified. We found that when TOC decreases, the major ODE accelerating reactions significantly speed up. In contrast, the major ODE decelerating reactions are only slightly affected. As a result of the different impacts of TOC on photolysis reactions, the occurrence of ODEs depends negatively on TOC. [ABSTRACT FROM AUTHOR]

Questions about how emissions are changing during the COVID-19 lockdown periods cannot be answered by observations of atmospheric trace gas concentrations alone, in part due to simultaneous changes in atmospheric transport, emissions, dynamics, photochemistry, and chemical feedback. A chemical transport model simulation benefiting from a multi-species inversion framework using well-characterized observations should differentiate those influences enabling to closely examine changes in emissions. Accordingly, we jointly constrain NO x and VOC emissions using well-characterized TROPOspheric Monitoring Instrument (TROPOMI) HCHO and NO 2 columns during the months of March, April, and May 2020 (lockdown) and 2019 (baseline). We observe a noticeable decline in the magnitude of NO x emissions in March 2020 (14 %–31 %) in several major cities including Paris, London, Madrid, and Milan, expanding further to Rome, Brussels, Frankfurt, Warsaw, Belgrade, Kyiv, and Moscow (34 %–51 %) in April. However, NO x emissions remain at somewhat similar values or even higher in some portions of the UK, Poland, and Moscow in March 2020 compared to the baseline, possibly due to the timeline of restrictions. Comparisons against surface monitoring stations indicate that the constrained model underrepresents the reduction in surface NO 2. This underrepresentation correlates with the TROPOMI frequency impacted by cloudiness. During the month of April, when ample TROPOMI samples are present, the surface NO 2 reductions occurring in polluted areas are described fairly well by the model (model: - 21 ± 17 %, observation: - 29 ± 21 %). The observational constraint on VOC emissions is found to be generally weak except for lower latitudes. Results support an increase in surface ozone during the lockdown. In April, the constrained model features a reasonable agreement with maximum daily 8 h average (MDA8) ozone changes observed at the surface (r=0.43), specifically over central Europe where ozone enhancements prevail (model: + 3.73 ± 3.94 %, + 1.79 ppbv, observation: + 7.35 ± 11.27 %, + 3.76 ppbv). The model suggests that physical processes (dry deposition, advection, and diffusion) decrease MDA8 surface ozone in the same month on average by - 4.83 ppbv, while ozone production rates dampened by largely negative JNO2 [NO 2 ]- kNO+O3 [NO][O 3 ] become less negative, leading ozone to increase by + 5.89 ppbv. Experiments involving fixed anthropogenic emissions suggest that meteorology contributes to 42 % enhancement in MDA8 surface ozone over the same region with the remaining part (58 %) coming from changes in anthropogenic emissions. Results illustrate the capability of satellite data of major ozone precursors to help atmospheric models capture ozone changes induced by abrupt emission anomalies. [ABSTRACT FROM AUTHOR]

Starting in 1969 and comprising three launches a week, the Uccle (Brussels, Belgium) ozonesonde dataset is one of longest and densest in the world. Moreover, as the only major change was the switch from Brewer-Mast (BM) to electrochemical concentration cell (ECC) ozonesonde types in 1997 (when the emissions of ozone-depleting substances peaked), the Uccle time series is very homogenous. In this paper, we briefly describe the efforts that were undertaken during the first 3 decades of the 50 years of ozonesonde observations to guarantee the homogeneity between ascent and descent profiles, under changing environmental conditions (e.g. SO 2), and between the different ozonesonde types. This paper focuses on the 50-year-long Uccle ozonesonde dataset and aims to demonstrate its past, present, and future relevance to ozone research in two application areas: (i) the assessment of the temporal evolution of ozone from the surface to the (middle) stratosphere, and (ii) as the backbone for validation and stability analysis of both stratospheric and tropospheric satellite ozone retrievals. Using the Long-term Ozone Trends and Uncertainties in the Stratosphere (LOTUS) multiple linear regression model (SPARC/IO3C/GAW, 2019), we found that the stratospheric ozone concentrations at Uccle have declined at a significant rate of around 2 % per decade since 1969, which is also rather consistent over the different stratospheric levels. This overall decrease can mainly be assigned to the 1969–1996 period with a rather consistent rate of decrease of around - 4 % per decade. Since 2000, a recovery of between + 1 % per decade and + 3 % per decade of the stratospheric ozone levels above Uccle has been observed, although it is not significant and is not seen for the upper stratospheric levels measured by ozonesondes. Throughout the entire free troposphere, a very consistent increase in the ozone concentrations of 2 % per decade to 3 % per decade has been measured since both 1969 and 1995, with the trend since 1995 being in almost perfect agreement with the trends derived from the In-service Aircraft for a Global Observing System (IAGOS) ascent/descent profiles at Frankfurt. As the number of tropopause folding events in the Uccle time series has increased significantly over time, increased stratosphere-to-troposphere transport of recovering stratospheric ozone might partly explain these increasing tropospheric ozone concentrations, despite the levelling-off of (tropospheric) ozone precursor emissions and notwithstanding the continued increase in mean surface ozone concentrations. Furthermore, we illustrate the crucial role of ozonesonde measurements for the validation of satellite ozone profile retrievals. With the operational validation of the Global Ozone Monitoring Experiment-2 (GOME-2), we show how the Uccle dataset can be used to evaluate the performance of a degradation correction for the MetOp-A/GOME-2 UV (ultraviolet) sensors. In another example, we illustrate that the Microwave Limb Sounder (MLS) overpass ozone profiles in the stratosphere agree within ± 5 % with the Uccle ozone profiles between 10 and 70 hPa. Another instrument on the same Aura satellite platform, the Tropospheric Emission Spectrometer (TES), is generally positively biased with respect to the Uccle ozonesondes in the troposphere by up to ∼ 10 ppbv, corresponding to relative differences of up to ∼ 15 %. Using the Uccle ozonesonde time series as a reference, we also demonstrate that the temporal stability of those last two satellite retrievals is excellent. [ABSTRACT FROM AUTHOR]

The National Institute of Water and Atmospheric Research/Bodeker Scientific (NIWA–BS) total column ozone (TCO) database and the associated BS-filled TCO database have been updated to cover the period 1979 to 2019, bringing both to version 3.5.1 (V3.5.1). The BS-filled database builds on the NIWA–BS database by using a machine-learning algorithm to fill spatial and temporal data gaps to provide gap-free TCO fields over Antarctica. These filled TCO fields then provide a more complete picture of wintertime changes in the ozone layer over Antarctica. The BS-filled database has been used to calculate continuous, homogeneous time series of indicators of Antarctic ozone depletion from 1979 to 2019, including (i) daily values of the ozone mass deficit based on TCO below a 220 DU threshold; (ii) daily measures of the area over Antarctica where TCO levels are below 150 DU , below 220 DU , more than 30 % below 1979 to 1981 climatological means, and more than 50 % below 1979 to 1981 climatological means; (iii) the date of disappearance of 150 DU TCO values, 220 DU TCO values, values 30 % or more below 1979 to 1981 climatological means, and values 50 % or more below 1979 to 1981 climatological means, for each year; and (iv) daily minimum TCO values over the range 75 to 90 ∘ S equivalent latitude. Since both the NIWA–BS and BS-filled databases provide uncertainties on every TCO value, the Antarctic ozone depletion metrics are provided, for the first time, with fully traceable uncertainties. To gain insight into how the vertical distribution of ozone over Antarctica has changed over the past 36 years, ozone concentrations, combined and homogenized from several satellite-based ozone monitoring instruments as well as the global ozonesonde network, were also analysed. A robust attribution to changes in the drivers of long-term secular variability in these metrics has not been performed in this analysis. As a result, statements about the recovery of Antarctic TCO from the effects of ozone-depleting substances cannot be made. That said, there are clear indications of a change in trend in many of the metrics reported on here around the turn of the century, close to when Antarctic stratospheric concentrations of chlorine and bromine peaked. [ABSTRACT FROM AUTHOR]

Within the framework of the International Arctic Systems for Observing the Atmosphere (IASOA), we report a modelling-based study on surface ozone across the Arctic. We use surface ozone from six sites – Summit (Greenland), Pallas (Finland), Barrow (USA), Alert (Canada), Tiksi (Russia), and Villum Research Station (VRS) at Station Nord (North Greenland, Danish realm) – and ozone-sonde data from three Canadian sites: Resolute, Eureka, and Alert. Two global chemistry models – a global chemistry transport model (parallelised-Tropospheric Offline Model of Chemistry and Transport, p-TOMCAT) and a global chemistry climate model (United Kingdom Chemistry and Aerosol, UKCA) – are used for model data comparisons. Remotely sensed data of BrO from the GOME-2 satellite instrument and ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) at Eureka, Canada, are used for model validation. The observed climatology data show that spring surface ozone at coastal sites is heavily depleted, making ozone seasonality at Arctic coastal sites distinctly different from that at inland sites. Model simulations show that surface ozone can be greatly reduced by bromine chemistry. In April, bromine chemistry can cause a net ozone loss (monthly mean) of 10–20 ppbv, with almost half attributable to open-ocean-sourced bromine and the rest to sea-ice-sourced bromine. However, the open-ocean-sourced bromine, via sea spray bromide depletion, cannot by itself produce ozone depletion events (ODEs; defined as ozone volume mixing ratios, VMRs, < 10 ppbv). In contrast, sea-ice-sourced bromine, via sea salt aerosol (SSA) production from blowing snow, can produce ODEs even without bromine from sea spray, highlighting the importance of sea ice surface in polar boundary layer chemistry. Modelled total inorganic bromine (Br Y) over the Arctic sea ice is sensitive to model configuration; e.g. under the same bromine loading, Br Y in the Arctic spring boundary layer in the p-TOMCAT control run (i.e. with all bromine emissions) can be 2 times that in the UKCA control run. Despite the model differences, both model control runs can successfully reproduce large bromine explosion events (BEEs) and ODEs in polar spring. Model-integrated tropospheric-column BrO generally matches GOME-2 tropospheric columns within ∼ 50 % in UKCA and a factor of 2 in p-TOMCAT. The success of the models in reproducing both ODEs and BEEs in the Arctic indicates that the relevant parameterizations implemented in the models work reasonably well, which supports the proposed mechanism of SSA production and bromide release on sea ice. Given that sea ice is a large source of SSA and halogens, changes in sea ice type and extent in a warming climate will influence Arctic boundary layer chemistry, including the oxidation of atmospheric elemental mercury. Note that this work dose not necessary rule out other possibilities that may act as a source of reactive bromine from the sea ice zone. [ABSTRACT FROM AUTHOR]

Reliable ozone trends after 2000 are essential to detect early ozone recovery. However, the long-term ground-based and satellite ozone profile trends reported in the literature show a high variability. There are multiple reasons for variability in the reported long-term trends such as the measurement timing and the dataset quality. The Payerne Switzerland microwave radiometer (MWR) ozone trends are significantly positive at 2 % to 3 % per decade in the upper stratosphere (5–1 hPa , 35–48 km), with a high variation with altitude. This is in accordance with the Northern Hemisphere (NH) trends reported by other ground-based instruments in the SPARC LOTUS project. In order to determine what part of the variability between different datasets comes from measurement timing, Payerne MWR and SOCOL v3.0 chemistry–climate model (CCM) trends were estimated for each hour of the day with a multiple linear regression model. Trends were quantified as a function of local solar time (LST). In the middle and upper stratosphere, differences as a function of LST are reported for both the MWR and simulated trends for the post-2000 period. However, these differences are not significant at the 95 % confidence level. In the lower mesosphere (1–0.1 hPa , 48–65 km), the 2010–2018 day- and nighttime trends have been considered. Here again, the variation in the trend with LST is not significant at the 95 % confidence level. Based on these results we conclude that significant trend differences between instruments cannot be attributed to a systematic temporal sampling effect. The dataset quality is of primary importance in a reliable trend derivation, and multi-instrument comparison analyses can be used to assess the long-term stability of data records by estimating the drift and bias of instruments. The Payerne MWR dataset has been homogenized to ensure a stable measurement contribution to the ozone profiles and to take into account the effects of three major instrument upgrades. At each instrument upgrade, a correction offset has been calculated using parallel measurements or simultaneous measurements by an independent instrument. At pressure levels smaller than 0.59 hPa (above ∼50 km), the homogenization corrections to be applied to the Payerne MWR ozone profiles are dependent on LST. Due to the lack of reference measurements with a comparable measurement contribution at a high time resolution, a comprehensive homogenization of the sub-daily ozone profiles was possible only for pressure levels larger than 0.59 hPa. The ozone profile dataset from the Payerne MWR, Switzerland, was compared with profiles from the GROMOS MWR in Bern, Switzerland, satellite instruments (MLS, MIPAS, HALOE, SCHIAMACHY, GOMOS), and profiles simulated by the SOCOL v3.0 CCM. The long-term stability and mean biases of the time series were estimated as a function of the measurement time (day- and nighttime). The homogenized Payerne MWR ozone dataset agrees within ±5 % with the MLS dataset over the 30 to 65 km altitude range and within ±10 % of the HARMonized dataset of OZone profiles (HARMOZ, limb and occultation measurements from ENVISAT) over the 30 to 65 km altitude range. In the upper stratosphere, there is a large nighttime difference between Payerne MWR and other datasets, which is likely a result of the mesospheric signal aliasing with lower levels in the stratosphere due to a lower vertical resolution at that altitude. Hence, the induced bias at 55 km is considered an instrumental artifact and is not further analyzed. [ABSTRACT FROM AUTHOR]

Biogenic very short-lived bromocarbons (VSL Br) currently represent ∼25 % of the total stratospheric bromine loading. Owing to their much shorter lifetime compared to anthropogenic long-lived bromine (e.g. halons) and chlorine (e.g. chlorofluorocarbons), the impact of VSL Br on ozone peaks in the lowermost stratosphere, which is a key climatic and radiative atmospheric region. Here we present a modelling study of the evolution of stratospheric ozone and its chemical loss within the tropics and at mid-latitudes during the 21st century. Two different experiments are explored: considering and neglecting the additional stratospheric injection of 5 ppt biogenic bromine naturally released from the ocean. Our analysis shows that the inclusion of VSL Br results in a realistic stratospheric bromine loading and improves the agreement between the model and satellite observations of the total ozone column (TOC) for the 1980–2015 period at mid-latitudes. We show that the overall ozone response to VSL Br at mid-latitudes follows the stratospheric evolution of long-lived inorganic chlorine and bromine throughout the 21st century. Additional ozone loss due to VSL Br is maximized during the present-day period (1990–2010), with TOC differences of -8 DU (-3 %) and -5.5 DU (-2 %) for the Southern Hemisphere and Northern Hemisphere mid-latitudes (SH-MLs and NH-MLs), respectively. Moreover, the projected TOC differences at the end of the 21st century are ∼50 % lower than the values found for the present-day period. We find that seasonal VSL Br impact on lowermost stratospheric ozone at mid-latitude is influenced by the seasonality of the heterogeneous inorganic-chlorine reactivation processes on ice crystals. Indeed, due to the more efficient reactivation of chlorine reservoirs (mainly ClONO2 and HCl) within the colder SH-ML lowermost stratosphere, the seasonal VSL Br impact shows a small but persistent hemispheric asymmetry through the whole modelled period. Our results indicate that, although the overall VSL Br -driven ozone destruction is greatest during spring, the halogen-mediated (Halog x-Loss) ozone loss cycle in the mid-latitude lowermost stratosphere during winter is comparatively more efficient than the HOx cycle with respect to other seasons. Indeed, when VSL Br are considered, Halog x-Loss dominates wintertime lowermost stratospheric ozone loss at SH-MLs between 1985 and 2020, with a contribution of inter-halogen ClOx – BrOx cycles to Halog x-Loss of ∼50 %. Within the tropics, a small (<-2.5 DU) and relatively constant (∼-1 %) ozone depletion mediated by VSL Br is closely related to their fixed emissions throughout the modelled period. By including the VSL Br sources, the seasonal Halog x-Loss contribution to lowermost stratospheric ozone loss is practically dominated by the BrOx cycle, reflecting the low sensitivity of very short-lived (VSL) bromine to background halogen abundances to drive tropical stratospheric ozone depletion. We conclude that the link between biogenic bromine sources and seasonal changes in heterogeneous chlorine reactivation is a key feature for future projections of mid-latitude lowermost stratospheric ozone during the 21st century. [ABSTRACT FROM AUTHOR]

In this paper, we present long-term observations of atmospheric nitrogen dioxide (NO2) and formaldehyde (HCHO) in Nanjing using a Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument. Ground-based MAX-DOAS measurements were performed from April 2013 to February 2017. The MAX-DOAS measurements of NO2 and HCHO vertical column densities (VCDs) are used to validate ozone monitoring instrument (OMI) satellite observations over Nanjing. The comparison shows that the OMI observations of NO2 correlate well with the MAX-DOAS data with Pearson correlation coefficient (R) of 0.91. However, OMI observations are on average a factor of 3 lower than the MAX-DOAS measurements. Replacing the a priori NO2 profiles by the MAX-DOAS profiles in the OMI NO2 VCD retrieval would increase the OMI NO2 VCDs by ∼30 % with correlation nearly unchanged. The comparison result of MAX-DOAS and OMI observations of HCHO VCD shows a good agreement with R of 0.75 and the slope of the regression line is 0.99. An age-weighted backward-propagation approach is applied to the MAX-DOAS measurements of NO2 and HCHO to reconstruct the spatial distribution of NO2 and HCHO over the Yangtze River Delta during summer and winter time. The reconstructed NO2 fields show a distinct agreement with OMI satellite observations. However, due to the short atmospheric lifetime of HCHO, the backward-propagated HCHO data do not show a strong spatial correlation with the OMI HCHO observations. The result shows that the MAX-DOAS measurements are sensitive to the air pollution transportation in the Yangtze River Delta, indicating the air quality in Nanjing is significantly influenced by regional transportation of air pollutants. The MAX-DOAS data are also used to evaluate the effectiveness of air pollution control measures implemented during the Youth Olympic Games 2014. The MAX-DOAS data show a significant reduction of ambient aerosol, NO2 and HCHO (30 %–50 %) during the Youth Olympic Games. Our results provide a better understanding of the transportation and sources of pollutants over the Yangtze River Delta as well as the effect of emission control measures during large international events, which are important for the future design of air pollution control policies. [ABSTRACT FROM AUTHOR]

This overview paper highlights the successes of the Ozone Monitoring Instrument (OMI) on board the Aura satellite spanning a period of nearly 14 years. Data from OMI has been used in a wide range of applications and research resulting in many new findings. Due to its unprecedented spatial resolution, in combination with daily global coverage, OMI plays a unique role in measuring trace gases important for the ozone layer, air quality, and climate change. With the operational very fast delivery (VFD; direct readout) and near real-time (NRT) availability of the data, OMI also plays an important role in the development of operational services in the atmospheric chemistry domain. [ABSTRACT FROM AUTHOR]

Multiple-regression analyses have been performed on 32 years of total ozone column data that was spatially gridded with a 1 × 1.5° resolution. The total ozone data consist of the MSR (Multi Sensor Reanalysis; 1979-2008) and 2 years of assimilated SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY) ozone data (2009-2010). The two-dimensionality in this data set allows us to perform the regressions locally and investigate spatial patterns of regression coefficients and their explanatory power. Seasonal dependencies of ozone on regressors are included in the analysis. A new physically oriented model is developed to parameterize stratospheric ozone. Ozone variations on nonseasonal timescales are parameterized by explanatory variables describing the solar cycle, stratospheric aerosols, the quasibiennial oscillation (QBO), El Niño-Southern Oscillation (ENSO) and stratospheric alternative halogens which are parameterized by the effective equivalent stratospheric chlorine (EESC). For several explanatory variables, seasonally adjusted versions of these explanatory variables are constructed to account for the difference in their effect on ozone throughout the year. To account for seasonal variation in ozone, explanatory variables describing the polar vortex, geopotential height, potential vorticity and average day length are included. Results of this regression model are compared to that of a similar analysis based on a more commonly applied statistically oriented model. The physically oriented model provides spatial patterns in the regression results for each explanatory variable. The EESC has a significant depleting effect on ozone at midand high latitudes, the solar cycle affects ozone positively mostly in the Southern Hemisphere, stratospheric aerosols affect ozone negatively at high northern latitudes, the effect of QBO is positive and negative in the tropics and mid- to high latitudes, respectively, and ENSO affects ozone negatively between 30° N and 30° S, particularly over the Pacific. The contribution of explanatory variables describing seasonal ozone variation is generally large at mid- to high latitudes. We observe ozone increases with potential vorticity and day length and ozone decreases with geopotential height and variable ozone effects due to the polar vortex in regions to the north and south of the polar vortices. Recovery of ozone is identified globally. However, recovery rates and uncertainties strongly depend on choices that can be made in defining the explanatory variables. The application of several trend models, each with their own pros and cons, yields a large range of recovery rate estimates. Overall these results suggest that care has to be taken in determining ozone recovery rates, in particular for the Antarctic ozone hole. [ABSTRACT FROM AUTHOR]

Most of the short-lived biogenic and anthropogenic chemical species that are emitted into the atmosphere break down efficiently by reaction with OH and do not reach the stratosphere. Here we show the existence of a pronounced minimum in the tropospheric column of ozone over the West Pacific, the main source region for stratospheric air, and suggest a corresponding minimum of the tropospheric column of OH. This has the potential to amplify the impact of surface emissions on the stratospheric composition compared to the impact when assuming globally uniform OH conditions. Specifically, the role of emissions of biogenic halogenated species for the stratospheric halogen budget and the role of increasing emissions of SO2 in Southeast Asia or from minor volcanic eruptions for the increasing stratospheric aerosol loading need to be reassessed in light of these findings. This is also important since climate change will further modify OH abundances and emissions of halogenated species. Our study is based on ozone sonde measurements carried out during the TransBrom cruise with the RV Sonne roughly along 140-150°E in October 2009 and corroborating ozone and OH measurements from satellites, aircraft campaigns and FTIR instruments. Model calculations with the GEOS-Chem Chemistry and Transport Model (CTM) and the ATLAS CTM are used to simulate the tropospheric OH distribution over the West Pacific and the transport pathways to the stratosphere. The potential effect of the OH minimum on species transported into the stratosphere is shown via modeling the transport and chemistry of CH2Br2 and SO2. [ABSTRACT FROM AUTHOR]

A long-term ozone loss time series is necessary to understand the evolution of ozone in Antarctica. Therefore, we construct the time series using ground-based, satellite and bias-corrected multi-sensor reanalysis (MSR) data sets for the period 1989-2010. The trends in ozone over 1979-2010 are also estimated to further elucidate its evolution in the wake of decreasing halogen levels in the stratosphere. Our analysis with ground-based observations shows that the average ozone loss in the Antarctic is about -33 to -50% (-90 to -155DU (Dobson Unit)) in 1989-1992, and then stayed at around -48% (-160 DU). The ozone loss in the warmer winters (e.g. 2002 and 2004) is lower (-37 to -46 %), and in the very cold winters (e.g. 2003 and 2006) it is higher (-52 to -55 %). These loss estimates are in good agreement with those estimated from satellite observations, where the differences are less than ±3 %. The ozone trends based on the equivalent effective Antarctic stratospheric chlorine (EEASC) and piecewise linear trend (PWLT) functions for the vortex averaged ground-based, Total Ozone Mapping Spectrometer/Ozone Monitoring Instrument (TOMS/OMI), and MSR data averaged over September-November exhibit about -4.6 DU yr-1 over 1979-1999, corroborating the role of halogens in the ozone decrease during the period. The ozone trends computed for the 2000-2010 period are about +1 DU yr-1 for EEASC and +2.6 DU yr-1 for the PWLT functions. The larger positive PWLT trends for the 2000- 2010 period indicate the influence of dynamics and other basis functions on the increase of ozone. The trends in both periods are significant at 95% confidence intervals for all analyses. Therefore, our study suggests that Antarctic ozone shows a significant positive trend toward its recovery, and hence, leaves a clear signature of the successful implementation of the Montreal Protocol. [ABSTRACT FROM AUTHOR]

We present the first Multi-Axis-(MAX-) DOAS observations in India performed during April 2010 and January 2011 in Delhi and nearby regions. The MAX-DOAS instrument was mounted on a car roof, which allowed us to perform measurements along individual driving routes. From car MAX-DOAS observations along closed circles around Delhi, together with information on wind speed and direction, the NOx emissions from the greater Delhi area were determined: our estimate of 4.4 x 1025 molecules s-1 is found to be slightly lower than the corresponding emission estimates using the EDGAR emission inventory and substantially smaller compared to a recent study by Gurjar et al. (2004). We also determined NOx emissions from Delhi using OMI satellite observations on the same days. These emissions are slightly smaller than those from the car MAXDOAS measurements. Finally the car MAX-DOAS observations were also used for the validation of simultaneous OMI satellite measurements of the tropospheric NO2 VCD and found a good agreement of the spatial patterns. Concerning the absolute values, OMI data are, on average, higher than the car MAX-DOAS observations close to strong emission sources, and vice versa over less polluted regions. Our results indicate that OMI NO2 VCDs are biased low over strongly polluted regions, probably caused by inadequate apriori profiles used in the OMI satellite retrieval. [ABSTRACT FROM AUTHOR]

The passive tracer method is used to estimate ozone loss from ground-based measurements in the Antarctic. A sensitivity study shows that the ozone depletion can be estimated within an accuracy of ~4%. The method is then applied to the ground-based observations from Arrival Heights, Belgrano, Concordia, Dumont d'Urville, Faraday, Halley, Marambio, Neumayer, Rothera, South Pole, Syowa, and Zhongshan for the diagnosis of ozone loss in the Antarctic. On average, the ten-day boxcar average of the vortex mean ozone column loss deduced from the groundbased stations was about 55±5% in 2005-2009. The ozone loss computed from the ground-based measurements is in very good agreement with those derived from satellite measurements (OMI and SCIAMACHY) and model simulations (REPROBUS and SLIMCAT), where the differences are within ±3-5%. The historical ground-based total ozone observations in October show that the depletion started in the late 1970s, reached a maximum in the early 1990s and stabilised afterwards due to saturation. There is no indication of ozone recovery yet. At southern mid-latitudes, a reduction of 20- 50% is observed for a few days in October-November at the newly installed Rio Gallegos station. Similar depletion of ozone is also observed episodically during the vortex overpasses at Kerguelen in October-November and at Macquarie Island in July-August of the recent winters. This illustrates the significance of measurements at the edges of Antarctica. [ABSTRACT FROM AUTHOR]

Ozone Depletion Events (ODE) during polar springtime are a well known phenomenon in the Arctic and Antarctic boundary layer. They are caused by the catalytic destruction of ozone by halogens producing reactive halogen oxides like bromine monoxide (BrO). The key halogen bromine can be rapidly transferred into the gas phase in an autocatalytic process - the so called "Bromine Explosion". However, the exact mechanism, which leads to an initial bromine release as well as the influence of transport and chemical processes on BrO, is still not clearly understood. In this study, BrO measurements from the satellite instrument GOME-2 are used together with model calculations with the dispersion model FLEXPART to study an arctic BrO event in March 2007, which could be tracked over several days and a large area. Full BrO activation was observed within one day east of Siberia with subsequent transport to Hudson Bay. The event was linked to a cyclone with very high surface wind speeds, which could have been involved in the production and lifting of aerosols or blowing snow. Considering the short life time of BrO, transported aerosols or snow can also provide the surface for BrO recycling within the plume for several days. The evolution of the BrO plume could be reproduced by FLEXPART simulations of a passive tracer indicating that the activated air mass was transported all the way from Siberia to Hudson Bay. To localise the most probable transport height, model runs initialised in different heights have been performed showing similar transport patterns throughout the troposphere but best agreement with the measurements between the surface and 3 km. The influence of changes in tropopause height on measured BrO values has been considered, but cannot completely explain the observed high BrO values. Backward trajectories from the area of BrO initialisation show upward lifting from the surface up to 3 km and no indication for intrusion of stratospheric air. These observations are consistent with a scenario in which bromine in the air mass was activated on the surface within the cyclone, lifted upwards and transported over several thousand kilometres to Hudson Bay. [ABSTRACT FROM AUTHOR]

We have used an off-line three-dimensional (3-D) chemical transport model (CTM) to study long-term changes in stratospheric O3. The model was run from 1977-2004 and forced by ECMWF ERA 40 and operational analyses. Model runs were performed to examine the impact of increasing halogens and additional stratospheric bromine from short-lived source gases. The analyses capture much of the observed interannual variability in column ozone, but them are also unrealistic features. In particular the ERA-40 analyses cause a large positive anomaly in northern hemisphere (NH) column 03 in the late 1980s. Also, the change from ERA-40 to operational winds at the start of 2002 introduces abrupt changes in some model fields (e.g. temperature, ozone) which affect analysis of trends. The model reproduces the observed column increase in NH mid-latitudes from the mid 1990s. Analysis of a run with fixed halogens shows that this increase is not due to a significant decrease in halogen-induced loss, i.e. is not an indication of recovery. The model predicts only a small decrease in halogen-induced loss after 1999. In the upper stratosphere, despite the modelled turnover of chlorine around 1999, O3 does not increase because of the effects of increasing ECMWF temperatures, decreasing modelled CH4 at this altitude, and abrupt changes in the SH temperatures at the end of the ERA-40 period. The impact of an additional 5 pptv stratospheric bromine from short-lived species decreases mid-latitude column O3 by about 10DU. However, the impact on the modelled relative O3 anomaly is generally small except during periods of large volcanic loading. [ABSTRACT FROM AUTHOR]

Trends in ozone columns and vertical distributions were calculated for the period 1979-2004 based on the ozone data set CATO (Candidoz Assimilated Three-dimensional Ozone) using a multiple linear regression model. CATO has been reconstructed from TOMS, GOME and SBUV total column ozone observations in an equivalent latitude and potential temperature framework and offers a pole to pole coverage of the stratosphere on 15 potential temperature levels. The regression model includes explanatory variables describing the influence of the quasi-biennial oscillation (QBO), volcanic eruptions, the solar cycle, the Brewer-Dobson circulation, Arctic ozone depletion, and the increase in stratospheric chlorine. The effects of displacements of the polar vortex and jet streams due to planetary waves, which may significantly affect trends at a given geographical latitude, are eliminated in the equivalent latitude framework. The QBO shows a strong signal throughout most of the lower stratosphere with peak amplitudes in the tropics of the order of 10-20% (peak to valley). The eruption of Pinatubo led to annual mean ozone reductions of 15-25% between the tropopause and 23 km in northern mid-latitudes and to similar percentage changes in the southern hemisphere but concentrated at altitudes below 17 km. Stratospheric ozone is elevated over a broad latitude range by up to 5% during solar maximum compared to solar minimum, the largest increase being observed around 30 km. This is at a lower altitude than reported previously, and no negative signal is found in the tropical lower stratosphere. The Brewer-Dobson circulation shows a dominant contribution to interannual variability at both high and low latitudes and accounts for some of the ozone increase seen in the northern hemisphere since the mid-1990s. Arctic ozone depletion significantly affects the high northern latitudes between January and March and extends its influence to the mid-latitudes during later months. The vertical distribution of the ozone trend shows distinct negative trends at about 18 km in the lower stratosphere with largest declines over the poles, and above 35 km in the upper stratosphere. A narrow band of large negative trends extends into the tropical lower stratosphere. Assuming that the observed negative trend before 1995 continued to 2004 cannot explain the ozone changes since 1996. A model accounting for recent changes in equivalent effective stratospheric chlorine, aerosols and Eliassen-Palm flux, on the other hand, closely tracks ozone changes since 1995. [ABSTRACT FROM AUTHOR]

The Dead Sea is an excellent natural laboratory for the investigation of Reactive Bromine Species (RBS) chemistry, due to the high RBS levels observed in this area, combined with anthropogenic air pollutants up to several ppb. The present study investigated the basic chemical mechanism of RBS at the Dead Sea using a numerical one-dimensional chemical model. Simulations were based on data obtained from comprehensive measurements performed at sites along the Dead Sea. The simulations showed that the high BrO levels measured frequently at the Dead Sea could only partially be attributed to the highly concentrated Br- present in the Dead Sea water. Furthermore, the RBS activity at the Dead Sea cannot solely be explained by a pure gas phase mechanism. This paper presents a chemical mechanism which can account for the observed chemical activity at the Dead Sea, with the addition of only two heterogeneous processes: the "Bromine Explosion" mechanism and the heterogeneous decomposition of BrONO2. Ozone frequently dropped below a threshold value of ∼1 to 2 ppbv at the Dead Sea evaporation ponds, and in such cases, O3 became a limiting factor for the production of BrOx (BrO+Br). The entrainment of O3 fluxes into the evaporation ponds was found to be essential for the continuation of RBS activity, and to be the main reason for the jagged diurnal pattern of BrO observed in the Dead Sea area, and for the positive correlation observed between BrO and O3 at low O3 concentrations. The present study has shown that the heterogeneous decomposition of BrONO2 has a great potential to affect the RBS activity in areas influenced by anthropogenic emissions, mainly due to the positive correlation between the rate of this process and the levels of NO2. Further investigation of the influence of the decomposition of BrONO2 may be especially important in understanding the RBS activity at mid-latitudes. [ABSTRACT FROM AUTHOR]

Trends in ozone columns and vertical distributions were calculated for the period 1979-2004 based on the ozone data set CATO (Candidoz Assimilated Three-dimensional Ozone) using a multiple linear regression model. CATO has been reconstructed from TOMS, GOME and SBUV total column ozone observations in an equivalent latitude and potential temperature framework and offers a pole to pole coverage of the stratosphere on 15 potential temperature levels. The regression model includes explanatory variables describing the influence of the quasi-biennial oscillation (QBO), volcanic eruptions, the solar cycle, the Brewer-Dobson circulation, Arctic ozone depletion, and the increase in stratospheric chlorine. The effects of displacements of the polar vortex and jet streams due to planetary waves, which may significantly affect trends at a given geographical latitude, are eliminated in the equivalent latitude framework. The QBO shows a strong signal throughout most of the lower stratosphere with peak amplitudes in the tropics of the order of 10-20% (peak to valley). The eruption of Pinatubo led to annual mean ozone reductions of 15-25% between the tropopause and 23 km in northern mid-latitudes and to similar percentage changes in the southern hemisphere but concentrated at altitudes below 17 km. Stratospheric ozone is elevated over a broad latitude range by up to 5% during solar maximum compared to solar minimum, the largest increase being observed around 30 km. This is at a lower altitude than reported previously, and no negative signal is found in the tropical lower stratosphere. The Brewer-Dobson circulation shows a dominant contribution to interannual variability at both high and low latitudes and accounts for some of the ozone increase seen in the northern hemisphere since the mid-1990s. Arctic ozone depletion significantly affects the high northern latitudes between January and March and extends its influence to the mid-latitudes during later months. The vertical distribution of the ozone trend shows distinct negative trends at about 18 km in the lower stratosphere with largest declines over the poles, and above 35 km in the upper stratosphere. A narrow band of large negative trends extends into the tropical lower stratosphere. Assuming that the observed negative trend before 1995 continued to 2004 cannot explain the ozone changes since 1996. A model accounting for recent changes in equivalent effective stratospheric chlorine, aerosols and Eliassen-Palm flux, on the other hand, closely tracks ozone changes since 1995. [ABSTRACT FROM AUTHOR]

The Royal Society expedition to Antarctica established a base at Halley Bay, in support of the International Geophysical Year of 1957-1958. Surface ozone was measured during 1958 only, using a prototype Brewer-Mast sonde. The envelope of maximum ozone was an annual cycle from 10 ppbv in January to 22 ppbv in August. These values are 35% less at the start of the year and 15% less at the end than modern values from Neumayer, also a coastal site. This may reflect a general increase in surface ozone since 1958 and differences in summer at the less windy site of Halley, or it may reflect ozone loss on the inlet together with long-term conditioning. There were short periods in September when ozone values decreased rapidly to near-zero, and some in August when ozone values were rapidly halved. Such ozone-loss episodes, catalysed by bromine compounds, became well-known in the Artic in the 1980s, and were observed more recently in the Antarctic. In 1958, very small ozone values were recorded for a week in midwinter during clear weather with light winds. The absence of similar midwinter reductions at Neumayer, or at Halley in the few measurements during 1987, means we must remain suspicious of these small values, but we can find no obvious reason to discount them. The dark reaction of ozone and seawater ice observed in the laboratory may be fast enough to explain them if the salinity and surface area of the ice is sufficiently amplified by frost flowers. [ABSTRACT FROM AUTHOR]

Global total ozone measurements from various satellite instruments such as SBUV, TOMS, and GOME show an increase in zonal mean total ozone at northern hemispheric (NH) mid to high latitudes since the mid-nineties. This increase could be expected from the peaking and start of decline in the effective stratospheric halogen loading, but the rather rapid increase observed in NH zonal mean total ozone suggests that another physical mechanism such as winter planetary wave activity has increased which has led to higher stratospheric Arctic temperatures. This has enhanced ozone transport into higher latitudes in recent years as part of the residual circulation and at the same time reduced the frequency of cold Arctic winters with enhanced polar ozone loss. Results from various multi-variate linear regression analyses using SBUV V8 total ozone with explanatory variables such as a linear trend or, alternatively, EESC (equivalent effective stratospheric chlorine) and on the other hand planetary wave driving (eddy heat flux) or, alternatively, polar ozone loss (PSC volume) in addition to proxies for stratospheric aerosol loading, QBO, and solar cycle, all considered to be main drivers for ozone variability, are presented. It is shown that the main contribution to the recent increase in NH total ozone is from the combined effect of rising tropospheric driven planetary wave activity associated with reduced polar ozone loss at high latitudes as well as increasing solar activity. This conclusion can be drawn regardless of the use of linear trend or EESC terms in our statistical model. It is also clear that more years of data will be needed to further improve our estimates of the relative contributions of the individual processes to decadal ozone variability. The question remains if the observed increase in planetary wave driving is part of natural decadal atmospheric variability or will persist. If the latter is the case, it could be interpreted as a possible signature of climate change. [ABSTRACT FROM AUTHOR]

The erythemally weighted (UV) irradiance below the severely depleted Arctic vortices in spring 1996 and 1997 were substantially elevated. On average the UV increased 36 and 33% relative to the 1979-1981 mean assuming clear skies from day 80-100 in 1996 and 1997, respectively. On clear sky days large regions of the Arctic experienced maximum UV increases exceeding 70 and 50% on single days in 1996 and 1997, respectively. A minor fraction of these increases are not anthropogenic and have a dynamical origin as seen by comparison to 1982, when hardly any ozone depletion is expected. [ABSTRACT FROM AUTHOR]

An assimilated data base of total column ozone measurements from satellites has been used to generate a set of indicators describing attributes of the Antarctic ozone hole for the period 1979 to 2003, including (i) daily measures of the area over Antarctica where ozone levels are below 150 DU, below 220 DU, more than 30% below 1979 to 1981 norms, and more than 50% below 1979 to 1981 norms, (ii) the date of disappearance of 150 DU ozone values, 220 DU ozone values, values 30% below 1979 to 1981 norms, and values 50% below 1979 to 1981 norms, for each year, (iii) daily minimum total column ozone values over Antarctica, and (iv) daily values of the ozone mass deficit based on a O3 <220 DU threshold. The assimilated data base combines satellite-based ozone measurements from 4 Total Ozone Mapping Spectrometer (TOMS) instruments, 3 different retrievals from the Global Ozone Monitoring Experiment (GOME), and data from 4 Solar Backscatter UltraViolet (SBUV) instruments. Comparisons with the global ground-based Dobson spectrophotometer network are used to remove offsets and drifts between the different data sets to produce a global homogeneous data set that combines the advantages of good spatial coverage of satellite data with good long-term stability of ground-based measurements. One potential use of the derived indices is detection of the expected recovery of the Antarctic ozone hole. The suitability of the derived indicators to this task is discussed in the context of their variability and their susceptibility to saturation effects which makes them less responsive to decreasing stratospheric halogen loading. It is also shown that if the corrections required to match recent Earth Probe TOMS measurements to Dobson measurements are not applied, some of the indictors are affected so as to obscure detection of the recovery of the Antarctic ozone hole. [ABSTRACT FROM AUTHOR]

A new algorithm approach called Weighting Function Differential Optical Absorption Spectroscopy (WFDOAS) is presented which has been developed to retrieve total ozone columns from nadir observations of the Global Ozone Monitoring Experiment. By fitting the vertically integrated ozone weighting function rather than ozone cross-section to the sun-normalized radiances, a direct retrieval of vertical column amounts is possible. The new WFDOAS approach takes into account the slant path wavelength modulation that is usually neglected in the standard DOAS approach using single airmass factors. This paper focuses on the algorithm description and error analysis, while in a companion paper by Weber et al. (2004) a detailed validation with groundbased measurements is presented. For the first time several auxiliary quantities directly derived from the GOME spectral range such as cloud-top-height and cloud fraction (O2-A band) and effective albedo using the Lambertian Equivalent Reflectivity (LER) near 377 nm are used in combination as input to the ozone retrieval. In addition the varying ozone dependent contribution to the Raman correction in scattered light known as Ring effect has been included. The molecular ozone filling-in that is accounted for in the new algorithm has the largest contribution to the improved total ozone results from WFDOAS compared to the operational product. The precision of the total ozone retrieval is estimated to be better than 3% for solar zenith angles below 80°. [ABSTRACT FROM AUTHOR]

The SLIMCAT three-dimensional chemical transport model (CTM) is used to infer chemical ozone loss from Polar Ozone and Aerosol Measurement (POAM) III observations of stratospheric ozone during the Arctic winter of 2002-2003. Inferring chemical ozone loss from satellite data requires quantifying ozone variations due to dynamical processes. To accomplish this, the SLIMCAT model was run in a "passive" mode from early December until the middle of March. In these runs, ozone is treated as an inert, dynamical tracer. Chemical ozone loss is inferred by subtracting the model passive ozone, evaluated at the time and location of the POAM observations, from the POAM measurements themselves. This "CTM Passive Subtraction" technique relies on accurate initialization of the CTM and a realistic description of vertical/horizontal transport, both of which are explored in this work. The analysis suggests that chemical ozone loss during the 2002-2003 winter began in late December. This loss followed a prolonged period in which many polar stratospheric clouds were detected, and during which vortex air had been transported to sunlit latitudes. A series of stratospheric warming events starting in January hindered chemical ozone loss later in the winter of 2003. Nevertheless, by 15 March, the final date of the analysis, ozone loss maximized at 425K at a value of about 1.2 ppmv, a moderate amount of loss compared to loss during the unusually cold winters in the late-1990s. SLIMCAT was also run with a detailed stratospheric chemistry scheme to obtain the modelpredicted loss. The SLIMCAT model simulation also shows a maximum ozone loss of 1.2 ppmv at 425 K, and the morphology of the loss calculated by SLIMCAT was similar to that inferred from the POAM data. These results from the recently updated version of SLIMCAT therefore give a much better quantitative description of polar chemical ozone loss than older versions of the same model. Both the inferred and modeled loss calculations show the early destruction in late December and the region of maximum loss descending in altitude through the remainder of the winter and early spring [ABSTRACT FROM AUTHOR]