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    Evaluating stratospheric ozone and water vapour changes in CMIP6 models from 1850 to 2100
    (Katlenburg-Lindau : European Geosciences Union, 2021) Keeble, James; Hassler, Birgit; Banerjee, Antara; Checa-Garcia, Ramiro; Chiodo, Gabriel; Davis, Sean; Eyring, Veronika; Griffiths, Paul T.; Morgenstern, Olaf; Nowack, Peer; Zeng, Guang; Zhang, Jiankai; Bodeker, Greg; Burrows, Susannah; Cameron-Smith, Philip; Cugnet, David; Danek, Christopher; Deushi, Makoto; Horowitz, Larry W.; Kubin, Anne; Li, Lijuan; Lohmann, Gerrit; Michou, Martine; Mills, Michael J.; Nabat, Pierre; Olivié, Dirk; Park, Sungsu; Seland, Øyvind; Stoll, Jens; Wieners, Karl-Hermann; Wu, Tongwen
    Stratospheric ozone and water vapour are key components of the Earth system, and past and future changes to both have important impacts on global and regional climate. Here, we evaluate long-term changes in these species from the pre-industrial period (1850) to the end of the 21st century in Coupled Model Intercomparison Project phase 6 (CMIP6) models under a range of future emissions scenarios. There is good agreement between the CMIP multi-model mean and observations for total column ozone (TCO), although there is substantial variation between the individual CMIP6 models. For the CMIP6 multi-model mean, global mean TCO has increased from ∼300 DU in 1850 to ∼ 305 DU in 1960, before rapidly declining in the 1970s and 1980s following the use and emission of halogenated ozone-depleting substances (ODSs). TCO is projected to return to 1960s values by the middle of the 21st century under the SSP2-4.5, SSP3-7.0, SSP4-3.4, SSP4-6.0, and SSP5-8.5 scenarios, and under the SSP3-7.0 and SSP5-8.5 scenarios TCO values are projected to be ∼ 10 DU higher than the 1960s values by 2100. However, under the SSP1-1.9 and SSP1-1.6 scenarios, TCO is not projected to return to the 1960s values despite reductions in halogenated ODSs due to decreases in tropospheric ozone mixing ratios. This global pattern is similar to regional patterns, except in the tropics where TCO under most scenarios is not projected to return to 1960s values, either through reductions in tropospheric ozone under SSP1-1.9 and SSP1-2.6, or through reductions in lower stratospheric ozone resulting from an acceleration of the Brewer-Dobson circulation under other Shared Socioeconomic Pathways (SSPs). In contrast to TCO, there is poorer agreement between the CMIP6 multi-model mean and observed lower stratospheric water vapour mixing ratios, with the CMIP6 multi-model mean underestimating observed water vapour mixing ratios by ∼ 0.5 ppmv at 70 hPa. CMIP6 multi-model mean stratospheric water vapour mixing ratios in the tropical lower stratosphere have increased by ∼ 0.5 ppmv from the pre-industrial to the present-day period and are projected to increase further by the end of the 21st century. The largest increases (∼ 2 ppmv) are simulated under the future scenarios with the highest assumed forcing pathway (e.g. SSP5-8.5). Tropical lower stratospheric water vapour, and to a lesser extent TCO, shows large variations following explosive volcanic eruptions. © Author(s) 2021.
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    Long-term wintertime trend of zonally asymmetric ozone in boreal extratropics during 1979-2016
    (Basel : MDPI AG, 2018) Schneidereit, A.; Peters, D.H.W.
    Strong zonally asymmetric ozone (ZAO) changes are observed in the boreal extratropics for winter. During the TOMS (Total Ozone Mapping Spectrometer) period (1979-1992) the decrease of zonally asymmetric total ozone (ZATO) was twice as large as the observed zonal mean total ozone trend over Europe in January mainly caused by ultra-long wave transport. Recent studies have demonstrated that the ozone evolution reveals three different quasi-bidecadal trend stages: (i) Decline, (ii) leveling, and (ii) healing. This study focuses on the ZAO structure in boreal extratropics and on ozone transport changes by ultra-long waves during winter months. ERA-Interim data together with a linearized transport model are used. During the healing stage ZATO increases significantly over the North Atlantic/European region for January. The ZATO increase (healing stage) and ZATO decrease (decline stage) are caused by different monthly mean ozone transport characteristics of ultra-long planetary waves over the North Atlantic/European region. Furthermore, the vertical advection (ageostrophic transport) of ozone versus its horizontal component dominates in the lower and middle stratosphere during the healing stage. It is hypothesized that these ageostrophic wind changes are mainly caused by a wave train directed northeastwards which seems to be directly linked to the Arctic warming. © 2018 by the authors.
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    Results from the validation campaign of the ozone radiometer GROMOS-C at the NDACC station of Réunion island
    (Katlenburg-Lindau : EGU, 2016) Fernandez, Susana; Rüfenacht, Rolf; Kämpfer, Niklaus; Portafaix, Thierry; Posny, Françoise; Payen, Guillaume
    Ozone performs a key role in the middle atmosphere and its monitoring is thus necessary. At the Institute of Applied Physics of the University of Bern, Switzerland, we built a new ground-based microwave radiometer, GROMOS-C (GRound based Ozone MOnitoring System for Campaigns). It has a compact design and can be operated remotely with very little maintenance requirements, being therefore suitable for remote deployments. It has been conceived to measure the vertical distribution of ozone in the middle atmosphere, by observing pressure-broadened emission spectra at a frequency of 110.836 GHz. In addition, meridional and zonal wind profiles can be retrieved, based on the Doppler shift of the ozone line measured in the four directions of observation (north, east, south and west). In June 2014 the radiometer was installed at the Maïdo observatory, on Réunion island (21.2° S, 55.5° E). High-resolution ozone spectra were recorded continuously over 7 months. Vertical profiles of ozone have been retrieved through an optimal estimation inversion process, using the Atmospheric Radiative Transfer Simulator ARTS2 as the forward model. The validation is performed against ozone profiles from the Microwave Limb Sounder (MLS) on the Aura satellite, the ozone lidar located at the observatory and with ozone profiles from weekly radiosondes. Zonal and meridional winds retrieved from GROMOS-C data are validated against another wind radiometer located in situ, WIRA. In addition, we compare both ozone and winds with ECMWF (European Centre for Medium-Range Weather Forecasts) model data. Results show that GROMOS-C provides reliable ozone profiles between 30 and 0.02 hPa. The comparison with lidar profiles shows a very good agreement at all levels. The accordance with the MLS data set is within 5 % for pressure levels between 25 and 0.2 hPa. GROMOS-C's wind profiles are in good agreement with the observations by WIRA and with the model data, differences are below 5 m s−1 for both.
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    Ozone–gravity wave interaction in the upper stratosphere/lower mesosphere
    (Katlenburg-Lindau : EGU, 2022) Gabriel, Axel
    The increase in amplitudes of upward propagating gravity waves (GWs) with height due to decreasing density is usually described by exponential growth. Recent measurements show some evidence that the upper stratospheric/lower mesospheric gravity wave potential energy density (GWPED) increases more strongly during the daytime than during the nighttime. This paper suggests that ozone-gravity wave interaction can principally produce such a phenomenon. The coupling between ozone-photochemistry and temperature is particularly strong in the upper stratosphere where the time-mean ozone mixing ratio decreases with height. Therefore, an initial ascent (or descent) of an air parcel must lead to an increase (or decrease) in ozone and in the heating rate compared to the environment, and, hence, to an amplification of the initial wave perturbation. Standard solutions of upward propagating GWs with linear ozone-temperature coupling are formulated, suggesting amplitude amplifications at a specific level during daytime of 5ĝ€¯% to 15ĝ€¯% for low-frequency GWs (periods ≥4ĝ€¯h), as a function of the intrinsic frequency which decreases if ozone-temperature coupling is included. Subsequently, the cumulative amplification during the upward level-by-level propagation leads to much stronger GW amplitudes at upper mesospheric altitudes, i.e., for single low-frequency GWs, up to a factor of 1.5 to 3 in the temperature perturbations and 3 to 9 in the GWPED increasing from summer low to polar latitudes. Consequently, the mean GWPED of a representative range of mesoscale GWs (horizontal wavelengths between 200 and 1100ĝ€¯km, vertical wavelengths between 3 and 9ĝ€¯km) is stronger by a factor of 1.7 to 3.4 (2 to 50ĝ€¯Jĝ€¯kg-1, or 2ĝ€¯% to 50ĝ€¯% in relation to the observed order of 100ĝ€¯Jĝ€¯kg-1, assuming initial GW perturbations of 1 to 2ĝ€¯K in the middle stratosphere). Conclusively, the identified process might be an important component in the middle atmospheric circulation, which has not been considered up to now.
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    Hydroxyl layer: trend of number density and intra-annual variability
    (Katlenburg, Lindau : Copernicus, 2015) Sonnemann, G.R.; Hartogh, P.; Berger, U.; Grygalashvyly, M.
    The layer of vibrationally excited hydroxyl (OH*) near the mesopause in Earth's atmosphere is widely used to derive the temperature at this height and to observe dynamical processes such as gravity waves. The concentration of OH* is controlled by the product of atomic hydrogen, with ozone creating a layer of enhanced concentration in the mesopause region. However, the basic influences on the OH* layer are atomic oxygen and temperature. The long-term monitoring of this layer provides information on a changing atmosphere. It is important to know which proportion of a trend results from anthropogenic impacts on the atmosphere and which proportion reflects natural variations. In a previous paper (Grygalashvyly et al., 2014), the trend of the height of the layer and the trend in temperature were investigated particularly in midlatitudes on the basis of our coupled dynamic and chemical transport model LIMA (Leibniz Institute Middle Atmosphere). In this paper we consider the trend for the number density between the years 1961 and 2009 and analyze the reason of the trends on a global scale. Further, we consider intra-annual variations. Temperature and wind have the strongest impacts on the trend. Surprisingly, the increase in greenhouse gases (GHGs) has no clear influence on the chemistry of OH*. The main reason for this lies in the fact that, in the production term of OH*, if atomic hydrogen increases due to increasing humidity of the middle atmosphere by methane oxidation, ozone decreases. The maximum of the OH* layer is found in the mesopause region and is very variable. The mesopause region is a very intricate domain marked by changeable dynamics and strong gradients of all chemically active minor constituents determining the OH* chemistry. The OH* concentration responds, in part, very sensitively to small changes in these parameters. The cause for this behavior is given by nonlinear reactions of the photochemical system being a nonlinear enforced chemical oscillator driven by the diurnal-periodic solar insolation. At the height of the OH* layer the system operates in the vicinity of chemical resonance. The solar cycle is mirrored in the data, but the long-term behavior due to the trend in the Lyman-α radiation is very small. The number density shows distinct hemispheric differences. The calculated OH* values show sometimes a step around a certain year. We introduce a method to find out the date of this step and discuss a possible reason for such behavior.
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    Longitude-dependent decadal ozone changes and ozone trends in boreal winter months during 1960-2000
    (Göttingen : Copernicus, 2008) Peters, D.H.W.; Gabriel, A.; Entzian, G.
    This study examines the longitude-dependent decadal changes and trends of ozone for the boreal winter months during the period of 1960–2000. These changes are caused primarily by changes in the planetary wave structure in the upper troposphere and lower stratosphere. The decadal changes and trends over 4 decades of geopotential perturbations, defined as a deviation from the zonal mean, are estimated by linear regression with time. The decadal changes in longitude-dependent ozone were calculated with a simple transport model of ozone based on the known planetary wave structure changes and prescribed zonal mean ozone gradients. For December of the 1960s and 1980s a statistically significant Rossby wave track appeared over the North Atlantic and Europe with an anticyclonic disturbance over the Eastern North Atlantic and Western Europe, flanked by cyclonic disturbances. In the 1970s and 1990s statistically significant cyclonic disturbances appeared over the Eastern North Atlantic and Europe, surrounded by anticyclonic anomalies over Northern Africa, Central Asia and Greenland. Similar patterns have been found for January. The Rossby wave track over the North Atlantic and Europe is stronger in the 1980s than in the 1960s. For February, the variability of the regression patterns is higher. For January we found a strong alteration in the modelled decadal changes in total ozone over Central and Northern Europe, showing a decrease of about 15 DU in the 1960s and 1980s and an increase of about 10 DU in the 1970s and 1990s. Over Central Europe the positive geopotential height trend (increase of 2.3 m/yr) over 40 years is of the same order (about 100 m) as the increase in the 1980s alone. This is important to recognize because it implies a total ozone decrease over Europe of the order of 14 DU for the 1960–2000 period, for January, if we use the standard change regression relation that about a 10-m geopotential height increase at 300 hPa is related to about a 1.4-DU total ozone decrease.
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    Modelling the wintertime response to upper tropospheric and lower stratospheric ozone anomalies over the North Atlantic and Europe
    (Göttingen : Copernicus GmbH, 2003) Kirchner, I.; Peters, D.
    During boreal winter months, mean longitude-dependent ozone changes in the upper troposphere and lower stratosphere are mainly used by different ozone transport by planetary waves. The response to radiative perturbation induced by these ozone changes near the tropopause on the circulation is unclear. This response is investigated with the ECHAM4 general circulation model in a sensitivity study. In the simulation two different mean January realizations of the ozone field are implemented in ECHAM4. Both ozone fields are estimated on the basis of the observed mean January planetary wave structure of the 1980s. The first field represents a 14-year average (reference, 1979-1992) and the second one represents the mean ozone field change (anomaly, 1988-92) in boreal extra-tropics during the end of the 1980s. The model runs were carried out pairwise, with identical initial conditions for both ozone fields. Five statistically independent experiments were performed, forced with the observed sea surface temperatures for the period 1988 to 1992. The results support the hypothesis that the zonally asymmetric ozone changes of the 80s triggered a systematic alteration of the circulation over the North Atlantic - European region. It is suggested that this feedback process is important for the understanding of the decadal coupling between troposphere and stratosphere, as well as between subtropics and extra-tropics in winter.
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    The Lagrangian structure of ozone mini-holes and potential vorticity anomalies in the Northern Hemisphere
    (Göttingen : Copernicus GmbH, 2002) James, P.M.; Peters, D.
    An ozone mini-hole is a synoptic-scale area of strongly reduced column total ozone, which undergoes a growth-decay cycle in association with baroclinic weather systems. The tracks of mini-hole events recorded during the TOMS observation period over the Northern Hemisphere provide a database for building anomaly fields of various meteorological parameters, following each mini-hole center in a Lagrangian sense. The resulting fields provide, for the first time, a complete mean Lagrangian picture of the three-dimensional structure of typical ozone mini-holes in the Northern Hemisphere. Mini-holes are shown to be associated with anomalous warm anticyclonic flow in the upper troposphere and cold cyclonic anomalies in the middle stratosphere. Ascending air columns occur upstream and descent downstream of the mini-hole centers. Band-pass filtering is used to reveal the transient synoptic nature of mini-holes embedded within larger scale circulation anomalies. Significant correlations between ozone and Ertel's potential vorticity on isentropes (IPV) both near the tropopause and in the middle stratosphere are shown and then utilized by reconstructing the Lagrangian analysis to follow local IPV anomalies instead of ozone minima. By using IPV as a proxy for ozone, the geopotential anomaly dipolar structure in the vertical characteristics of mini-holes is shown to result from a superposition of two largely independent dynamical components, stratospheric and tropospheric, typically operating on different time scales. Hence, ozone mini-holes may be viewed primarily as phenomena of coincidence.
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    Upper stratospheric ozone decrease events due to a positive feedback between ozone and the ozone dissociation rate
    (Göttingen : Copernicus, 2009) Sonnemann, G.R.; Hartogh, P.
    Ozone measurements taken with a ground based microwave instrument at Lindau (51.66° N, 10.13° E) over some years showed strong ozone decrease events within the stratopause region, particularly during the winter half-year. These events are characterized by a marked drop of the ozone mixing ratio from two to three ppmv to less than half a ppmv in extreme cases. Simultaneous water vapor measurements at the same place, also carried out by a microwave instrument, showed a strong increase of its mixing ratio and the temperature was also enhanced during these episodes. The theoretical analysis brought evidence that these events result from a positive feedback in the complex radiatively-chemical system between the ozone column density and the ozone dissociation rate.
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    Short term associations of ambient nitrogen dioxide with daily total, cardiovascular, and respiratory mortality: multilocation analysis in 398 cities
    (London : BMJ Publ. Group, 2021) Meng, Xia; Liu, Cong; Chen, Renjie; Sera, Francesco; Vicedo-Cabrera, Ana Maria; Milojevic, Ai; Guo, Yuming; Tong, Shilu; Coelho, Micheline de Sousa Zanotti Stagliorio; Saldiva, Paulo Hilario Nascimento; Lavigne, Eric; Correa, Patricia Matus; Ortega, Nicolas Valdes; Osorio, Samuel; Garcia, null; Kyselý, Jan; Urban, Aleš; Orru, Hans; Maasikmets, Marek; Jaakkola, Jouni J. K.; Ryti, Niilo; Huber, Veronika; Schneider, Alexandra; Katsouyanni, Klea; Analitis, Antonis; Hashizume, Masahiro; Honda, Yasushi; Ng, Chris Fook Sheng; Nunes, Baltazar; Teixeira, João Paulo; Holobaca, Iulian Horia; Fratianni, Simona; Kim, Ho; Tobias, Aurelio; Íñiguez, Carmen; Forsberg, Bertil; Åström, Christofer; Ragettli, Martina S.; Guo, Yue-Liang Leon; Pan, Shih-Chun; Li, Shanshan; Bell, Michelle L.; Zanobetti, Antonella; Schwartz, Joel; Wu, Tangchun; Gasparrini, Antonio; Kan, Haidong
    Objective To evaluate the short term associations between nitrogen dioxide (NO2) and total, cardiovascular, and respiratory mortality across multiple countries/regions worldwide, using a uniform analytical protocol. Design Two stage, time series approach, with overdispersed generalised linear models and multilevel meta-analysis. Setting 398 cities in 22 low to high income countries/regions. Main outcome measures Daily deaths from total (62.8 million), cardiovascular (19.7 million), and respiratory (5.5 million) causes between 1973 and 2018. Results On average, a 10 μg/m3 increase in NO2 concentration on lag 1 day (previous day) was associated with 0.46% (95% confidence interval 0.36% to 0.57%), 0.37% (0.22% to 0.51%), and 0.47% (0.21% to 0.72%) increases in total, cardiovascular, and respiratory mortality, respectively. These associations remained robust after adjusting for co-pollutants (particulate matter with aerodynamic diameter ≤10 μm or ≤2.5 μm (PM10 and PM2.5, respectively), ozone, sulfur dioxide, and carbon monoxide). The pooled concentration-response curves for all three causes were almost linear without discernible thresholds. The proportion of deaths attributable to NO2 concentration above the counterfactual zero level was 1.23% (95% confidence interval 0.96% to 1.51%) across the 398 cities. Conclusions This multilocation study provides key evidence on the independent and linear associations between short term exposure to NO2 and increased risk of total, cardiovascular, and respiratory mortality, suggesting that health benefits would be achieved by tightening the guidelines and regulatory limits of NO2.