The Impact of Tropospheric Rocket Exhaust on Stratospheric Ozone

1994 ◽  
Author(s):  
Michael J. Prather
1999 ◽  
Author(s):  
Peter D. Lohn ◽  
Eric P. Wong ◽  
Tyrrel W. Smith ◽  
Edwards Jr. ◽  
Pilson John R. ◽  
...  

2017 ◽  
Author(s):  
Amanda C. Maycock ◽  
Katja Matthes ◽  
Susann Tegtmeier ◽  
Hauke Schmidt ◽  
Rémi Thiéblemont ◽  
...  

Abstract. The impact of changes in incoming solar irradiance on stratospheric ozone abundances should be included in climate model simulations to fully capture the atmospheric response to solar variability. This study presents the first systematic comparison of the solar-ozone response (SOR) during the 11 year solar cycle amongst different chemistry-climate models (CCMs) and ozone databases specified in climate models that do not include chemistry. We analyse the SOR in eight CCMs from the WCRP/SPARC Chemistry-Climate Model Initiative (CCMI-1) and compare these with three ozone databases: the Bodeker Scientific database, the SPARC/AC&C database for CMIP5, and the SPARC/CCMI database for CMIP6. The results reveal substantial differences in the representation of the SOR between the CMIP5 and CMIP6 ozone databases. The peak amplitude of theSOR in the upper stratosphere (1–5 hPa) decreases from 5 % to 2 % between the CMIP5 and CMIP6 databases. This difference is because the CMIP5 database was constructed from a regression model fit to satellite observations, whereas the CMIP6 database is constructed from CCM simulations, which use a spectral solar irradiance (SSI) dataset with relatively weak UV forcing. The SOR in the CMIP6 ozone database is therefore implicitly more similar to the SOR in the CCMI-1 models than to the CMIP5 ozone database, which shows a greater resemblance in amplitude and structure to the SOR in the Bodeker database. The latitudinal structure of the annual mean SOR in the CMIP6 ozone database and CCMI-1 models is considerably smoother than in the CMIP5 database, which shows strong gradients in the SOR across the midlatitudes owing to the paucity of observations at high latitudes. The SORs in the CMIP6 ozone database and in the CCMI-1 models show a strong seasonal dependence, including large meridional gradients at mid to high latitudes during winter; such seasonal variations in the SOR are not included in the CMIP5 ozone database. Sensitivity experiments with a global atmospheric model without chemistry (ECHAM6.3) are performed to assess the impact of changes in the representation of the SOR and SSI forcing between CMIP5 and CMIP6. The experiments show that the smaller amplitude of the SOR in the CMIP6 ozone database compared to CMIP5 causes a decrease in the modelled tropical stratospheric temperature response over the solar cycle of up to 0.6 K, or around 50 % of the total amplitude. The changes in the SOR explain most of the difference in the amplitude of the tropical stratospheric temperature response in the case with combined changes in SOR and SSI between CMIP5 and CMIP6. The results emphasise the importance of adequately representing the SOR in climate models to capture the impact of solar variability on the atmosphere. Since a number of limitations in the representation of the SOR in the CMIP5 ozone database have been identified, CMIP6 models without chemistry are encouraged to use the CMIP6 ozone database to capture the climate impacts of solar variability.


2016 ◽  
Vol 16 (18) ◽  
pp. 11521-11534 ◽  
Author(s):  
Luis F. Millán ◽  
Nathaniel J. Livesey ◽  
Michelle L. Santee ◽  
Jessica L. Neu ◽  
Gloria L. Manney ◽  
...  

Abstract. This study investigates the representativeness of two types of orbital sampling applied to stratospheric temperature and trace gas fields. Model fields are sampled using real sampling patterns from the Aura Microwave Limb Sounder (MLS), the HALogen Occultation Experiment (HALOE) and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). The MLS sampling acts as a proxy for a dense uniform sampling pattern typical of limb emission sounders, while HALOE and ACE-FTS represent coarse nonuniform sampling patterns characteristic of solar occultation instruments. First, this study revisits the impact of sampling patterns in terms of the sampling bias, as previous studies have done. Then, it quantifies the impact of different sampling patterns on the estimation of trends and their associated detectability. In general, we find that coarse nonuniform sampling patterns may introduce non-negligible errors in the inferred magnitude of temperature and trace gas trends and necessitate considerably longer records for their definitive detection. Lastly, we explore the impact of these sampling patterns on tropical vertical velocities derived from stratospheric water vapor measurements. We find that coarse nonuniform sampling may lead to a biased depiction of the tropical vertical velocities and, hence, to a biased estimation of the impact of the mechanisms that modulate these velocities. These case studies suggest that dense uniform sampling such as that available from limb emission sounders provides much greater fidelity in detecting signals of stratospheric change (for example, fingerprints of greenhouse gas warming and stratospheric ozone recovery) than coarse nonuniform sampling such as that of solar occultation instruments.


2015 ◽  
Vol 15 (16) ◽  
pp. 9435-9453 ◽  
Author(s):  
G. Shi ◽  
A. M. Buffen ◽  
M. G. Hastings ◽  
C. Li ◽  
H. Ma ◽  
...  

Abstract. Snowpits along a traverse from coastal East Antarctica to the summit of the ice sheet (Dome Argus) are used to investigate the post-depositional processing of nitrate (NO3−) in snow. Seven snowpits from sites with accumulation rates between 24 and 172 kg m−2 a−1 were sampled to depths of 150 to 300 cm. At sites from the continental interior (low accumulation, < 55 kg m−2 a−1), nitrate mass fraction is generally > 200 ng g−1 in surface snow and decreases quickly with depth to < 50 ng g−1. Considerably increasing values of δ15N of nitrate are also observed (16–461 ‰ vs. air N2), particularly in the top 20 cm, which is consistent with predicted fractionation constants for the photolysis of nitrate. The δ18O of nitrate (17–84 ‰ vs. VSMOW (Vienna Standard Mean Ocean Water)), on the other hand, decreases with increasing δ15N, suggestive of secondary formation of nitrate in situ (following photolysis) with a low δ18O source. Previous studies have suggested that δ15N and δ18O of nitrate at deeper snow depths should be predictable based upon an exponential change derived near the surface. At deeper depths sampled in this study, however, the relationship between nitrate mass fraction and δ18O changes, with increasing δ18O of nitrate observed between 100 and 200 cm. Predicting the impact of post-depositional loss, and therefore changes in the isotopes with depth, is highly sensitive to the depth interval over which an exponential change is assumed. In the snowpits collected closer to the coast (accumulation > 91 kg m−2 a−1), there are no obvious trends detected with depth and instead seasonality in nitrate mass fraction and isotopic composition is found. In comparison to the interior sites, the coastal pits are lower in δ15N (−15–71 ‰ vs. air N2) and higher in δ18O of nitrate (53–111 ‰ vs. VSMOW). The relationships found amongst mass fraction, δ15N, δ18O and Δ17O (Δ17O = δ17O–0.52 × δ18O) of nitrate cannot be explained by local post-depositional processes alone, and are instead interpreted in the context of a primary atmospheric signal. Consistent with other Antarctic observational and modeling studies, the isotopic results are suggestive of an important influence of stratospheric ozone chemistry on nitrate formation during the cold season and a mix of tropospheric sources and chemistry during the warm season. Overall, the findings in this study speak to the sensitivity of nitrate isotopic composition to post-depositional processing and highlight the strength of combined use of the nitrogen and oxygen isotopes for a mechanistic understanding of this processing.


2020 ◽  
Author(s):  
Javer A. Barrera ◽  
Rafael P. Fernandez ◽  
Fernando Iglesias-Suarez ◽  
Carlos A. Cuevas ◽  
Jean-Francois Lamarque ◽  
...  

Abstract. Biogenic very short-lived bromine (VSLBr) represents, nowadays, ~ 25 % of the total stratospheric bromine loading. Owing to their much shorter lifetime compared to anthropogenic long-lived bromine (LLBr, e.g., halons) and chlorine (LLCl, e.g., chlorofluorocarbons) substances, the impact of VSLBr on ozone peaks at the extratropical lowermost stratosphere, a key climatic and radiative atmospheric region. Here we present a modelling study of the evolution of stratospheric ozone and its chemical losses in extra-polar regions during the 21st century, under two different scenarios: considering and neglecting the additional stratospheric injection of 5 ppt biogenic VSLBr naturally released from the ocean. Our analysis shows that the inclusion of VSLBr result in a realistic stratospheric bromine loading and improves the quantitative 1980–2015 model-satellite agreement of total ozone column (TOC) in the mid-latitudes. We show that the overall ozone response to VSLBr within the mid-latitudes follows the stratospheric abundances evolution of long-lived inorganic chlorine and bromine throughout the 21st century. Additional ozone losses due to VSLBr are maximised during the present-day period (1990–2010), with TOC differences of −8 DU (−3 %) and −5.5 DU (−2 %) for the southern (SH-ML) and northern (NH-ML) mid-latitudes, respectively. Moreover, the projected TOC differences at the end of the 21st century are at least half of the values found for the present-day period. In the tropics, a small (


2014 ◽  
Vol 14 (19) ◽  
pp. 10431-10438 ◽  
Author(s):  
X. Yang ◽  
N. L. Abraham ◽  
A. T. Archibald ◽  
P. Braesicke ◽  
J. Keeble ◽  
...  

Abstract. Naturally produced very short-lived substances (VSLS) account for almost a quarter of the current stratospheric inorganic bromine, Bry. Following VSLS oxidation, bromine radicals (Br and BrO) can catalytically destroy ozone. The extent to which possible increases in surface emissions or transport of these VSLS bromocarbons to the stratosphere could counteract the effect of halogen reductions under the Montreal Protocol is an important policy question. Here, by using a chemistry–climate model, UM-UKCA, we investigate the impact of a hypothetical doubling (an increase of 5 ppt Bry) of VSLS bromocarbons on ozone and how the resulting ozone changes depend on the background concentrations of chlorine and bromine. Our model experiments indicate that for the 5 ppt increase in Bry from VSLS, the ozone decrease in the lowermost stratosphere of the Southern Hemisphere (SH) may reach up to 10% in the annual mean; the ozone decrease in the Northern Hemisphere (NH) is smaller (4–6%). The largest impact on the ozone column is found in the Antarctic spring. There is a significantly larger ozone decrease following the doubling of the VSLS burden under a high stratospheric chlorine background than under a low chlorine background, indicating the importance of the inter-halogen reactions. For example, the decline in the high-latitude, lower-stratospheric ozone concentration as a function of Bry is higher by about 30–40% when stratospheric Cly is ~ 3 ppb (present day), compared with Cly of ~ 0.8 ppb (a pre-industrial or projected future situation). Bromine will play an important role in the future ozone layer. However, even if bromine levels from natural VSLS were to increase significantly later this century, changes in the concentration of ozone will likely be dominated by the decrease in anthropogenic chlorine. Our calculation suggests that for a 5 ppt increase in Bry from VSLS, the Antarctic ozone hole recovery date could be delayed by approximately 6–8 years, depending on Cly levels.


2021 ◽  
Author(s):  
Ewa Bednarz ◽  
Ryan Hossaini ◽  
Luke Abraham ◽  
Peter Braesicke ◽  
Martyn Chipperfield

&lt;p&gt;The emissions of most long-lived halogenated ozone-depleting substances (ODSs) are now decreasing, owing to controls on their production introduced by Montreal Protocol and its amendments. However, short-lived halogenated compounds can also have substantial impact on atmospheric chemistry, including stratospheric ozone, particularly if emitted near climatological uplift regions. It has recently become evident that emissions of some chlorinated very short-lived species (VSLSs), such as chloroform (CHCl&lt;sub&gt;3&lt;/sub&gt;) and dichloromethane (CH&lt;sub&gt;2&lt;/sub&gt;Cl&lt;sub&gt;2&lt;/sub&gt;), could be larger than previously believed and increasing, particularly in Asia. While these may exert a significant influence on atmospheric chemistry and climate, their impacts remain poorly characterised.&amp;#160;&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;We address this issue using the UM-UKCA chemistry-climate model (CCM). While not only the first, to our knowledge, model study addressing this problem using a CCM, it is also the first such study employing a whole atmosphere model, thereby simulating the tropospheric Cl-VSLSs emissions and the resulting stratospheric impacts in a fully consistent manner. We use a newly developed Double-Extended Stratospheric-Tropospheric (DEST) chemistry scheme, which includes emissions of all major chlorinated and brominated VSLSs alongside an extended treatment of long-lived ODSs.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;We examine the impacts of rising Cl-VSLSs emissions on atmospheric chlorine tracers and ozone, including their long-term trends. We pay particular attention to the role of &amp;#8216;nudging&amp;#8217;, as opposed to the free-running model set up, for the simulated Cl-VSLSs impacts, thereby demostrating the role of atmospheric dynamics in modulating the atmospheric responses to Cl-VSLSs. In addition, we employ novel estimates of Cl-VSLS emissions over the recent past and compare the results with the simulations that prescribe Cl-VSLSs using simple lower boundary conditions. This allows us to demonstrate the impact such choice has on the dominant location and seasonality of the Cl-VSLSs transport into the stratosphere.&lt;/p&gt;


2019 ◽  
Vol 19 (22) ◽  
pp. 14387-14401 ◽  
Author(s):  
Dimitris Akritidis ◽  
Andrea Pozzer ◽  
Prodromos Zanis

Abstract. Using a transient simulation for the period 1960–2100 with the state-of-the-art ECHAM5/MESSy Atmospheric Chemistry (EMAC) global model and a tropopause fold identification algorithm, we explore the future projected changes in tropopause folds, stratosphere-to-troposphere transport (STT) of ozone, and tropospheric ozone under the RCP6.0 scenario. Statistically significant changes in tropopause fold frequencies from 1970–1999 to 2070–2099 are identified in both hemispheres, regionally exceeding 3 %, and are associated with the projected changes in the position and intensity of the subtropical jet streams. A strengthening of ozone STT is projected for the future in both hemispheres, with an induced increase in transported stratospheric ozone tracer throughout the whole troposphere, reaching up to 10 nmol mol−1 in the upper troposphere, 8 nmol mol−1 in the middle troposphere, and 3 nmol mol−1 near the surface. Notably, the regions exhibiting the largest changes of ozone STT at 400 hPa coincide with those with the highest fold frequency changes, highlighting the role of the tropopause folding mechanism in STT processes under a changing climate. For both the eastern Mediterranean and Middle East (EMME) and Afghanistan (AFG) regions, which are known as hotspots of fold activity and ozone STT during the summer period, the year-to-year variability of middle-tropospheric ozone with stratospheric origin is largely explained by the short-term variations in ozone at 150 hPa and tropopause fold frequency. Finally, ozone in the lower troposphere is projected to decrease under the RCP6.0 scenario during MAM (March, April, and May) and JJA (June, July, and August) in the Northern Hemisphere and during DJF (December, January, and February) in the Southern Hemisphere, due to the decline of ozone precursor emissions and the enhanced ozone loss from higher water vapour abundances, while in the rest of the troposphere ozone shows a remarkable increase owing mainly to the STT strengthening and the stratospheric ozone recovery.


Author(s):  
Eric L. Fleming ◽  
Paul A. Newman ◽  
Qing Liang ◽  
John S. Daniel

2020 ◽  
Vol 13 (1) ◽  
pp. 363-383 ◽  
Author(s):  
Mariano Mertens ◽  
Astrid Kerkweg ◽  
Volker Grewe ◽  
Patrick Jöckel ◽  
Robert Sausen

Abstract. Anthropogenic and natural emissions influence the tropospheric ozone budget, thereby affecting air quality and climate. To study the influence of different emission sources on the ozone budget, often source apportionment studies with a tagged tracer approach are performed. Studies investigating air quality issues usually rely on regional models with a fine spatial resolution, while studies focusing on climate-related questions often use coarsely resolved global models. It is well known that simulated ozone mixing ratios depend on the resolution of the model and the resolution of the emission inventory. Whether the contributions simulated using source apportionment approaches also depend on the model resolution, however, is still unclear. Therefore, this study attempts for the first time to analyse the impact of the model, the model resolution, and the emission inventory resolution on simulated ozone contributions using a diagnostic tagging method. The differences in the ozone contributions caused by these factors are compared with differences that arise from the usage of different emission inventories. To do so, we apply the MECO(n) (MESSy-fied ECHAM and COSMO models nested n times) model system which couples online a global chemistry-climate model with a regional chemistry-climate model equipped with a tagging scheme for source apportionment. The results of the global model (at 300 km horizontal resolution) are compared with the results of the regional model at 50 km (Europe) and 12 km (Germany) resolutions. Besides model-specific differences and biases that are discussed in detail, our results have important implications for other modelling studies and modellers applying source apportionment methods. First, contributions from anthropogenic emissions averaged over the continental scale are quite robust with respect to the model, model resolution, and emission inventory resolution. Second, differences on the regional scale caused by different models and model resolutions can be quite large, and regional models are indispensable for source apportionment studies on the subcontinental scale. Third, contributions from stratospheric ozone transported to the surface differ strongly between the models, mainly caused by differences in the efficiency of the vertical mixing. As stratospheric ozone plays an important role for ground level ozone, but the models show large differences in the amount of downward transported ozone, source apportionment methods should account for this source explicitly to better understand inter-model differences.


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