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  • 1
    Electronic Resource
    Electronic Resource
    Springer
    Annales geophysicae 12 (1994), S. 342-354 
    ISSN: 0992-7689
    Source: Springer Online Journal Archives 1860-2000
    Topics: Geosciences , Physics
    Notes: Abstract A three-dimensional transport model has been used to compare and contrast the extent of processing by polar stratospheric clouds during the northern hemisphere winters of 1991/1992 and 1992/1993. The model has also been used to compare the potential for ozone loss between these two winters. The TOMCAT off-line model is forced using meteorological analyses from the ECMWF. During winter 1992/1993 polar stratospheric clouds (PSCs) in the model persisted into late February/early March, which is much later than in 1991/1992. This persistence of PSCs should have resulted in much more ozone loss in the later winter. Interestingly, however, the extent of PSC processing and ozone loss was greater in January 1992 than January 1993. In January 1992 PSCs occurred at the edge of a distorted polar vortex whilst in January 1993 the PSCs were located at the centre of a much more zonally symmetrical vortex. In March 1993, distortions of the vortex led to the tearing off of vortex air and its mixing into midlatitudes.
    Type of Medium: Electronic Resource
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  • 2
    Electronic Resource
    Electronic Resource
    [s.l.] : Macmillan Magazines Ltd.
    Nature 400 (1999), S. 551-554 
    ISSN: 1476-4687
    Source: Nature Archives 1869 - 2009
    Topics: Biology , Chemistry and Pharmacology , Medicine , Natural Sciences in General , Physics
    Notes: [Auszug] The reduction in the amount of ozone in the atmospheric column over the Arctic region, observed during the 1990s,, resembles the onset of the Antarctic ozone ‘hole’ in the mid-1980s, but the two polar regions differ significantly with respect to the relative contributions of ...
    Type of Medium: Electronic Resource
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  • 3
    ISSN: 1573-0662
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract The chemically induced ozone loss inside the Arctic vortex during the winter 1994/95 has been quantified by coordinated launches of over 1000 ozonesondes from 35 stations within the Match 94/95 campaign. Trajectory calculations, which allow diabatic heating or cooling, were used to trigger the balloon launches so that the ozone concentrations in a large number of air parcels are each measured twice a few days apart. The difference in ozone concentration is calculated for each pair and is interpreted as a change caused by chemistry. The data analysis has been carried out for January to March between 370 K and 600 K potential temperature. Ozone loss along these trajectories occurred exclusively during sunlit periods, and the periods of ozone loss coincided with, but slightly lagged, periods where stratospheric temperatures were low enough for polar stratospheric clouds to exist. Two clearly separated periods of ozone loss show up. Ozone loss rates first peaked in late January with a maximum value of 53 ppbv per day (1.6 % per day) at 475 K and faster losses higher up. Then, in mid-March ozone loss rates at 475 K reached 34 ppbv per day (1.3 % per day), faster losses were observed lower down and no ozone loss was found above 480 K during that period. The ozone loss in hypothetical air parcels with average diabetic descent rates has been integrated to give an accumulated loss through the winter. The most severe depletion of 2.0 ppmv (60 %) took place in air that was at 515 K on 1 January and at 450 K on 20 March. Vertical integration over the levels from 370 K to 600 K gives a column loss rate, which reached a maximum value of 2.7 Dobson Units per day in mid-March. The accumulated column loss between 1 January and 31 March was found to be 127 DU (∼36 %).
    Type of Medium: Electronic Resource
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  • 4
    Electronic Resource
    Electronic Resource
    Springer
    Journal of atmospheric chemistry 21 (1995), S. 61-79 
    ISSN: 1573-0662
    Keywords: ClO ; HCl ; ozone loss
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract We call attention to the likely importance of the potential reaction OH+ClO→HCl+O2. It may only be a minor channel for the reaction of OH with ClO, which is often ignored in models, but if it occurs it considerably increases the rate of recovery of HCl after an air parcel has encountered a polar stratospheric cloud (PSC). The net effect of this reaction on the ozone concentration depends on the relative HCl concentration and whether the air parcel is in a PSC. When an air parcel is in a PSC and the HCl concentration is less than the sum of the HOCl and ClONO2 concentrations, heterogeneous ClO x production is rate limited by the production of HCl. Under these conditions the reaction allows HCl to be reprocessed more rapidly by the heterogeneous reactions of HCl with HOCl and ClONO2. This allows high ClO x concentration to be maintained for longer, and at a slightly higher level, than would otherwise be possible which in turn leads to more ozone depletion. When there are PSCs but HCl is in excess, or outside of the PSC regions (i.e. during the recovery phase), the reaction will always reduce the ClO/HCl ratio and hence slightly reduce the ozone loss.
    Type of Medium: Electronic Resource
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  • 5
    ISSN: 1573-0662
    Keywords: ClO ; Fourier transform infrared
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Infrared absorption features due to ClO in the lower stratosphere have been identified from groundbased solar absorption spectra taken from Aberdeen, U.K. (57° N, 2° W) on 20 January 1995. A vertical column abundance of 3.42 (±0.47)×1015 molec cm-2 has been derived from 13 independent absorption features in the P and R branches of the (0–1) vibration-rotation band of 35ClO, spanning the spectral region 817–855 cm-1. The observed absorption features are consistent with very high levels of ClO (approximately 2.6 parts per billion by volume (ppbv)) in the altitude range 16–22 km. A comparison of this profile with a 3D chemical transport model profile indicates the observation was made inside the polar vortex and shows good qualitative agreement but the model underestimates the concentrations of ClO. Simultaneous measurements of other species were made including HCl, HF and ClONO2. These columns yield a value for HCl+ClONO2+ClO of 7.02±0.65×1015 molec cm-2. This is lower than the total inorganic chlorine (ClO y ) column of 10.7±1.6×1015 molec cm-2 estimated from mean measured (HCl+ClONO2)/HF ratios together with in-vortex HF measurements. The discrepancy is probably due to significant amounts of the ClO dimer (Cl2O2) in the lower part of the stratosphere. The measurements of highly elevated levels of ClO are used to estimate O3 loss rates at the 400, 475 and 550 K levels making assumptions about the probable distribution of ClO and Cl2O2. These are compared with loss rates derived from ozone sonde data.
    Type of Medium: Electronic Resource
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  • 6
    Publication Date: 2019-09-23
    Description: Emissions of halogenated very short-lived substances (VSLS) are poorly constrained. However, their inclusion in global models is required to simulate a realistic inorganic bromine (Bry) loading in both the troposphere, where bromine chemistry perturbs global oxidizing capacity, and in the stratosphere, where it is a major sink for ozone (O3). We have performed simulations using a 3-D chemical transport model (CTM) including three top-down and a single bottom-up derived emission inventory of the major brominated VSLS bromoform (CHBr3) and dibromomethane (CH2Br2). We perform the first concerted evaluation of these inventories, comparing both the magnitude and spatial distribution of emissions. For a quantitative evaluation of each inventory, model output is compared with independent long-term observations at National Oceanic and Atmospheric Administration (NOAA) ground-based stations and with aircraft observations made during the NSF HIAPER Pole-to-Pole Observations (HIPPO) project. For CHBr3, the mean absolute deviation between model and surface observation ranges from 0.22 (38%) to 0.78 (115%) parts per trillion (ppt) in the tropics, depending on emission inventory. For CH2Br2, the range is 0.17 (24%) to 1.25 (167%) ppt. We also use aircraft observations made during the 2011 "Stratospheric Ozone: Halogen Impacts in a Varying Atmosphere" (SHIVA) campaign, in the tropical West Pacific. Here, the performance of the various inventories also varies significantly, but overall the CTM is able to reproduce observed CHBr3 well in the free troposphere using an inventory based on observed sea-to-air fluxes. Finally, we identify the range of uncertainty associated with these VSLS emission inventories on stratospheric bromine loading due to VSLS (BryVSLS). Our simulations show BryVSLS ranges from ~ 4.0 to 8.0 ppt depending on the inventory. We report an optimised estimate at the lower end of this range (~ 4 ppt) based on combining the CHBr3 and CH2Br2 inventories which give best agreement with the compilation of observations in the tropics.
    Type: Article , PeerReviewed , info:eu-repo/semantics/article
    Format: text
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  • 7
    Publication Date: 2020-07-24
    Description: The 11-year solar cycles in ozone and temperature are examined using new simulations of coupled chemistry climate models. The results show a secondary maximum in stratospheric tropical ozone, in agreement with satellite observations and in contrast with most previously published simulations. The mean model response varies by up to about 2.5% in ozone and 0.8 K in temperature during a typical solar cycle, at the lower end of the observed ranges of peak responses. Neither the upper atmospheric effects of energetic particles nor the presence of the quasi biennial oscillation is necessary to simulate the lower stratospheric response in the observed low latitude ozone concentration. Comparisons are also made between model simulations and observed total column ozone. As in previous studies, the model simulations agree well with observations. For those models which cover the full temporal range 1960–2005, the ozone solar signal below 50 hPa changes substantially from the first two solar cycles to the last two solar cycles. Further investigation suggests that this difference is due to an aliasing between the sea surface temperatures and the solar cycle during the first part of the period. The relationship between these results and the overall structure in the tropical solar ozone response is discussed. Further understanding of solar processes requires improvement in the observations of the vertically varying and column integrated ozone.
    Type: Article , PeerReviewed
    Format: text
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  • 8
    Publication Date: 2016-10-04
    Description: We carry out a case study of the transport and chemistry of bromoform and its product gases (PGs) in a sea breeze driven convective episode on 19 November 2011 along the North West coast of Borneo during the "Stratospheric ozone: Halogen Impacts in a Varying Atmosphere" (SHIVA) campaign. We use ground based, ship, aircraft and balloon sonde observations made during the campaign, and a 3-D regional online transport and chemistry model capable of resolving clouds and convection explicitly that includes detailed bromine chemistry. The model simulates the temperature, wind speed, wind direction fairly well for the most part, and adequately captures the convection location, timing, and intensity. The simulated transport of bromoform from the boundary layer up to 12 km compares well to aircraft observations to support our conclusions. The model makes several predictions regarding bromine transport from the boundary layer to the level of convective detrainment (11 to 12 km). First, the majority of bromine undergoes this transport as bromoform. Second, insoluble organic bromine carbonyl species are transported to between 11 and 12 km, but only form a small proportion of the transported bromine. Third, soluble bromine species, which include bromine organic peroxides, hydrobromic acid (HBr), and hypobromous acid (HOBr), are washed out efficiently within the core of the convective column. Fourth, insoluble inorganic bromine species (principally Br2) are not washed out of the convective column, but are also not transported to the altitude of detrainment in large quantities. We expect that Br2 will make a larger relative contribution to the total vertical transport of bromine atoms in scenarios with higher CHBr3 mixing ratios in the boundary layer, which have been observed in other regions. Finally, given the highly detailed description of the chemistry, transport and washout of bromine compounds within our simulations, we make a series of recommendations about the physical and chemical processes that should be represented in 3-D chemical transport models (CTMs) and chemistry climate models (CCMs), which are the primary theoretical means of estimating the contribution made by CHBr3 and other very short-lived substances (VSLS) to the stratospheric bromine budget.
    Type: Article , NonPeerReviewed , info:eu-repo/semantics/article
    Format: text
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  • 9
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    World Meteorological Organization
    In:  In: Scientific Assessment of Ozone Depletion: 2010, Chapter 2. World Meteorological Organization, Geneva, Switzerland, pp. 1-80.
    Publication Date: 2012-07-06
    Type: Book chapter , NonPeerReviewed
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  • 10
    Publication Date: 2018-01-19
    Description: The goal of the Chemistry-Climate Model Validation (CCMVal) activity is to improve understanding of chemistry-climate models (CCMs) through process-oriented evaluation and to provide reliable projections of stratospheric ozone and its impact on climate. An appreciation of the details of model formulations is essential for understanding how models respond to the changing external forcings of greenhouse gases and ozone-depleting substances, and hence for understanding the ozone and climate forecasts produced by the models participating in this activity. Here we introduce and review the models used for the second round (CCMVal-2) of this intercomparison, regarding the implementation of chemical, transport, radiative, and dynamical processes in these models. In particular, we review the advantages and problems associated with approaches used to model processes of relevance to stratospheric dynamics and chemistry. Furthermore, we state the definitions of the reference simulations performed, and describe the forcing data used in these simulations. We identify some developments in chemistry-climate modeling that make models more physically based or more comprehensive, including the introduction of an interactive ocean, online photolysis, troposphere-stratosphere chemistry, and non-orographic gravity-wave deposition as linked to tropospheric convection. The relatively new developments indicate that stratospheric CCM modeling is becoming more consistent with our physically based understanding of the atmosphere.
    Type: Article , PeerReviewed
    Format: text
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