scholarly journals Contribution of liquid, NAT and ice particles to chlorine activation and ozone depletion in Antarctic winter and spring

2015 ◽  
Vol 15 (4) ◽  
pp. 2019-2030 ◽  
Author(s):  
O. Kirner ◽  
R. Müller ◽  
R. Ruhnke ◽  
H. Fischer
Keyword(s):  
Atmospheric Chemistry ◽  
Ozone Depletion ◽  
Climate Model ◽  
Heterogeneous Reactions ◽  
Heterogeneous Chemistry ◽  
Ice Particles ◽  
Synoptic Conditions ◽  
Almost All ◽  
Stratospheric Clouds ◽  
The Impact

Abstract. Heterogeneous reactions in the Antarctic stratosphere are the cause of chlorine activation and ozone depletion, but the relative roles of different types of polar stratospheric clouds (PSCs) in chlorine activation is an open question. We use multi-year simulations of the chemistry-climate model ECHAM5/MESSy for Atmospheric Chemistry (EMAC) to investigate the impact that the various types of PSCs have on Antarctic chlorine activation and ozone loss. One standard and three sensitivity EMAC simulations have been performed. In all simulations a Newtonian relaxation technique using the ERA-Interim reanalysis was applied to simulate realistic synoptic conditions. In the three sensitivity simulations, we only changed the heterogeneous chemistry on PSC particles by switching the chemistry on liquid, nitric acid trihydrate (NAT) and ice particles on and off. The results of these simulations show that the significance of heterogeneous reactions on NAT and ice particles for chlorine activation and ozone depletion in Antarctic winter and spring is small in comparison to the significance of heterogeneous reactions on liquid particles. Liquid particles alone are sufficient to activate almost all of the available chlorine, with the exception of the upper PSC regions between 10 and 30 hPa, where temporarily ice particles show a relevant contribution. Shortly after the first PSC occurrence, NAT particles contribute a small fraction to chlorine activation. Heterogeneous chemistry on liquid particles is responsible for more than 90% of the ozone depletion in Antarctic spring in the model simulations. In high southern latitudes, heterogeneous chemistry on ice particles causes only up to 5 DU of additional ozone depletion in the column and heterogeneous chemistry on NAT particles less than 0.5 DU. The simulated HNO3, ClO and O3 results agree closely with observations from the Microwave Limb Sounder (MLS) onboard NASA's Aura satellite.

scholarly journals Contribution of liquid, NAT and ice particles to chlorine activation and ozone depletion during Antarctic winter and spring

2014 ◽  
Vol 14 (10) ◽  
pp. 14833-14854
Author(s):  
O. Kirner ◽  
R. Müller ◽  
R. Ruhnke ◽  
H. Fischer
Keyword(s):  
Ozone Depletion ◽  
Climate Model ◽  
Heterogeneous Reactions ◽  
Heterogeneous Chemistry ◽  
Ice Particles ◽  
Reservoir Species ◽  
Almost All ◽  
Column Ozone ◽  
Open Question ◽  
The Impact

Abstract. Heterogeneous reactions in the Antarctic stratosphere are the cause of chlorine activation and ozone depletion, but the relative roles of different types of PSCs in chlorine activation is an open question. We use multi-year simulations of the chemistry-climate model EMAC to investigate the impact that the various types of PSCs have on Antarctic chlorine activation and ozone loss. One standard and three sensitivity EMAC simulations have been performed. The results of these simulations show that the significance of heterogeneous reactions on NAT and ice particles, in comparison to liquid particles, is subordinate regarding chlorine activation and ozone depletion in Antarctic winter and spring. The heterogeneous chemistry on liquid particles is sufficient to activate at least 90% of the chlorine reservoir species. With the exception of the upper PSC regions between 10 and 30 hPa where temporarily the ice particles have a relevant contribution to the chlorine activation and during the initial PSC occurrence with short NAT contributions the liquid particles alone are sufficient to activate almost all of the available chlorine. In the model simulations heterogeneous chemistry on liquid particles is responsible for more than 90% of the ozone depletion in Antarctic spring. Only up to 5 DU of column ozone in high southern latitudes is depleted by chlorine activation due to additional heterogeneous chemistry on ice particles and less than 0.5 DU due to additional heterogeneous chemistry on NAT particles.

scholarly journals The impact of polar stratospheric ozone loss on Southern Hemisphere stratospheric circulation and climate

2014 ◽  
Vol 14 (12) ◽  
pp. 18049-18082
Author(s):  
J. Keeble ◽  
P. Braesicke ◽  
N. L. Abraham ◽  
H. K. Roscoe ◽  
J. A. Pyle
Keyword(s):  
Southern Hemisphere ◽  
Lower Stratosphere ◽  
Climate Model ◽  
Stratospheric Ozone ◽  
Vertical Component ◽  
Polar Vortex ◽  
Heterogeneous Reactions ◽  
Ozone Loss ◽  
Stratospheric Clouds ◽  
The Impact

Abstract. The impact of polar stratospheric ozone loss resulting from chlorine activation on polar stratospheric clouds is examined using a pair of model integrations run with the fully coupled chemistry climate model UM-UKCA. Suppressing chlorine activation through heterogeneous reactions is found to produce modelled ozone differences consistent with observed ozone differences between the present and pre-ozone hole period. Statistically significant high latitude Southern Hemisphere (SH) ozone loss begins in August and peaks in October-November, with >75% of ozone destroyed at 50 hPa. Associated with this ozone destruction is a >12 K decrease of the lower polar stratospheric temperatures and an increase of >6 K in the upper stratosphere. The heating components of this temperature change are diagnosed and it is found that the temperature dipole is the result of decreased shortwave heating in the lower stratosphere and increased dynamical heating in the upper stratosphere. The cooling of the polar lower stratosphere leads, through thermal wind balance, to an acceleration of the polar vortex and delays its breakdown by ~2 weeks. A link between lower stratospheric zonal wind speed, the vertical component of the EP flux, Fz, and the residual mean vertical circulation, w*, is identified. In December and January, increased westerly winds lead to increases in Fz, associated with an increase in tropopause height. The resulting increase in wavebreaking leads to enhanced downwelling/reduced upwelling over the polar cap. Many of the stratospheric signals modelled in this study propagate down to the troposphere, and lead to significant surface changes in December.

scholarly journals Impacts of Ozone Changes in the Tropopause Layer on Stratospheric Water Vapor

Atmosphere ◽  
2021 ◽  
Vol 12 (3) ◽  
pp. 291
Author(s):  
Jinpeng Lu ◽  
Fei Xie ◽  
Hongying Tian ◽  
Jiali Luo
Keyword(s):  
Water Vapor ◽  
Ozone Depletion ◽  
Climate Model ◽  
Global Climate ◽  
Stratospheric Water Vapor ◽  
Radiative Processes ◽  
Low Latitudes ◽  
Cold Point ◽  
The Impact ◽  
Tropopause Temperature

Stratospheric water vapor (SWV) changes play an important role in regulating global climate change, and its variations are controlled by tropopause temperature. This study estimates the impacts of tropopause layer ozone changes on tropopause temperature by radiative process and further influences on lower stratospheric water vapor (LSWV) using the Whole Atmosphere Community Climate Model (WACCM4). It is found that a 10% depletion in global (mid-low and polar latitudes) tropopause layer ozone causes a significant cooling of the tropical cold-point tropopause with a maximum cooling of 0.3 K, and a corresponding reduction in LSWV with a maximum value of 0.06 ppmv. The depletion of tropopause layer ozone at mid-low latitudes results in cooling of the tropical cold-point tropopause by radiative processes and a corresponding LSWV reduction. However, the effect of polar tropopause layer ozone depletion on tropical cold-point tropopause temperature and LSWV is opposite to and weaker than the effect of tropopause layer ozone depletion at mid-low latitudes. Finally, the joint effect of tropopause layer ozone depletion (at mid-low and polar latitudes) causes a negative cold-point tropopause temperature and a decreased tropical LSWV. Conversely, the impact of a 10% increase in global tropopause layer ozone on LSWV is exactly the opposite of the impact of ozone depletion. After 2000, tropopause layer ozone decreased at mid-low latitudes and increased at high latitudes. These tropopause layer ozone changes at different latitudes cause joint cooling in the tropical cold-point tropopause and a reduction in LSWV. Clarifying the impacts of tropopause layer ozone changes on LSWV clearly is important for understanding and predicting SWV changes in the context of future global ozone recovery.

Impact of heterogeneous chemistry on the distribution of Glyoxal and Methylglyoxal in the troposphere

2021 ◽  
Author(s):  
Ramiro Checa-Garcia ◽  
Didier Didier Hauglustaine ◽  
Yves Balkanski ◽  
Paola Formenti
Keyword(s):  
Atmospheric Chemistry ◽  
Climate Models ◽  
Climate Model ◽  
Global Climate ◽  
Global Climate Model ◽  
Experimental Simulation ◽  
Heterogeneous Chemistry ◽  
Closed Set ◽  
Sensitivity Studies ◽  
The Tropics

<p>Glyoxal (GL) and methylglyoxal (MGL) are the smallest di-carbonyls present in the atmosphere. They hydrate easily, a process that is followed by an oligomerisation. As a consequence, it is considered that they participate actively in the formation of secondary organic aerosols (SOA) and therefore, they are being introduced in the current climate models with interactive chemistry to assess their importance on atmospheric chemistry. In our study we present the introduction of glyoxal in the INCA global model. A new closed set of gas-phase  reactions is analysed first with a box model. Then the simulated global distribution of glyoxal by the global climate model is compared with satellite observations. We show that the oxidation of volatile organic compounds and acetylene, together with the photolysis of more complex di-carbonyls allows us to reproduce well glyoxal seasonal cycle in the tropics but it requires an additional sink in several northern hemispheric regions. Additional sensitivity studies are being conducted by introducing  GL and MGL interactions with dust and SOA according to new uptake  coefficients obtained by dedicated experiments in the CESAM instrument (Chamber of Experimental Simulation of Atmospheric Multiphases). The effects of these heterogeneous chemistry processes will be quantified in the light of the new chamber measurements  and also evaluated in terms of optical properties of aged dust aerosol  and the changes in direct radiative effects  of the involved aerosol species.</p>

Atmospheric impacts of short-lived chlorinated species over the recent past: a chemistry-climate perspective

2021 ◽  
Author(s):  
Ewa Bednarz ◽  
Ryan Hossaini ◽  
Luke Abraham ◽  
Peter Braesicke ◽  
Martyn Chipperfield
Keyword(s):  
Atmospheric Chemistry ◽  
Climate Model ◽  
Stratospheric Ozone ◽  
Lower Boundary ◽  
Montreal Protocol ◽  
Recent Past ◽  
Substantial Impact ◽  
Ozone Depleting Substances ◽  
The Impact

<p>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<sub>3</sub>) and dichloromethane (CH<sub>2</sub>Cl<sub>2</sub>), 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. </p><p> </p><p>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.</p><p> </p><p>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 ‘nudging’, 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.</p>

scholarly journals Implications of potential future grand solar minimum for ozone layer and climate

2017 ◽  
Author(s):  
Pavle Arsenovic ◽  
Eugene Rozanov ◽  
Julien Anet ◽  
Andrea Stenke ◽  
Thomas Peter
Keyword(s):  
Solar Activity ◽  
Greenhouse Gas ◽  
21St Century ◽  
Atmospheric Chemistry ◽  
Solar Minimum ◽  
Climate Model ◽  
Ghg Emissions ◽  
Ozone Production ◽  
22Nd Century ◽  
The Impact

Abstract. Continued anthropogenic greenhouse gas (GHG) emissions are expected to cause further global warming throughout the 21st century. Understanding potential interferences with natural forcings is thus of great interest. Here we investigate the impact of a recently proposed 21st century grand solar minimum on atmospheric chemistry and climate using the SOCOL3-MPIOM chemistry-climate model with interactive ocean. We examine several model simulations for the period 2000–2199, following the greenhouse gas scenario RCP4.5, but with different solar forcings: the reference simulation is forced by perpetual repetition of solar cycle 23 until the year 2199, whereas the grand solar minimum simulations assume strong declines in solar activity of 3.5 and 6.5 W m−2 with different durations. Decreased solar activity is found to yield up to a doubling of the GHG induced stratospheric and mesospheric cooling. Under the grand solar minimum scenario tropospheric temperatures are also projected to decrease. On the global scale the reduced solar forcing compensates at most 15 % of the expected greenhouse warming at the end of 21st and around 25 % at the end of 22nd century. The regional effects are predicted to be stronger, in particular in northern high latitude winter. In the stratosphere, the reduced incoming ultraviolet radiation leads to less ozone production by up to 8 %, which overcompensates the anticipated ozone increase due to reduced stratospheric temperatures and an acceleration of the Brewer-Dobson circulation. This, in turn, leads to a delay in total ozone column recovery from anthropogenic chlorine-induced depletion, with a global ozone recovery to the pre-ozone hole values happening only upon completion of the grand solar minimum in the 22nd century or later.

Investigation of strongly enhanced methane Part I: Chemical feedbacks and rapid adjustments.

2020 ◽  
Author(s):  
Franziska Winterstein ◽  
Patrick Jöckel ◽  
Martin Dameris ◽  
Michael Ponater ◽  
Fabian Tanalski ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
Climate Model ◽  
Numerical Study ◽  
Stratospheric Ozone ◽  
Lower Boundary ◽  
Tropospheric Chemistry ◽  
Substantial Part ◽  
Mixing Ratios ◽  
The Impact

<p>Methane (CH<sub>4</sub>) is the second most important greenhouse gas, which atmospheric concentration is influenced by human activities and currently on a sharp rise. We present a study with numerical simulations using a Chemistry-Climate-Model (CCM), which are performed to assess possible consequences of strongly enhanced CH<sub>4</sub> concentrations in the Earth's atmosphere for the climate.</p><p>Our analysis includes experiments with 2xCH<sub>4</sub> and 5xCH<sub>4</sub> present day (2010) lower boundary mixing ratios using the CCM EMAC. The simulations are conducted with prescribed oceanic conditions, mimicking present day tropospheric temperatures as its changes are largely suppressed. By doing so we are able to investigate the quasi-instantaneous chemical impact on the atmosphere. We find that the massive increase in CH<sub>4</sub> strongly influences the tropospheric chemistry by reducing the OH abundance and thereby extending the tropospheric CH<sub>4</sub> lifetime as well as the residence time of other chemical pollutants. The region above the tropopause is impacted by a substantial rise in stratospheric water vapor (SWV). The stratospheric ozone (O<sub>3</sub>) column increases overall, but SWV induced stratospheric cooling also leads to enhanced ozone depletion in the Antarctic lower stratosphere. Regional  patterns of ozone change are affected by modification of stratospheric dynamics, i.e. increased tropical up-welling and stronger meridional transport  towards the polar regions. We calculate the net radiative impact (RI) of the 2xCH<sub>4</sub> experiment to be 0.69 W m<sup>-2</sup> and for the 5xCH<sub>4</sub> experiment to be 1.79 W m<sup>-2</sup>. A substantial part of the RI is contributed by chemically induced O<sub>3</sub> and SWV changes, in line with previous radiative forcing estimates and is for the first time splitted and spatially asigned to its chemical contributors.</p><p>This numerical study using a CCM with prescibed oceanic conditions shows the rapid responses to significantly enhanced CH<sub>4</sub> mixing ratios, which is the first step towards investigating the impact of possible strong future CH<sub>4</sub> emissions on atmospheric chemistry and its feedback on climate.</p>

scholarly journals Impact of high solar zenith angles on dynamical and chemical processes in a coupled chemistry-climate model

2003 ◽  
Vol 3 (4) ◽  
pp. 3681-3711
Author(s):  
D. Lamago ◽  
M. Dameris ◽  
C. Schnadt ◽  
V. Eyring ◽  
C. Brühl
Keyword(s):  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Climate Model ◽  
Chemical Processes ◽  
Sensitivity Experiment ◽  
Mean Values ◽  
Ozone Destruction ◽  
The Impact ◽  
Fully Coupled ◽  
Ozone Column

Abstract. Actinic fluxes at high solar zenith angles (SZAs) are important for atmospheric chemistry, especially under twilight conditions in polar winter and spring. The results of a sensitivity experiment employing the fully coupled 3D chemistry-climate model ECHAM4.L39(DLR)/CHEM have been analysed to quantify the impact of SZAs greater than 87.5° on dynamical and chemical processes in the lower stratosphere, in particular their influence on the ozone layer. Although the actinic fluxes at SZAs larger than 87.5° are small, ozone concentrations are significantly affected because daytime photolytic ozone destruction is switched on earlier, especially the conversion of Cl2 and Cl2O2 into ClO at the end of polar night in the lower stratosphere. Comparing climatological mean ozone column values of a simulation considering SZAs up to 93° with those of the sensitivity run with SZAs confined to 87.5° total ozone is reduced by about 20% in the polar Southern Hemisphere, i.e., the ozone hole is "deeper'' if twilight conditions are considered in the model because there is 2–3 weeks more time for ozone destruction. This causes an additional cooling of the polar lower stratosphere (50 hPa) up to −4 K with obvious consequences for chemical processes. In the Northern Hemisphere the impact of high SZAs cannot be determined on the basis of climatological mean values due to the pronounced dynamic variability of the stratosphere in winter and spring.

scholarly journals Evaluation of CLaMS, KASIMA and ECHAM5/MESSy1 simulations in the lower stratosphere using observations of Odin/SMR and ILAS/ILAS-II

2009 ◽  
Vol 9 (1) ◽  
pp. 1977-2020
Author(s):  
F. Khosrawi ◽  
R. Müller ◽  
M. H. Proffitt ◽  
R. Ruhnke ◽  
O. Kirner ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
General Circulation ◽  
Lower Stratosphere ◽  
Climate Model ◽  
Middle Atmosphere ◽  
Circulation Model ◽  
Lagrangian Model ◽  
Data Sets ◽  
Data Set ◽  
The Impact

Abstract. 1-year data sets of monthly averaged nitrous oxide (N2O) and ozone (O3) derived from satellite measurements were used as a tool for the evaluation of atmospheric photochemical models. Two 1-year data sets, one derived from the Improved Limb Atmospheric Spectrometer (ILAS and ILAS-II) and one from the Odin Sub-Millimetre Radiometer (Odin/SMR) were employed. Here, these data sets are used for the evaluation of two Chemical Transport Models (CTMs), the Karlsruhe Simulation Model of the Middle Atmosphere (KASIMA) and the Chemical Lagrangian Model of the Stratosphere (CLaMS) as well as for one Chemistry-Climate Model (CCM), the atmospheric chemistry general circulation model ECHAM5/MESSy1 (E5M1) in the lower stratosphere with focus on the Northern Hemisphere. Since the Odin/SMR measurements cover the entire hemisphere, the evaluation is performed for the entire hemisphere as well as for the low latitudes, midlatitudes and high latitudes using the Odin/SMR 1-year data set as reference. To assess the impact of using different data sets for such an evaluation study we repeat the evaluation for the polar lower stratosphere using the ILAS/ILAS-II data set. Only small differences were found using ILAS/ILAS-II instead of Odin/SMR as a reference, thus, showing that the results are not influenced by the particular satellite data set used for the evaluation. The evaluation of CLaMS, KASIMA and E5M1 shows that all models are in good agreement with Odin/SMR and ILAS/ILAS-II. Differences are generally in the range of ±20%. Larger differences (up to −40%) are found in all models at 500±25 K for N2O mixing ratios greater than 200 ppb. Generally, the largest differences were found for the tropics and the lowest for the polar regions. However, an underestimation of polar winter ozone loss was found both in KASIMA and E5M1 both in the Northern and Southern Hemisphere.

scholarly journals Stratospheric lifetime ratio of CFC-11 and CFC-12 from satellite and model climatologies

2014 ◽  
Vol 14 (11) ◽  
pp. 16865-16906 ◽  
Author(s):  
L. Hoffmann ◽  
C. M. Hoppe ◽  
R. Müller ◽  
G. S. Dutton ◽  
J. C. Gille ◽  
...  
Keyword(s):  
Global Warming ◽  
Atmospheric Chemistry ◽  
Climate Model ◽  
Transport Model ◽  
Stratospheric Ozone ◽  
Michelson Interferometer ◽  
Coupled Model ◽  
Model System ◽  
Satellite Observations ◽  
The Impact

Abstract. Chlorofluorocarbons (CFCs) play a key role in stratospheric ozone loss and are strong infrared absorbers that contribute to global warming. The stratospheric lifetimes of CFCs are a measure of their global loss rates that are needed to determine global warming and ozone depletion potentials. We applied the tracer-tracer correlation approach to zonal mean climatologies from satellite measurements and model data to assess the lifetimes of CFCl3 (CFC-11) and CF2Cl2 (CFC-12). We present estimates of the CFC-11/CFC-12 lifetime ratio and the absolute lifetime of CFC-12, based on a reference lifetime of 52 yr for CFC-11. We analyzed climatologies from three satellite missions, the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS), the HIgh Resolution Dynamics Limb Sounder (HIRDLS), and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). We found a CFC-11/CFC-12 lifetime ratio of 0.47±0.08 and a CFC-12 lifetime of 111(96–132) yr for ACE-FTS, a ratio of 0.46±0.07 and a lifetime of 112(97–133) yr for HIRDLS, and a ratio of 0.46±0.08 and a lifetime of 112(96–135) yr for MIPAS. The error-weighted, combined CFC-11/CFC-12 lifetime ratio is 0.47±0.04 and the CFC-12 lifetime estimate is 112(102–123) yr. These results agree with the recent Stratosphere-troposphere Processes And their Role in Climate (SPARC) reassessment, which recommends lifetimes of 52(43–67) yr and 102(88–122) yr, respectively. Having smaller uncertainties than the results from other recent studies, our estimates can help to better constrain CFC-11 and CFC-12 lifetime recommendations in future scientific studies and assessments. Furthermore, the satellite observations were used to validate first simulation results from a new coupled model system, which integrates a Lagrangian chemistry transport model into a climate model. For the coupled model we found a CFC-11/CFC-12 lifetime ratio of 0.48±0.07 and a CFC-12 lifetime of 110(95–129) yr, based on a ten-year perpetual run. Closely reproducing the satellite observations, the new model system will likely become a useful tool to assess the impact of advective transport, mixing, and photochemistry as well as climatological variability on the stratospheric lifetimes of long-lived tracers.

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