Atmospheric Chemistry

Author(s):  
Donald J. Kern

The complex chemistry and basic physics of Earth's atmosphere will be reduced to three main sections within the context of the chemical reactivities of predominant chemical species and the additional role of photochemistry from solar radiation. The three areas of chemical interactions and photochemical reactions in the atmosphere discussed are (1) the reactivities and relationships between chemical species that can affect tropospheric and stratospheric ozone concentrations, (2) reactions between chemical species that create acid rain, and (3) the chemical species, sources, and reactions that are believed to be contributing to climate change. These three areas in atmospheric dynamics will comprise this chapter along with some of the documented effects on ecological systems, human health, and infrastructure.

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

<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>


2012 ◽  
Vol 12 (19) ◽  
pp. 9335-9353 ◽  
Author(s):  
H. G. Ouwersloot ◽  
J. Vilà-Guerau de Arellano ◽  
A. C. Nölscher ◽  
M. C. Krol ◽  
L. N. Ganzeveld ◽  
...  

Abstract. We studied the atmospheric boundary layer (ABL) dynamics and the impact on atmospheric chemistry during the HUMPPA-COPEC-2010 campaign. We used vertical profiles of potential temperature and specific moisture, obtained from 132 radio soundings, to determine the main boundary layer characteristics during the campaign. We propose a classification according to several main ABL prototypes. Further, we performed a case study of a single day, focusing on the convective boundary layer, to analyse the influence of the dynamics on the chemical evolution of the ABL. We used a mixed layer model, initialized and constrained by observations. In particular, we investigated the role of large scale atmospheric dynamics (subsidence and advection) on the ABL development and the evolution of chemical species concentrations. We find that, if the large scale forcings are taken into account, the ABL dynamics are represented satisfactorily. Subsequently, we studied the impact of mixing with a residual layer aloft during the morning transition on atmospheric chemistry. The time evolution of NOx and O3 concentrations, including morning peaks, can be explained and accurately simulated by incorporating the transition of the ABL dynamics from night to day. We demonstrate the importance of the ABL height evolution for the representation of atmospheric chemistry. Our findings underscore the need to couple the dynamics and chemistry at different spatial scales (from turbulence to mesoscale) in chemistry-transport models and in the interpretation of observational data.


2014 ◽  
Vol 10 (5) ◽  
pp. 1925-1938 ◽  
Author(s):  
A. Mauri ◽  
B. A. S. Davis ◽  
P. M. Collins ◽  
J. O. Kaplan

Abstract. The atmospheric circulation is a key area of uncertainty in climate model simulations of future climate change, especially in mid-latitude regions such as Europe where atmospheric dynamics have a significant role in climate variability. It has been proposed that the mid-Holocene was characterized in Europe by a stronger westerly circulation in winter comparable with a more positive AO/NAO, and a weaker westerly circulation in summer caused by anti-cyclonic blocking near Scandinavia. Model simulations indicate at best only a weakly positive AO/NAO, whilst changes in summer atmospheric circulation have not been widely investigated. Here we use a new pollen-based reconstruction of European mid-Holocene climate to investigate the role of atmospheric circulation in explaining the spatial pattern of seasonal temperature and precipitation anomalies. We find that the footprint of the anomalies is entirely consistent with those from modern analogue atmospheric circulation patterns associated with a strong westerly circulation in winter (positive AO/NAO) and a weak westerly circulation in summer associated with anti-cyclonic blocking (positive SCAND). We find little agreement between the reconstructed anomalies and those from 14 GCMs that performed mid-Holocene experiments as part of the PMIP3/CMIP5 project, which show a much greater sensitivity to top-of-the-atmosphere changes in solar insolation. Our findings are consistent with data–model comparisons on contemporary timescales that indicate that models underestimate the role of atmospheric circulation in recent climate change, whilst also highlighting the importance of atmospheric dynamics in explaining interglacial warming.


2017 ◽  
Vol 17 (18) ◽  
pp. 11313-11329 ◽  
Author(s):  
Stefanie Falk ◽  
Björn-Martin Sinnhuber ◽  
Gisèle Krysztofiak ◽  
Patrick Jöckel ◽  
Phoebe Graf ◽  
...  

Abstract. Very short-lived substances (VSLS) contribute as source gases significantly to the tropospheric and stratospheric bromine loading. At present, an estimated 25 % of stratospheric bromine is of oceanic origin. In this study, we investigate how climate change may impact the ocean–atmosphere flux of brominated VSLS, their atmospheric transport, and chemical transformations and evaluate how these changes will affect stratospheric ozone over the 21st century. Under the assumption of fixed ocean water concentrations and RCP6.0 scenario, we find an increase of the ocean–atmosphere flux of brominated VSLS of about 8–10 % by the end of the 21st century compared to present day. A decrease in the tropospheric mixing ratios of VSLS and an increase in the lower stratosphere are attributed to changes in atmospheric chemistry and transport. Our model simulations reveal that this increase is counteracted by a corresponding reduction of inorganic bromine. Therefore the total amount of bromine from VSLS in the stratosphere will not be changed by an increase in upwelling. Part of the increase of VSLS in the tropical lower stratosphere results from an increase in the corresponding tropopause height. As the depletion of stratospheric ozone due to bromine depends also on the availability of chlorine, we find the impact of bromine on stratospheric ozone at the end of the 21st century reduced compared to present day. Thus, these studies highlight the different factors influencing the role of brominated VSLS in a future climate.


2016 ◽  
Vol 9 (10) ◽  
pp. 3685-3697 ◽  
Author(s):  
Nathan P. Gillett ◽  
Hideo Shiogama ◽  
Bernd Funke ◽  
Gabriele Hegerl ◽  
Reto Knutti ◽  
...  

Abstract. Detection and attribution (D&A) simulations were important components of CMIP5 and underpinned the climate change detection and attribution assessments of the Fifth Assessment Report of the Intergovernmental Panel on Climate Change. The primary goals of the Detection and Attribution Model Intercomparison Project (DAMIP) are to facilitate improved estimation of the contributions of anthropogenic and natural forcing changes to observed global warming as well as to observed global and regional changes in other climate variables; to contribute to the estimation of how historical emissions have altered and are altering contemporary climate risk; and to facilitate improved observationally constrained projections of future climate change. D&A studies typically require unforced control simulations and historical simulations including all major anthropogenic and natural forcings. Such simulations will be carried out as part of the DECK and the CMIP6 historical simulation. In addition D&A studies require simulations covering the historical period driven by individual forcings or subsets of forcings only: such simulations are proposed here. Key novel features of the experimental design presented here include firstly new historical simulations with aerosols-only, stratospheric-ozone-only, CO2-only, solar-only, and volcanic-only forcing, facilitating an improved estimation of the climate response to individual forcing, secondly future single forcing experiments, allowing observationally constrained projections of future climate change, and thirdly an experimental design which allows models with and without coupled atmospheric chemistry to be compared on an equal footing.


Author(s):  
I. K. Larin

A brief overview of the work of Russian scientists in the field of atmospheric chemistry in 20152018, including work on the chemistry of the troposphere, the chemistry of the ozone layer and on the role of chemistry in climate change is presented. Review has been prepared in the Commission on atmospheric chemistry of the meteorology and atmospheric sciences section of the national Geophysics Committee. The report was presented and approved at the XXVII General Assembly of the International Union of Geodesy and Geophysics (IUGG) 1.


2020 ◽  
Author(s):  
Peer Nowack ◽  
Nathan Luke Abraham ◽  
Peter Braesicke

<p>There is a plethora of ways in which the representation of upper tropospheric and stratospheric ozone (‘ozone feedbacks’) can affect the outcome of climate change simulations. Prominent examples include modulations of the tropospheric and stratospheric circulation, climate sensitivity, cloud formation, and stratospheric water vapour (e.g. [1-8]). Here I first revisit some recent work providing evidence for such effects. I then provide an update on a recently developed machine learning parameterization for ozone using the UK Earth System Model (UKESM1, [9]). Such a parameterization could adequately represent ozone feedbacks without adding the high computational expense of a fully interactive atmospheric chemistry scheme. The parameterization could also provide several notable scientific advantages, for example concerning the treatment of important chemistry-climate model biases. Finally, I put my results into the context of several other methods suggested as potential means for addressing ozone-related effects in idealized climate sensitivity simulations, also considering the still substantial uncertainties related to modelling ozone [10,11] and associated climate feedbacks [5,12].</p><p>References:</p><p>[1] Son et al. (2008), The impact of stratospheric ozone recovery on the Southern Hemisphere westerly jet. Science 320, 1486, doi:10.1126/science.1155939.</p><p>[2] Dietmüller et al. (2014), Interactive ozone induces a negative feedback in CO2-driven climate change simulations, Journal of Geophysical Research: Atmospheres 119, 1796-1805, doi:10.1002/2013JD020575.</p><p>[3] Chiodo & Polvani (2016), Reduction of climate sensitivity to solar forcing due to stratospheric ozone feedback, Journal of Climate 29, 4651-4663, doi:10.1175/JCLI-D-15-0721.1.</p><p>[4] Chiodo & Polvani (2017), Reduced Southern Hemispheric circulation response to quadrupled CO2 due to stratospheric ozone feedback, Geophysical Research Letters 43, 465-474, doi:10.1002/2016GL071011.</p><p>[5] Nowack et al. (2015), A large ozone-circulation feedback and its implications for global warming assessments. Nature Climate Change 5, 41-45, doi:10.1038/nclimate2451.</p><p>[6] Nowack et al. (2017), On the role of ozone feedback in the ENSO amplitude response under global warming, Geophysical Research Letters 44, doi:10.1002/2016GL072418.</p><p>[7] Nowack et al. (2018), The impact of stratospheric ozone feedbacks on climate sensitivity estimates. Journal of Geophysical Research: Atmospheres 123, 4630-4641, doi:10.1002/2017JD027943.</p><p>[8] Rieder et al. (2019), Is interactive ozone chemistry important to represent polar cap stratospheric temperature variability in Earth-System Models?, Environmental Research Letters 14, 044026, doi: 10.1088/1748-9326/ab07ff.</p><p>[9] Nowack et al. (2018), Using machine learning to build temperature-based ozone parameterizations for climate sensitivity simulations, Environmental Research Letters 13, 104016, doi:10.1088/1748-9326/aae2be.</p><p>[10] Chiodo & Polvani (2019), The response of the ozone layer to quadrupled CO2 concentrations: implications for climate, Journal of Climate 31, 3893-3907, doi:10.1175/JCLI-D-17-0492.1.</p><p>[11] Keeble et al. (2020), Evaluating stratospheric ozone and water vapour changes in CMIP6 models from 1850-2100, Atmospheric Chemistry and Physics Discussions.</p><p>[12] Dacie et al. (2019), A 1D RCE study of factors affecting the tropical tropopause layer and surface climate. Journal of Climate 32, 6769-6782, doi:10.1175/JCLI-D-18-0778.1.</p>


2019 ◽  
Vol 59 ◽  
pp. 10.1-10.52 ◽  
Author(s):  
T. J. Wallington ◽  
J. H. Seinfeld ◽  
J. R. Barker

Abstract Remarkable progress has occurred over the last 100 years in our understanding of atmospheric chemical composition, stratospheric and tropospheric chemistry, urban air pollution, acid rain, and the formation of airborne particles from gas-phase chemistry. Much of this progress was associated with the developing understanding of the formation and role of ozone and of the oxides of nitrogen, NO and NO2, in the stratosphere and troposphere. The chemistry of the stratosphere, emerging from the pioneering work of Chapman in 1931, was followed by the discovery of catalytic ozone cycles, ozone destruction by chlorofluorocarbons, and the polar ozone holes, work honored by the 1995 Nobel Prize in Chemistry awarded to Crutzen, Rowland, and Molina. Foundations for the modern understanding of tropospheric chemistry were laid in the 1950s and 1960s, stimulated by the eye-stinging smog in Los Angeles. The importance of the hydroxyl (OH) radical and its relationship to the oxides of nitrogen (NO and NO2) emerged. The chemical processes leading to acid rain were elucidated. The atmosphere contains an immense number of gas-phase organic compounds, a result of emissions from plants and animals, natural and anthropogenic combustion processes, emissions from oceans, and from the atmospheric oxidation of organics emitted into the atmosphere. Organic atmospheric particulate matter arises largely as gas-phase organic compounds undergo oxidation to yield low-volatility products that condense into the particle phase. A hundred years ago, quantitative theories of chemical reaction rates were nonexistent. Today, comprehensive computer codes are available for performing detailed calculations of chemical reaction rates and mechanisms for atmospheric reactions. Understanding the future role of atmospheric chemistry in climate change and, in turn, the impact of climate change on atmospheric chemistry, will be critical to developing effective policies to protect the planet.


2013 ◽  
Vol 9 (5) ◽  
pp. 5569-5592 ◽  
Author(s):  
A. Mauri ◽  
B. A. S. Davis ◽  
P. M. Collins ◽  
J. O. Kaplan

Abstract. The atmospheric circulation is a key area of uncertainty in climate model simulations of future climate change, especially in mid-latitude regions such as Europe where atmospheric dynamics have a significant role in climate variability. It has been proposed that the mid-Holocene was characterized in Europe by a stronger westerly circulation in winter comparable with a more positive AO/NAO, and a weaker westerly circulation in summer caused by anti-cyclonic blocking near Scandinavia. Model simulations indicate at best only a weakly positive AO/NAO, whilst changes in summer atmospheric circulation have not been widely investigated. Here we use a new pollen-based reconstruction of European mid-Holocene climate to investigate the role of atmospheric circulation in explaining the spatial pattern of seasonal temperature and precipitation anomalies. We find that the footprint of the anomalies is entirely consistent with those from modern analogue atmospheric circulation patterns associated with a strong westerly circulation in winter (positive AO/NAO) and a weak westerly circulation in summer (positive SCAND). We find little agreement between the reconstructed anomalies and those from a climate model simulation, which as with most model simulations shows a much greater sensitivity to local radiative forcing from top-of-the-atmosphere changes in solar insolation. Our findings are consistent with data-model comparisons on contemporary timescales that indicate that models underestimate the role of atmospheric circulation in climate change, whilst also highlighting the importance of atmospheric dynamics in explaining interglacial warming.


2017 ◽  
Author(s):  
Stefanie Falk ◽  
Björn-Martin Sinnhuber ◽  
Gisèle Krysztofiak ◽  
Patrick Jöckel ◽  
Phoebe Graf ◽  
...  

Abstract. Very short-lived source gases (VSLS) contribute significantly to the tropospheric and stratospheric bromine loading. At present, an estimated 25 % of stratospheric bromine is of oceanic origin. In this study, we investigate how climate change may impact the ocean-atmosphere flux of brominated VSLS, their atmospheric transport, chemical transformations, and evaluate how these changes will affect stratospheric ozone over the 21st century. Under the assumption of fixed ocean water concentrations and RCP6.0 scenario, we find an increase of the ocean-atmosphere flux of brominated VSLS of about 8–10 % by the end of the 21st century compared to present day. A decrease in the tropospheric mixing ratios of VSLS and an increase in the lower stratosphere are attributed to changes in atmospheric chemistry and transport. Our model simulations reveal that, in line with the reduction in the troposphere, the total amount of bromine from VSLS in the stratosphere will decrease during the 21st century. Part of the apparent increase of VSLS in the tropical lower stratosphere results from an increase in the corresponding tropopause height. As the depletion of stratospheric ozone due to bromine depends also on the availability of chlorine, we find the impact of bromine on stratospheric ozone at the end of the 21st century reduced compared to present day. Thus, these studies highlight the different factors influencing the role of brominated VSLS in a future climate.


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