scholarly journals Are contributions of emissions to ozone a matter of scale? – a study using MECO(n) (MESSy v2.50)

2020 ◽  
Vol 13 (1) ◽  
pp. 363-383 ◽  
Author(s):  
Mariano Mertens ◽  
Astrid Kerkweg ◽  
Volker Grewe ◽  
Patrick Jöckel ◽  
Robert Sausen
Keyword(s):  
Air Quality ◽  
Source Apportionment ◽  
Emission Inventory ◽  
Climate Model ◽  
Stratospheric Ozone ◽  
Model Resolution ◽  
Regional Models ◽  
Continental Scale ◽  
The Impact ◽  
Apportionment Methods

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.

scholarly journals Are contributions of emissions to ozone a matter of scale? – A study using MECO(n) (MESSy v2.50)

2019 ◽  
Author(s):  
Mariano Mertens ◽  
Astrid Kerkweg ◽  
Volker Grewe ◽  
Patrick Jöckel ◽  
Robert Sausen
Keyword(s):  
Source Apportionment ◽  
Emission Inventory ◽  
Climate Model ◽  
Ground Level ◽  
Emission Sources ◽  
Emission Inventories ◽  
Anthropogenic Emission ◽  
Model Resolution ◽  
Ground Level Ozone ◽  
Transport Emissions

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 high spatial resolution, while studies focusing on climate related questions often use coarsely resolved global models. It is well known that simulated ozone concentrations depend on the resolution of the model and the resolution of the emission inventory. Whether the contributions simulated by source apportionment approaches also depend on the model resolution, however, is still unclear. Therefore, this study is a first attempt to analyse the impact of the model, the model resolution, and the emission inventory resolution on simulated ozone contributions diagnosed with a tagging method. The differences of the ozone contributions caused by these factors are compared with differences which arise due to different emission inventories. To do so we apply the MECO(n) model system which on-line couples 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 (300 km resolution) are compared with the results of the regional model at 50 km (Europe) and 12 km (Germany) resolution. Averaged over Europe the simulated contributions of land transport emissions to ground-level ozone differ by 10 % at maximum. For other anthropogenic emission sources the differences are in the same order of magnitude, while the contribution of stratospheric ozone to ground level ozone differs by up to 30 % on average. This suggests that ozone contributions of anthropogenic emission sources averaged on continental scale are rather robust with respect to different models, model and emission inventory resolutions. On regional scale, however, we quantified differences of the contribution of land transport emissions to ozone of up to 20 %. Depending on the region the largest differences are either caused by inter model differences, or differences of the anthropogenic emission inventories. Clearly, the results strongly depend on the compared models and emission inventories and cannot necessarily be generalised, however we show how the inclusion of source apportionment methods can help in analysing inter-model differences.

scholarly journals Numerical analysis of agricultural emissions impacts on PM<sub>2.5</sub> in China using a high-resolution ammonia emission inventory

2020 ◽  
Vol 20 (16) ◽  
pp. 9979-9996
Author(s):  
Xiao Han ◽  
Lingyun Zhu ◽  
Mingxu Liu ◽  
Yu Song ◽  
Meigen Zhang
Keyword(s):  
Air Quality ◽  
High Resolution ◽  
Source Apportionment ◽  
Mass Concentration ◽  
Emission Inventory ◽  
Atmospheric Modeling ◽  
Central China ◽  
High Mass ◽  
Nh3 Emission ◽  
The Impact

Abstract. China is one of the largest agricultural countries in the world. Thus, NH3 emission from agricultural activities in China considerably affects the country's regional air quality and visibility. In this study, a high-resolution agricultural NH3 emission inventory compiled on 1 km × 1 km horizontal resolution was applied to calculate the NH3 mass burden in China and reliably estimate the influence of NH3 on agriculture. The key parameter emission factors of this inventory were enhanced by considering many experiment results, and the dynamic data of spatial and temporal information were updated using statistical data of 2015. In addition to fertilizers and husbandry, farmland ecosystems, livestock waste, crop residue burning, wood-based fuel combustion, and other NH3 emission sources were included in this inventory. Furthermore, a source apportionment tool, namely, the Integrated Source Apportionment Method (ISAM) coupled with the air quality modeling system Regional Atmospheric Modeling System and Community Multiscale Air Quality, was applied to capture the contribution of NH3 emitted from total agriculture (Tagr) in China. The aerosol mass concentration in 2015 was simulated, and results showed that the high mass concentration of NH3 exceeded 10 µg m−3 and mainly appeared in the North China Plain, Central China, the Yangtze River Delta, and the Sichuan Basin. Moreover, the annual average contribution of Tagr NH3 to PM2.5 mass burden was 14 %–22 % in China. Specific to the PM2.5 components, Tagr NH3 contributed dominantly to ammonium formation (87.6 %) but trivially to sulfate formation (2.2 %). In addition, several brute-force sensitivity tests were conducted to estimate the impact of Tagr NH3 emission reduction on PM2.5 mass burden. In contrast to the result of ISAM, even though the Tagr NH3 only provided 10.1 % contribution to nitrate under the current emission scenario, the reduction of nitrate could reach 95.8 % upon removal of the Tagr NH3 emission. This deviation occurred because the contribution of NH3 to nitrate should be small under a “rich NH3”environment and large under a “poor NH3” environment. Thus, the influence of NH3 on nitrate formation would be enhanced with the decrease in ambient NH3 mass concentration.

scholarly journals Modelling the impact of megacities on local, regional and global tropospheric ozone and the deposition of nitrogen species

2013 ◽  
Vol 13 (24) ◽  
pp. 12215-12231 ◽  
Author(s):  
Z. S. Stock ◽  
M. R. Russo ◽  
T. M. Butler ◽  
A. T. Archibald ◽  
M. G. Lawrence ◽  
...  
Keyword(s):  
Air Quality ◽  
Urban Areas ◽  
Climate Model ◽  
Surface Ozone ◽  
Global Scale ◽  
Chemical Environment ◽  
Ozone Production ◽  
The Uk ◽  
The Impact ◽  
Local Emissions

Abstract. We examine the effects of ozone precursor emissions from megacities on present-day air quality using the global chemistry–climate model UM-UKCA (UK Met Office Unified Model coupled to the UK Chemistry and Aerosols model). The sensitivity of megacity and regional ozone to local emissions, both from within the megacity and from surrounding regions, is important for determining air quality across many scales, which in turn is key for reducing human exposure to high levels of pollutants. We use two methods, perturbation and tagging, to quantify the impact of megacity emissions on global ozone. We also completely redistribute the anthropogenic emissions from megacities, to compare changes in local air quality going from centralised, densely populated megacities to decentralised, lower density urban areas. Focus is placed not only on how changes to megacity emissions affect regional and global NOx and O3, but also on changes to NOy deposition and to local chemical environments which are perturbed by the emission changes. The perturbation and tagging methods show broadly similar megacity impacts on total ozone, with the perturbation method underestimating the contribution partially because it perturbs the background chemical environment. The total redistribution of megacity emissions locally shifts the chemical environment towards more NOx-limited conditions in the megacities, which is more conducive to ozone production, and monthly mean surface ozone is found to increase up to 30% in megacities, depending on latitude and season. However, the displacement of emissions has little effect on the global annual ozone burden (0.12% change). Globally, megacity emissions are shown to contribute ~3% of total NOy deposition. The changes in O3, NOx and NOy deposition described here are useful for quantifying megacity impacts and for understanding the sensitivity of megacity regions to local emissions. The small global effects of the 100% redistribution carried out in this study suggest that the distribution of emissions on the local scale is unlikely to have large implications for chemistry–climate processes on the global scale.

scholarly journals Development of PM<sub>2.5</sub> source impact spatial fields using a hybrid source apportionment air quality model

2015 ◽  
Vol 8 (7) ◽  
pp. 2153-2165 ◽  
Author(s):  
C. E. Ivey ◽  
H. A. Holmes ◽  
Y. T. Hu ◽  
J. A. Mulholland ◽  
A. G. Russell
Keyword(s):  
Air Quality ◽  
Source Apportionment ◽  
Large Scale ◽  
Major Ions ◽  
Current Knowledge ◽  
Direct Method ◽  
Hybrid Approach ◽  
Sensitivity Analyses ◽  
Adjustment Factors ◽  
The Impact

Abstract. An integral part of air quality management is knowledge of the impact of pollutant sources on ambient concentrations of particulate matter (PM). There is also a growing desire to directly use source impact estimates in health studies; however, source impacts cannot be directly measured. Several limitations are inherent in most source apportionment methods motivating the development of a novel hybrid approach that is used to estimate source impacts by combining the capabilities of receptor models (RMs) and chemical transport models (CTMs). The hybrid CTM–RM method calculates adjustment factors to refine the CTM-estimated impact of sources at monitoring sites using pollutant species observations and the results of CTM sensitivity analyses, though it does not directly generate spatial source impact fields. The CTM used here is the Community Multiscale Air Quality (CMAQ) model, and the RM approach is based on the chemical mass balance (CMB) model. This work presents a method that utilizes kriging to spatially interpolate source-specific impact adjustment factors to generate revised CTM source impact fields from the CTM–RM method results, and is applied for January 2004 over the continental United States. The kriging step is evaluated using data withholding and by comparing results to data from alternative networks. Data withholding also provides an estimate of method uncertainty. Directly applied (hybrid, HYB) and spatially interpolated (spatial hybrid, SH) hybrid adjustment factors at withheld observation sites had a correlation coefficient of 0.89, a linear regression slope of 0.83 ± 0.02, and an intercept of 0.14 ± 0.02. Refined source contributions reflect current knowledge of PM emissions (e.g., significant differences in biomass burning impact fields). Concentrations of 19 species and total PM2.5 mass were reconstructed for withheld observation sites using HYB and SH adjustment factors. The mean concentrations of total PM2.5 at withheld observation sites were 11.7 (± 8.3), 16.3 (± 11), 8.59 (± 4.7), and 9.2 (± 5.7) μg m−3 for the observations, CTM, HYB, and SH predictions, respectively. Correlations improved for concentrations of major ions, including nitrate (CMAQ–DDM (decoupled direct method): 0.404, SH: 0.449), ammonium (CMAQ–DDM: 0.454, SH: 0.492), and sulfate (CMAQ–DDM: 0.706, SH: 0.730). Errors in simulated concentrations of metals were reduced considerably: 295 % (CMAQ–DDM) to 139 % (SH) for vanadium; and 1340 % (CMAQ–DDM) to 326 % (SH) for manganese. Errors in simulated concentrations of some metals are expected to remain given the uncertainties in source profiles. Species concentrations were reconstructed using SH results, and the error relative to observed concentrations was greatly reduced as compared to CTM-simulated concentrations. Results demonstrate that the hybrid method along with a spatial extension can be used for large-scale, spatially resolved source apportionment studies where observational data are spatially and temporally limited.

scholarly journals The representation of solar cycle signals in stratospheric ozone. Part II: Analysis of global models

2017 ◽  
Author(s):  
Amanda C. Maycock ◽  
Katja Matthes ◽  
Susann Tegtmeier ◽  
Hauke Schmidt ◽  
Rémi Thiéblemont ◽  
...  
Keyword(s):  
Solar Cycle ◽  
Solar Irradiance ◽  
Climate Models ◽  
Climate Model ◽  
Stratospheric Ozone ◽  
Temperature Response ◽  
Solar Variability ◽  
High Latitudes ◽  
Stratospheric Temperature ◽  
The Impact

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&amp;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.

scholarly journals How sensitive is the recovery of stratospheric ozone to changes in concentrations of very short-lived bromocarbons?

2014 ◽  
Vol 14 (19) ◽  
pp. 10431-10438 ◽  
Author(s):  
X. Yang ◽  
N. L. Abraham ◽  
A. T. Archibald ◽  
P. Braesicke ◽  
J. Keeble ◽  
...  
Keyword(s):  
Climate Model ◽  
Stratospheric Ozone ◽  
Montreal Protocol ◽  
Background Concentrations ◽  
Future Situation ◽  
Antarctic Ozone ◽  
The Antarctic ◽  
The Impact ◽  
Ozone Column ◽  
Policy Question

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.

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

&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;

Large Increase in Incident Shortwave Radiation due to the Ozone Hole Offset by High Climatological Albedo over Antarctica

2017 ◽  
Vol 30 (13) ◽  
pp. 4883-4890 ◽  
Author(s):  
G. Chiodo ◽  
L. M. Polvani ◽  
M. Previdi
Keyword(s):  
Surface Temperature ◽  
Ozone Depletion ◽  
Climate Model ◽  
Stratospheric Ozone ◽  
Surface Energy Budget ◽  
Ozone Hole ◽  
Radiative Heating ◽  
Shortwave Radiation ◽  
Stratospheric Ozone Depletion ◽  
Continental Scale

Despite increasing scientific scrutiny in recent years, the direct impact of the ozone hole on surface temperatures over Antarctica remains uncertain. Here, this question is explored by using the Community Earth System Model–Whole Atmosphere Community Climate Model (CESM-WACCM), contrasting two ensembles of runs with and without stratospheric ozone depletion. It is found that, during austral spring, the ozone hole leads to a surprisingly large increase in surface downwelling shortwave (SW) radiation over Antarctica of 3.8 W m−2 in clear sky and 1.8 W m−2 in all sky. However, despite this large increase in incident SW radiation, no ozone-induced surface warming is seen in the model. It is shown that the lack of a surface temperature response is due to reflection of most of the increased downward SW, resulting in an insignificant change to the net SW radiative heating. To first order, this reflection is simply due to the high climatological surface albedo of the Antarctic snow (97% in visible SW), resulting in a net zero ozone-induced surface SW forcing. In addition, it is shown that stratospheric ozone depletion has a negligible effect on longwave (LW) radiation and other components of the surface energy budget. These results suggest a minimal role for ozone depletion in forcing Antarctic surface temperature trends on a continental scale.

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