scholarly journals An exploratory performance assessment of the <i>CHIMERE</i> model (version 2017r4) for the northwestern Iberian Peninsula and the summer season

2020 ◽  
Author(s):  
Swen Brands ◽  
Guillermo Fernández-García ◽  
Marta García-Vivanco ◽  
Marcos Tesouro Montecelo ◽  
Nuria Gallego Fernández ◽  
...  

Abstract. Here, the capability of the chemical weather forecasting model CHIMERE (version 2017r4) to reproduce surface ozone, particulate matter and nitrogen dioxide concentrations in complex terrain is investigated for the period from June 21 to August 21, 2018. The study area is the northwestern Iberian Peninsula, where both coastal and mountain climates can be found in direct vicinity and a large fraction of the land area is covered by forests. Driven by lateral boundary conditions from the ECMWF Composition Integrated Forecast System, anthropogenic emissions from two commonly used top-down inventories and meteorological data from the Weather Research and Forecasting Model, CHIMERE's performance with respect to observations is tested with a range of sensitivity experiments. We assess the effects of 1) an increase in horizontal resolution, 2) an increase in vertical resolution, 3) the use of distinct model chemistries and 4) the use of distinct anthropogenic emissions inventories, downscaling techniques and landuse databases. In comparsion with the older HTAP emission inventory downscaled with basic options, the updated and sophistically downscaled EMEP inventory only leads to partial model improvements and so does the computationally costly horizontal resolution increase. Model performance changes caused by the choice of distinct chemical mechanisms are not systematic either and rather depend on the considered anthropgenic emission configuration and pollutant. Albeit the results are thus heterogeneous in general terms, the model's response to a vertical resolution increase confined to the lower to middle troposphere is homogeneous in the sense of improving virtually all verification aspects. We conclude that, as long as the aforementioned top-down emission inventories are used, it is generally not necessary to use a horizontal model mesh much finer than the native grid of the inventories. A relatively coarse horizontal mesh combined with 20 model layers between 999 and 500 hPa is sufficient to yield balanced results. The chemical mechanism should be chosen as a function of the intended application.

2020 ◽  
Vol 13 (9) ◽  
pp. 3947-3973
Author(s):  
Swen Brands ◽  
Guillermo Fernández-García ◽  
Marta García Vivanco ◽  
Marcos Tesouro Montecelo ◽  
Nuria Gallego Fernández ◽  
...  

Abstract. Here, the capability of the chemical weather forecasting model CHIMERE (version 2017r4) to reproduce surface ozone, particulate matter and nitrogen dioxide concentrations in complex terrain is investigated for the period from 21 June to 21 August 2018. The study area is the northwestern Iberian Peninsula, where both coastal and mountain climates can be found in direct vicinity and a large fraction of the land area is covered by forests. Driven by lateral boundary conditions from the European Centre for Medium-Range Weather Forecasts (ECMWF) Composition Integrated Forecast System, anthropogenic emissions from two commonly used top-down inventories and meteorological data from the Weather Research and Forecasting Model, CHIMERE's performance with respect to observations is tested with a range of sensitivity experiments. We assess the effects of (1) an increase in horizontal resolution, (2) an increase in vertical resolution, (3) the use of distinct model chemistries, and (4) the use of distinct anthropogenic emissions inventories, downscaling techniques and land use databases. In comparison with the older HTAP emission inventory downscaled with basic options, the updated and sophistically downscaled EMEP inventory only leads to partial model improvements, and so does the computationally costly horizontal resolution increase. Model performance changes caused by the choice of distinct chemical mechanisms are not systematic either and rather depend on the considered anthropogenic emission configuration and pollutant. Although the results are thus heterogeneous in general terms, the model's response to a vertical resolution increase confined to the lower to middle troposphere is homogeneous in the sense of improving virtually all verification aspects. For our study region and the two aforementioned top-down emission inventories, we conclude that it is not necessary to run CHIMERE on a horizontal mesh much finer than the native grid of these inventories. A relatively coarse horizontal mesh combined with 20 model layers between 999 and 500 hPa is sufficient to yield balanced results. The chemical mechanism should be chosen as a function of the intended application.


2019 ◽  
Author(s):  
Swen Brands ◽  
Guillermo Fernández-García ◽  
Marcos Tesouro Montecelo ◽  
Nuria Gallego Fernández ◽  
Anthony David Saunders Estévez ◽  
...  

Abstract. Here, the capability of the chemical weather forecasting model CHIMERE (version 2017r4) to reproduce summertime surface ozone, particulate matter and nitrogen dioxide concentrations in complex terrain is investigated. The study area is the northwestern Iberian Peninsula, where both coastal and mountain climates can be found in direct vicinity and a large fraction of the land area is covered by forests. Fed by lateral boundary conditions from the ECMWF Composition Integrated Forecast System, meteorological data from the Weather Research and Forecasting Model (WRF) and the HTAP v2.2 emission inventory, CHIMERE's performance compared to observations is tested with a range of sensitivity experiments, exploring the role of horizontal and vertical resolution and the effects of applying distinct chemistry mechanisms. Using a high horizontal and vertical resolution yields the most balanced verification results. If both the daily maximum and minimum values are important for the given application, then the full Melchior mechanism should be used. If, however, the daily maxima are considered more important than the minima, SAPRC should be used instead. In any case, model performance for nitrogen dioxide is clearly not satisfactory for our study region, probably indicating deficiencies in the emission inventory.


2018 ◽  
Vol 11 (7) ◽  
pp. 2825-2840 ◽  
Author(s):  
Tim Butler ◽  
Aurelia Lupascu ◽  
Jane Coates ◽  
Shuai Zhu

Abstract. A system for source attribution of tropospheric ozone produced from both NOx and volatile organic compound (VOC) precursors is described, along with its implementation in the Community Earth System Model (CESM) version 1.2.2 using CAM4. The user can specify an arbitrary number of tag identities for each NOx or VOC species in the model, and the tagging system rewrites the model chemical mechanism and source code to incorporate tagged tracers and reactions representing these tagged species, as well as ozone produced in the stratosphere. If the user supplies emission files for the corresponding tagged tracers, the model will produce tagged ozone tracers which represent the contribution of each of the tag identities to the modelled total tropospheric ozone. Our tagged tracers preserve Ox. The size of the tagged chemical mechanism scales linearly with the number of specified tag identities. Separate simulations are required for NOx and VOC tagging, which avoids the sharing of tag identities between NOx and VOC species. Results are presented and evaluated for both NOx and VOC source attribution. We show that northern hemispheric surface ozone is dominated year-round by anthropogenic emissions of NOx, but that the mix of corresponding VOC precursors changes over the course of the year; anthropogenic VOC emissions contribute significantly to surface ozone in winter–spring, while biogenic VOCs are more important in summer. The system described here can provide important diagnostic information about modelled ozone production, and could be used to construct source–receptor relationships for tropospheric ozone.


2015 ◽  
Vol 15 (13) ◽  
pp. 7703-7723 ◽  
Author(s):  
K. Markakis ◽  
M. Valari ◽  
O. Perrussel ◽  
O. Sanchez ◽  
C. Honore

Abstract. While previous research helped to identify and prioritize the sources of error in air-quality modeling due to anthropogenic emissions and spatial scale effects, our knowledge is limited on how these uncertainties affect climate-forced air-quality assessments. Using as reference a 10-year model simulation over the greater Paris (France) area at 4 km resolution and anthropogenic emissions from a 1 km resolution bottom-up inventory, through several tests we estimate the sensitivity of modeled ozone and PM2.5 concentrations to different potentially influential factors with a particular interest over the urban areas. These factors include the model horizontal and vertical resolution, the meteorological input from a climate model and its resolution, the use of a top-down emission inventory, the resolution of the emissions input and the post-processing coefficients used to derive the temporal, vertical and chemical split of emissions. We show that urban ozone displays moderate sensitivity to the resolution of emissions (~ 8 %), the post-processing method (6.5 %) and the horizontal resolution of the air-quality model (~ 5 %), while annual PM2.5 levels are particularly sensitive to changes in their primary emissions (~ 32 %) and the resolution of the emission inventory (~ 24 %). The air-quality model horizontal and vertical resolution have little effect on model predictions for the specific study domain. In the case of modeled ozone concentrations, the implementation of refined input data results in a consistent decrease (from 2.5 up to 8.3 %), mainly due to inhibition of the titration rate by nitrogen oxides. Such consistency is not observed for PM2.5. In contrast this consistency is not observed for PM2.5. In addition we use the results of these sensitivities to explain and quantify the discrepancy between a coarse (~ 50 km) and a fine (4 km) resolution simulation over the urban area. We show that the ozone bias of the coarse run (+9 ppb) is reduced by ~ 40 % by adopting a higher resolution emission inventory, by 25 % by using a post-processing technique based on the local inventory (same improvement is obtained by increasing model horizontal resolution) and by 10 % by adopting the annual emission totals of the local inventory. The bias of PM2.5 concentrations follows a more complex pattern, with the positive values associated with the coarse run (+3.6 μg m−3), increasing or decreasing depending on the type of the refinement. We conclude that in the case of fine particles, the coarse simulation cannot selectively incorporate local-scale features in order to reduce its error.


2018 ◽  
Author(s):  
Tim Butler ◽  
Aurelia Lupascu ◽  
Jane Coates ◽  
Shuai Zhu

Abstract. A system for source attribution of tropospheric ozone produced from both NOx and VOC precursors is described, along with its implementation in the Community Earth System Model (CESM) version 1.2.2 using CAM4. The user can specify an arbitrary number of tag identities for each NOx or VOC species in the model, and the tagging system rewrites the model chemical mechanism and source code to incorporate tagged tracers and reactions representing these tagged species, as well as ozone produced in the stratosphere. If the user supplies emission files for the corresponding tagged tracers, the model will produce tagged ozone tracers which represent the contribution of each of the tag identities to the modelled total tropospheric ozone. Our tagged tracers preserve Ox. The size of the tagged chemical mechanism scales linearly with the number of specified tag identities. Separate simulations are required for NOx and VOC tagging, which avoids the sharing of tag identities between NOx and VOC species. Results are presented and evaluated for both NOx and VOC source attribution. We show that northern hemispheric surface ozone is dominated year-round by anthropogenic emissions of NOx, but that the mix of corresponding VOC precursors changes over the course of the year; anthropogenic VOC emissions contribute significantly to surface ozone in winter-spring, while biogenic VOC are more important in summer. The system described here can provide important diagnostic information about modelled ozone production, and could be used to construct source-receptor relationships for tropospheric ozone.


2013 ◽  
Vol 13 (4) ◽  
pp. 2091-2113 ◽  
Author(s):  
J. E. Shilling ◽  
R. A. Zaveri ◽  
J. D. Fast ◽  
L. Kleinman ◽  
M. L. Alexander ◽  
...  

Abstract. The CARES campaign was conducted during June, 2010 in the vicinity of Sacramento, California to study aerosol formation and aging in a region where anthropogenic and biogenic emissions regularly mix. Here, we describe measurements from an Aerodyne High Resolution Aerosol Mass Spectrometer (AMS), an Ionicon Proton Transfer Reaction Mass Spectrometer (PTR-MS), and trace gas detectors (CO, NO, NOx) deployed on the G-1 research aircraft to investigate ambient gas- and particle-phase chemical composition. AMS measurements showed that the particle phase is dominated by organic aerosol (OA) (85% on average) with smaller concentrations of sulfate (5%), nitrate (6%) and ammonium (3%) observed. PTR-MS data showed that isoprene dominated the biogenic volatile organic compound concentrations (BVOCs), with monoterpene concentrations generally below the detection limit. Using two different metrics, median OA concentrations and the slope of plots of OA vs. CO concentrations (i.e., ΔOA/ΔCO), we contrast organic aerosol evolution on flight days with different prevailing meteorological conditions to elucidate the role of anthropogenic and biogenic emissions on OA formation. Airmasses influenced predominantly by biogenic emissions had median OA concentrations of 2.2 μg m−3 and near zero ΔOA/ΔCO. Those influenced predominantly by anthropogenic emissions had median OA concentrations of 4.7 μg m−3 and ΔOA/ΔCO ratios of 35–44 μg m−3 ppmv. But, when biogenic and anthropogenic emissions mixed, OA levels were enhanced, with median OA concentrations of 11.4 μg m−3 and ΔOA/ΔCO ratios of 77–157 μg m−3 ppmv. Taken together, our observations show that production of OA was enhanced when anthropogenic emissions from Sacramento mixed with isoprene-rich air from the foothills. After considering several anthropogenic/biogenic interaction mechanisms, we conclude that NOx concentrations play a strong role in enhancing SOA formation from isoprene, though the chemical mechanism for the enhancement remains unclear. If these observations are found to be robust in other seasons and in areas outside of Sacramento, regional and global aerosol modules will need to incorporate more complex representations of NOx-dependent SOA mechanisms and yields into their algorithms. Ultimately, accurately predicting OA mass concentrations and their effect on radiation balance will require a mechanistically-based treatment of the interactions of biogenic and anthropogenic emissions.


2021 ◽  
Author(s):  
Hella Garny ◽  
Simone Dietmüller ◽  
Roland Eichinger ◽  
Aman Gupta ◽  
Marianna Linz

&lt;p&gt;The stratospheric transport circulation, or Brewer-Dobson Circulation (BDC), is often conceptually seperated into advection along the residual circulation and two-way mixing. In particular the latter part has recently been found to exert a strong influence on inter-model differences of mean age of Air (AoA), a common measure of the BDC. However, the precise reason for model differences in two-way mixing remains unknown, as many model&lt;br&gt;components in multi-model projects differ. One component that likely plays an important role is model resolution, both vertically and horizontally. To analyse this aspect, we carried out a set of simulations with identical and constant year 2000 climate forcing varying the spectral horizontal&lt;br&gt;resolution (T31,T42,T63,T85) and the number of vertical levels (L31,L47,L90). We find that increasing the vertical resolution leads to an increase in mean AoA. Most of this change can be attributed to aging by mixing. The mixing efficiency, defined as the ratio of isentropic mixing strength and the diabatic circulation, shows the same dependency on vertical resolution. While horizontal resolution changes do not systematically change mean AoA, we do&lt;br&gt;find a systematic decrease in the mixing efficiency with increasing horizontal resolution. Non-systematic changes in the residual circulation partly compensate the mixing efficiency changes, leading to the non-systematic mean AoA changes. The mixing efficiency changes with vertical and horizontal resolution are consistent with expectations on the effects of numerical dispersion on mean AoA. To further investigate the most relevant regions of mixing differences, we analyse height-resolved mixing efficiency differences. Overall, this work will help to shed light on the underlying reasons for the large biases of climate models in simulating stratospheric transport.&lt;/p&gt;


2021 ◽  
Author(s):  
Carla Gama ◽  
Alexandra Monteiro ◽  
Myriam Lopes ◽  
Ana Isabel Miranda

&lt;p&gt;Tropospheric ozone (O&lt;sub&gt;3&lt;/sub&gt;) is a critical pollutant over the Mediterranean countries, including Portugal, due to systematic exceedances to the thresholds for the protection of human health. Due to the location of Portugal, on the Atlantic coast at the south-west point of Europe, the observed O&lt;sub&gt;3&lt;/sub&gt; concentrations are very much influenced not only by local and regional production but also by northern mid-latitudes background concentrations. Ozone trends in the Iberian Peninsula were previously analysed by Monteiro et al. (2012), based on 10-years of O&lt;sub&gt;3&lt;/sub&gt; observations. Nevertheless, only two of the eleven background monitoring stations analysed in that study are located in Portugal and these two stations are located in Porto and Lisbon urban areas. Although during pollution events O&lt;sub&gt;3&lt;/sub&gt; levels in urban areas may be high enough to affect human health, the highest concentrations are found in rural locations downwind from the urban and industrialized areas, rather than in cities. This happens because close to the sources (e.g., in urban areas) freshly emitted NO locally scavenges O&lt;sub&gt;3&lt;/sub&gt;. A long-term study of the spatial and temporal variability and trends of the ozone concentrations over Portugal is missing, aiming to answer the following questions:&lt;/p&gt;&lt;p&gt;-&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160; What is the temporal variability of ozone concentrations?&lt;/p&gt;&lt;p&gt;-&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160; Which trends can we find in observations?&lt;/p&gt;&lt;p&gt;-&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160; How were the ozone spring maxima concentrations affected by the COVID-19 lockdown during spring 2020?&lt;/p&gt;&lt;p&gt;In this presentation, these questions will be answered based on the statistical analysis of O&lt;sub&gt;3&lt;/sub&gt; concentrations recorded within the national air quality monitoring network between 2005 and 2020 (16 years). The variability of the surface ozone concentrations over Portugal, on the timescales from diurnal to annual, will be presented and discussed, taking into account the physical and chemical processes that control that variability. Using the TheilSen function from the OpenAir package for R (Carslaw and Ropkins 2012), which quantifies monotonic trends and calculates the associated p-value through bootstrap simulations, O&lt;sub&gt;3&lt;/sub&gt; concentration long-term trends will be estimated for the different regions and environments (e.g., rural, urban).&amp;#160; Moreover, taking advantage of the unique situation provided by the COVID-19 lockdown during spring 2020, when the government imposed mandatory confinement and citizens movement restriction, leading to a reduction in traffic-related atmospheric emissions, the role of these emissions on ozone levels during the spring period will be studied and presented.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;Carslaw and Ropkins, 2012. Openair&amp;#8212;an R package for air quality data analysis. Environ. Model. Softw. 27-28,52-61. https://doi.org/10.1016/j.envsoft.2011.09.008&lt;/p&gt;&lt;p&gt;Monteiro et al., 2012. Trends in ozone concentrations in the Iberian Peninsula by quantile regression and clustering. Atmos. Environ. 56, 184-193. https://doi.org/10.1016/j.atmosenv.2012.03.069&lt;/p&gt;


2016 ◽  
Vol 16 (18) ◽  
pp. 11601-11615 ◽  
Author(s):  
Jane Coates ◽  
Kathleen A. Mar ◽  
Narendra Ojha ◽  
Tim M. Butler

Abstract. Surface ozone is a secondary air pollutant produced during the atmospheric photochemical degradation of emitted volatile organic compounds (VOCs) in the presence of sunlight and nitrogen oxides (NOx). Temperature directly influences ozone production through speeding up the rates of chemical reactions and increasing the emissions of VOCs, such as isoprene, from vegetation. In this study, we used an idealised box model with different chemical mechanisms (Master Chemical Mechanism, MCMv3.2; Common Representative Intermediates, CRIv2; Model for OZone and Related Chemical Tracers, MOZART-4; Regional Acid Deposition Model, RADM2; Carbon Bond Mechanism, CB05) to examine the non-linear relationship between ozone, NOx and temperature, and we compared this to previous observational studies. Under high-NOx conditions, an increase in ozone from 20 to 40 °C of up to 20 ppbv was due to faster reaction rates, while increased isoprene emissions added up to a further 11 ppbv of ozone. The largest inter-mechanism differences were obtained at high temperatures and high-NOx emissions. CB05 and RADM2 simulated more NOx-sensitive chemistry than MCMv3.2, CRIv2 and MOZART-4, which could lead to different mitigation strategies being proposed depending on the chemical mechanism. The increased oxidation rate of emitted VOC with temperature controlled the rate of Ox production; the net influence of peroxy nitrates increased net Ox production per molecule of emitted VOC oxidised. The rate of increase in ozone mixing ratios with temperature from our box model simulations was about half the rate of increase in ozone with temperature observed over central Europe or simulated by a regional chemistry transport model. Modifying the box model set-up to approximate stagnant meteorological conditions increased the rate of increase of ozone with temperature as the accumulation of oxidants enhanced ozone production through the increased production of peroxy radicals from the secondary degradation of emitted VOCs. The box model simulations approximating stagnant conditions and the maximal ozone production chemical regime reproduced the 2 ppbv increase in ozone per degree Celsius from the observational and regional model data over central Europe. The simulated ozone–temperature relationship was more sensitive to mixing than the choice of chemical mechanism. Our analysis suggests that reductions in NOx emissions would be required to offset the additional ozone production due to an increase in temperature in the future.


2017 ◽  
Vol 145 (6) ◽  
pp. 2385-2404 ◽  
Author(s):  
Alice K. DuVivier ◽  
John J. Cassano ◽  
Steven Greco ◽  
G. David Emmitt

Abstract Mesoscale barrier jets in the Denmark Strait are common in winter months and have the capability to influence open ocean convection. This paper presents the first detailed observational study of a summertime (21 May 2015) barrier wind event in the Denmark Strait using dropsondes and observations from an airborne Doppler wind lidar (DWL). The DWL profiles agree well with dropsonde observations and show a vertically narrow (~250–400 m) barrier jet of 23–28 m s−1 near the Greenland coast that broadens (~300–1000 m) and strengthens farther off coast. In addition, otherwise identical regional high-resolution Weather Research and Forecasting (WRF) Model simulations of the event are analyzed at four horizontal grid spacings (5, 10, 25, and 50 km), two vertical resolutions (40 and 60 levels), and two planetary boundary layer (PBL) parameterizations [Mellor–Yamada–Nakanishi–Niino, version 2.5 (MYNN2.5) and University of Washington (UW)] to determine what model configurations best simulate the observed jet structure. Comparison of the WRF simulations with wind observations from satellites, dropsondes, and the airborne DWL scans indicate that the combination of both high horizontal resolution (5 km) and vertical resolution (60 levels) best captures observed barrier jet structure and speeds as well as the observed cloud field, including some convective clouds. Both WRF PBL schemes produced reasonable barrier jets with the UW scheme slightly outperforming the MYNN2.5 scheme. However, further investigation at high horizontal and vertical resolution is needed to determine the impact of the WRF PBL scheme on surface energy budget terms, particularly in the high-latitude maritime environment around Greenland.


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