scholarly journals Modeling wet deposition and concentration of inorganics over Northeast Asia with MRI-PM/c

2012 ◽  
Vol 5 (6) ◽  
pp. 1363-1375 ◽  
Author(s):  
M. Kajino ◽  
M. Deushi ◽  
T. Maki ◽  
N. Oshima ◽  
Y. Inomata ◽  
...  

Abstract. We conducted a regional-scale simulation over Northeast Asia for the year 2006 using an aerosol chemical transport model, with time-varying lateral and upper boundary concentrations of gaseous species predicted by a global stratospheric and tropospheric chemistry-climate model. The present one-way nested global-through-regional-scale model is named the Meteorological Research Institute–Passive-tracers Model system for atmospheric Chemistry (MRI-PM/c). We evaluated the model's performance with respect to the major anthropogenic and natural inorganic components, SO42−, NH4+, NO3−, Na+ and Ca2+ in the air, rain and snow measured at the Acid Deposition Monitoring Network in East Asia (EANET) stations. Statistical analysis showed that approximately 40–50 % and 70–80 % of simulated concentration and wet deposition of SO42−, NH4+, NO3−and Ca2+ are within factors of 2 and 5 of the observations, respectively. The prediction of the sea-salt originated component Na+ was not successful at near-coastal stations (where the distance from the coast ranged from 150 to 700 m), because the model grid resolution (Δx=60 km) is too coarse to resolve it. The simulated Na+ in precipitation was significantly underestimated by up to a factor of 30.

2012 ◽  
Vol 5 (2) ◽  
pp. 1341-1379
Author(s):  
M. Kajino ◽  
M. Deushi ◽  
T. Maki ◽  
N. Oshima ◽  
Y. Inomata ◽  
...  

Abstract. We conducted a regional-scale simulation (with grid spacing = 60 km) over Northeast Asia for the entire year of 2006 by using an aerosol chemical transport model, the lateral and upper boundary concentrations of which we predicted with a global stratospheric and tropospheric chemistry-climate model, with a horizontal resolution of T42 (grid spacing ~300 km) and a time resolution of 1 h. The present one-way nested global-through-regional-scale model is called the Meteorological Research Institute – Passive-tracers Model system for atmospheric Chemistry (MRI-PM/c). We evaluated the model performance with respect to the major inorganic components in rain and snow measured by stations of the Acid Deposition Monitoring Network in East Asia (EANET). Through statistical analysis, we show that the model successfully reproduced the regional-scale processes of emission, transport, transformation, and wet deposition of major inorganic species derived from anthropogenic and natural sources, including SO42−, NH4+, NO3−, Na+ and Ca2+. Interestingly, the only exception was Na+ in precipitation at near-coastal stations (where the distance from the coast was from 150 to 700 m), concentrations of which were significantly underestimated by the model, by up to a factor of 30. This result suggested that the contribution of short-lived, super-large sea salt droplets (SLSD; D > 10–100 μm) was substantial in precipitation samples at stations near the coast of Japan; thus samples were horizontally representative only within the traveling distances of SLSD (from 1 to 10 km). Nevertheless, the calculated effect of SLSD on precipitation pH was very low, a change of about +0.014 on average, even if the ratio of SLSD to all sea salt in precipitation was assumed to be 90%.


2015 ◽  
Vol 15 (2) ◽  
pp. 829-843 ◽  
Author(s):  
T. Sakazaki ◽  
M. Shiotani ◽  
M. Suzuki ◽  
D. Kinnison ◽  
J. M. Zawodny ◽  
...  

Abstract. This paper contains a comprehensive investigation of the sunset–sunrise difference (SSD, i.e., the sunset-minus-sunrise value) of the ozone mixing ratio in the latitude range of 10° S–10° N. SSD values were determined from solar occultation measurements based on data obtained from the Stratospheric Aerosol and Gas Experiment (SAGE) II, the Halogen Occultation Experiment (HALOE), and the Atmospheric Chemistry Experiment–Fourier transform spectrometer (ACE–FTS). The SSD was negative at altitudes of 20–30 km (−0.1 ppmv at 25 km) and positive at 30–50 km (+0.2 ppmv at 40–45 km) for HALOE and ACE–FTS data. SAGE II data also showed a qualitatively similar result, although the SSD in the upper stratosphere was 2 times larger than those derived from the other data sets. On the basis of an analysis of data from the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) and a nudged chemical transport model (the specified dynamics version of the Whole Atmosphere Community Climate Model: SD–WACCM), we conclude that the SSD can be explained by diurnal variations in the ozone concentration, particularly those caused by vertical transport by the atmospheric tidal winds. All data sets showed significant seasonal variations in the SSD; the SSD in the upper stratosphere is greatest from December through February, while that in the lower stratosphere reaches a maximum twice: during the periods March–April and September–October. Based on an analysis of SD–WACCM results, we found that these seasonal variations follow those associated with the tidal vertical winds.


2014 ◽  
Vol 14 (11) ◽  
pp. 16043-16083
Author(s):  
T. Sakazaki ◽  
M. Shiotani ◽  
M. Suzuki ◽  
D. Kinnison ◽  
J. M. Zawodny ◽  
...  

Abstract. This paper contains a comprehensive investigation of the sunset–sunrise difference (SSD; i.e., the sunset-minus-sunrise value) of the ozone mixing ratio in the latitude range of 10° S–10° N. SSD values were determined from solar occultation measurements based on data obtained from the Stratospheric Aerosol and Gas Experiment (SAGE) II, the Halogen Occultation Experiment (HALOE), and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). The SSD was negative at altitudes of 20–30 km (–0.1 ppmv at 25 km) and positive at 30–50 km (+0.2 ppmv at 40–45 km) for HALOE and ACE–FTS data. SAGE II data also showed a qualitatively similar result, although the SSD in the upper stratosphere was two times larger than those derived from the other datasets. On the basis of an analysis of data from the Superconducting Submillimeter Limb Emission Sounder (SMILES), and a nudged chemical-transport model (the Specified Dynamics version of the Whole Atmosphere Community Climate Model: SD–WACCM), we conclude that the SSD can be explained by diurnal variations in the ozone concentration, particularly those caused by vertical transport by the atmospheric tidal winds. All datasets showed significant seasonal variations in the SSD; the SSD in the upper stratosphere is greatest from December through February, while that in the lower stratosphere reaches a maximum twice: during the periods March–April and September–October. Based on an analysis of SD–WACCM results, we found that these seasonal variations follow those associated with the tidal vertical winds.


2020 ◽  
Author(s):  
Maxime Prignon ◽  
Peter F. Bernath ◽  
Simon Chabrillat ◽  
Martyn P. Chipperfield ◽  
Sandip S. Dhomse ◽  
...  

<p>Man-made halogenated compounds emitted from the Earth’s surface ultimately reach the stratosphere where they undergo photolysis, leading to three main fluorine reservoirs: hydrogen fluoride (HF), carbonyl fluoride (COF<sub>2</sub>) and carbonyl chloride fluoride (COClF). This process is directly influenced by the strength of the mean meridional circulation of the stratosphere, the Brewer-Dobson Circulation (BDC). The BDC is projected to speed-up with the greenhouse gases induced global warming. However, studies have highlighted a multiyear variability in the strength of the BDC resulting in hemispheric asymmetries in observed and modelled trends of age of air and long-lived tracers.</p><p>Total inorganic fluorine (F<sub>y</sub>, the fluorine weighted sum of HF, COF<sub>2</sub> and COClF) is used here as a tracer of the stratospheric circulation changes. We perform an analysis and interpretation of Fourier transform infrared (FTIR) multidecadal time-series of HF and COF<sub>2</sub> from the Jungfraujoch (Switzerland, 46.55°N) and Lauder (New-Zealand, 45.03°S) stations and from the space-borne Atmospheric Chemistry Experiment - Fourier Transform Spectrometer (ACE-FTS). Indeed, the summation of HF and COF<sub>2</sub> is a very good proxy of F<sub>y </sub>as we determine, from ACE-FTS and the chemical-transport model (CTM) TOMCAT, that COClF is only accounting for less than 5% of the total F<sub>y </sub>budget.</p><p>The kinematic CTM BASCOE (Belgian assimilation system for chemical observations) is used here to assess the representation of the investigated circulation changes in four state-of-the-art meteorological reanalyses, i.e., ERA-Interim, JRA-55, MERRA and MERRA-2. We also investigate if WACCM4 (Whole Atmosphere Community Climate Model version 4) is able to reproduce these changes through a free-running simulation.</p><p>The ground-based and satellite FTIR time-series of COF<sub>2</sub> show contrasting results over their common time period (2004-2019), with a positive total column trend above the Jungfraujoch, and a non-significant (ground-based) or decreasing trend (ACE-FTS) above Lauder. We find large discrepancies between the BASCOE-CTM simulations, with MERRA-2 inducing overly large simulated F<sub>y</sub> total columns which could confirm the weaker tropical upwelling highlighted in previous age of air studies.</p>


2019 ◽  
Author(s):  
Lya Lugon ◽  
Karine Sartelet ◽  
Youngseob Kim ◽  
Jérémy Vigneron ◽  
Olivier Chrétien

Abstract. Regional-scale chemistry-transport models have coarse spatial resolution, and thus can only simulate background concentrations. They fail to simulate the high concentrations observed close to roads and in streets, i.e. where a large part of the urban population lives. Local-scale models may be used to simulate concentrations in streets. They often assume that background concentrations are constant and/or use simplified chemistry. Recently developed, the multi-scale model Street-in-Grid (SinG) estimates gaseous pollutant concentrations simultaneously at local and regional scales, coupling them dynamically. This coupling combines the regional-scale chemistry-transport model Polair3D and the street network model MUNICH (Model of Urban Network of Intersecting Canyons and Highway). MUNICH models explicitly street canyons and intersections, and it is coupled to the first vertical level of the chemical-transport model, enabling the transfer of pollutant mass between the street canyon roof and the atmosphere. The original versions of SinG and MUNICH adopt a stationary hypothesis to estimate pollutant concentrations in streets. Although the computation of NOx concentration is numerically stable with the stationary approach, the partitioning between NO and NO2 is highly dependent on the time step of coupling between transport and chemistry processes. In this study, a new non-stationary approach is presented with a fine coupling between transport and chemistry, leading to numerically stable partitioning between NO and NO2. Simulations of NO, NO2 and NOx concentrations over Paris city with SinG, MUNICH and Polair3D are compared to observations at traffic and urban stations to estimate the added value of multi-scale modeling with a dynamical coupling between the regional and local scales. As expected, the regional chemical-transport model underestimates NO and NO2 concentrations in the streets. However, there is a good agreement between the measurements and the concentrations simulated with MUNICH and SinG. The dynamic coupling between the local and regional scales tends to be important for streets with an intermediate aspect ratio and with high traffic emissions.


2016 ◽  
Vol 189 ◽  
pp. 105-120 ◽  
Author(s):  
Rachel E. Dunmore ◽  
Lisa K. Whalley ◽  
Tomás Sherwen ◽  
Mathew J. Evans ◽  
Dwayne E. Heard ◽  
...  

There is growing global consumption of non-fossil fuels such as ethanol made from renewable biomass. Previous studies have shown that one of the main air quality disadvantages of using ethanol blended fuels is a significant increase in the production of acetaldehyde, an unregulated and toxic pollutant. Most studies on the impacts of ethanol blended gasoline have been carried out in the US and Brazil, with much less focus on the UK and Europe. We report time resolved measurements of ethanol in London during the winter and summer of 2012. In both seasons the mean mixing ratio of ethanol was around 5 ppb, with maximum values over 30 ppb, making ethanol currently the most abundant VOC in London air. We identify a road transport related source, with ‘rush-hour’ peaks observed. Ethanol is strongly correlated with other road transport-related emissions, such as small aromatics and light alkanes, and has no relationship to summer biogenic emissions. To determine the impact of road transport-related ethanol emission on secondary species (i.e. acetaldehyde and ozone), we use both a chemically detailed box model (incorporating the Master Chemical Mechanism, MCM) and a global and nested regional scale chemical transport model (GEOS-Chem), on various processing time scales. Using the MCM model, only 16% of the modelled acetaldehyde was formed from ethanol oxidation. However, the model significantly underpredicts the total levels of acetaldehyde, indicating a missing primary emission source, that appears to be traffic-related. Further support for a primary emission source comes from the regional scale model simulations, where the observed concentrations of ethanol and acetaldehyde can only be reconciled with the inclusion of large primary emissions. Although only constrained by one set of observations, the regional modelling suggests a European ethanol source similar in magnitude to that of ethane (∼60 Gg per year) and greater than that of acetaldehyde (∼10 Gg per year). The increased concentrations of ethanol and acetaldehyde from primary emissions impacts both radical and NOx cycling over Europe, resulting in significant regional impacts on NOy speciation and O3 concentrations, with potential changes to human exposure to air pollutants.


2014 ◽  
Vol 7 (6) ◽  
pp. 7733-7803 ◽  
Author(s):  
J. Flemming ◽  
V. Huijnen ◽  
J. Arteta ◽  
P. Bechtold ◽  
A. Beljaars ◽  
...  

Abstract. A representation of atmospheric chemistry has been included in the Integrated Forecasting System (IFS) of the European Centre for Medium-range Weather Forecasts (ECMWF). The new chemistry modules complement the aerosol modules of the IFS for atmospheric composition, which is named C-IFS. C-IFS for chemistry supersedes a coupled system, in which the Chemical Transport Model (CTM) Model for OZone and Related chemical Tracers 3 was two-way coupled to the IFS (IFS-MOZART). This paper contains a description of the new on-line implementation, an evaluation with observations and a comparison of the performance of C-IFS with MOZART and with a re-analysis of atmospheric composition produced by IFS-MOZART within the Monitoring Atmospheric Composition and Climate (MACC) project. The chemical mechanism of C-IFS is an extended version of the Carbon Bond 2005 (CB05) chemical mechanism as implemented in the CTM Transport Model 5 (TM5). CB05 describes tropospheric chemistry with 54 species and 126 reactions. Wet deposition and lightning nitrogen monoxide (NO) emissions are modelled in C-IFS using the detailed input of the IFS physics package. A one-year simulation by C-IFS, MOZART and the MACC re-analysis is evaluated against ozonesondes, carbon monoxide (CO) aircraft profiles, European surface observations of ozone (O3), CO, sulphur dioxide (SO2) and nitrogen dioxide (NO2) as well as satellite retrievals of CO, tropospheric NO2 and formaldehyde. Anthropogenic emissions from the MACC/CityZen (MACCity) inventory and biomass burning emissions from the Global Fire Assimilation System (GFAS) data set were used in the simulations by both C-IFS and MOZART. C-IFS (CB05) showed an improved performance with respect to MOZART for CO, upper tropospheric O3, winter time SO2 and was of a similar accuracy for other evaluated species. C-IFS (CB05) is about ten times more computationally efficient than IFS-MOZART.


2015 ◽  
Vol 8 (4) ◽  
pp. 975-1003 ◽  
Author(s):  
J. Flemming ◽  
V. Huijnen ◽  
J. Arteta ◽  
P. Bechtold ◽  
A. Beljaars ◽  
...  

Abstract. A representation of atmospheric chemistry has been included in the Integrated Forecasting System (IFS) of the European Centre for Medium-Range Weather Forecasts (ECMWF). The new chemistry modules complement the aerosol modules of the IFS for atmospheric composition, which is named C-IFS. C-IFS for chemistry supersedes a coupled system in which chemical transport model (CTM) Model for OZone and Related chemical Tracers 3 was two-way coupled to the IFS (IFS-MOZART). This paper contains a description of the new on-line implementation, an evaluation with observations and a comparison of the performance of C-IFS with MOZART and with a re-analysis of atmospheric composition produced by IFS-MOZART within the Monitoring Atmospheric Composition and Climate (MACC) project. The chemical mechanism of C-IFS is an extended version of the Carbon Bond 2005 (CB05) chemical mechanism as implemented in CTM Transport Model 5 (TM5). CB05 describes tropospheric chemistry with 54 species and 126 reactions. Wet deposition and lightning nitrogen monoxide (NO) emissions are modelled in C-IFS using the detailed input of the IFS physics package. A 1 year simulation by C-IFS, MOZART and the MACC re-analysis is evaluated against ozonesondes, carbon monoxide (CO) aircraft profiles, European surface observations of ozone (O3), CO, sulfur dioxide (SO2) and nitrogen dioxide (NO2) as well as satellite retrievals of CO, tropospheric NO2 and formaldehyde. Anthropogenic emissions from the MACC/CityZen (MACCity) inventory and biomass burning emissions from the Global Fire Assimilation System (GFAS) data set were used in the simulations by both C-IFS and MOZART. C-IFS (CB05) showed an improved performance with respect to MOZART for CO, upper tropospheric O3, and wintertime SO2, and was of a similar accuracy for other evaluated species. C-IFS (CB05) is about 10 times more computationally efficient than IFS-MOZART.


2021 ◽  
Author(s):  
E.Yu. Mordvin ◽  
A.A. Lagutin ◽  
N.V. Volkov

The paper considers the behavior of total methane content in the atmosphere of Western Siberia obtained using the global chemical transport model MOZART-4 (Model for OZone And Related chemical Tracers, version 4). We discuss details of the model configuration for simulation of methane content until the end of the XXI century within the Representative Concentration Pathways (RCP4.5 and RCP8.5). Boundary conditions at the lower levels of the model (methane content in the surface air layer) was obtained using data from the Earth System Research Laboratories (ESRL) project and the results of the Atmospheric Chemistry-Transport Models (ACTM) for 2007–2010. The methane content in the stratosphere was also defining according to the ACTM results. The climate data used in MOZART-4 is based on the results of the Goddard Earth Observing System, Version 5 (GEOS-5). The modification of the boundary conditions carried out in the work made it possible to reproduce the summer and winter maximum in the annual course of CH4. These results are confirmed by satellite and aircraft observations made on the territory of Western Siberia. It was found that the total methane content in the atmosphere of the studied region (45–65 N, 60–90 E) in 2000–2020 increased with a trend of about 3.5 ± 0.2 ppb/year. In 2000–2006, there is virtually no trend. The increase of CH4 in 2007–2020 has a trend of ∼ 5.0 ± 0.2 ppb/year. The global data obtained as a result of the simulation can be used as initial and boundary conditions of the chemical version of the regional climate model RegCM-CHEM4.


2020 ◽  
Vol 20 (13) ◽  
pp. 7717-7740
Author(s):  
Lya Lugon ◽  
Karine Sartelet ◽  
Youngseob Kim ◽  
Jérémy Vigneron ◽  
Olivier Chrétien

Abstract. Regional-scale chemistry-transport models have coarse spatial resolution (coarser than 1 km ×1 km) and can thus only simulate background concentrations. They fail to simulate the high concentrations observed close to roads and in streets, where a large part of the urban population lives. Local-scale models may be used to simulate concentrations in streets. They often assume that background concentrations are constant and/or use simplified chemistry. Recently developed, the multi-scale model Street-in-Grid (SinG) estimates gaseous pollutant concentrations simultaneously at local and regional scales by coupling them dynamically. This coupling combines the regional-scale chemistry-transport model Polair3D and a street-network model, the Model of Urban Network of Intersecting Canyons and Highway (MUNICH), with a two-way feedback. MUNICH explicitly models street canyons and intersections, and it is coupled to the first vertical level of the chemical-transport model, enabling the transfer of pollutant mass between the street-canyon roof and the atmosphere. The original versions of SinG and MUNICH adopt a stationary hypothesis to estimate pollutant concentrations in streets. Although the computation of the NOx concentration is numerically stable with the stationary approach, the partitioning between NO and NO2 is highly dependent on the time step of coupling between transport and chemistry processes. In this study, a new nonstationary approach is presented with a fine coupling between transport and chemistry, leading to numerically stable partitioning between NO and NO2. Simulations of NO, NO2 and NOx concentrations over Paris with SinG, MUNICH and Polair3D are compared to observations at traffic and urban stations to estimate the added value of multi-scale modeling with a two-way dynamical coupling between the regional and local scales. As expected, the regional chemical-transport model underestimates NO and NO2 concentrations in the streets. However, there is good agreement between the measurements and the concentrations simulated with MUNICH and SinG. The two-way dynamic coupling between the local and regional scales tends to be important for streets with an intermediate aspect ratio and with high traffic emissions.


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