Modelling the impacts of aircraft traffic on the chemical composition of the upper troposphere

2003 ◽  
Vol 217 (5) ◽  
pp. 237-243 ◽  
Author(s):  
C Giannakopoulos ◽  
P Good ◽  
K S Law ◽  
D E Shallcross ◽  
K-Y Wang
Keyword(s):  
Chemical Composition ◽  
Transport Model ◽  
Three Dimensional ◽  
Grid Cell ◽  
Temporal Variations ◽  
Chemistry Transport Model ◽  
Mean Values ◽  
Upper Troposphere ◽  
Local Perturbations ◽  
Cent Increase

A three-dimensional chemistry-transport model has been used to assess the impacts of aircraft traffic in the upper troposphere. Aircraft engines emit NOx, which has the potential to perturb the chemical composition at the flight altitude paths, i.e. at a 10–12 km height for subsonic flights. The model used includes a comprehensive chemistry scheme, so perturbations to other species apart from NOx could also be examined. More specifically, the model showed that the monthly mean increase for NOx due to aircraft is around 60 pptv (parts per trillion volume (30 per cent increase) and for HNO3 it is 100 pptv (30 per cent increase). Consequently, O3 is enhanced by 2500 pptv (5 per cent increase) due to aircraft traffic. To assess the regional and temporal variations in the perturbations, a time series analysis above a central European grid cell located at 47 °N 18 °E has also been performed. The analysis has indicated that the local perturbations can be much larger than the monthly mean values and can reach 200 pptv for NOx, 150 pptv for HNO3 and 5000 pptv for O3.

scholarly journals Modeling anthropogenically controlled secondary organic aerosols in a megacity: a simplified framework for global and climate models

2011 ◽  
Vol 4 (4) ◽  
pp. 901-917 ◽  
Author(s):  
A. Hodzic ◽  
J. L. Jimenez
Keyword(s):  
Mexico City ◽  
Biomass Burning ◽  
Climate Models ◽  
Transport Model ◽  
Anthropogenic Pollution ◽  
Temporal Variations ◽  
Anthropogenic Sources ◽  
Organic Vapors ◽  
Chemistry Transport Model ◽  
Evolution Of Oxygen

Abstract. A simplified parameterization for secondary organic aerosol (SOA) formation in polluted air and biomass burning smoke is tested and optimized in this work, towards the goal of a computationally inexpensive method to calculate pollution and biomass burning SOA mass and hygroscopicity in global and climate models. A regional chemistry-transport model is used as the testbed for the parameterization, which is compared against observations from the Mexico City metropolitan area during the MILAGRO 2006 field experiment. The empirical parameterization is based on the observed proportionality of SOA concentrations to excess CO and photochemical age of the airmass. The approach consists in emitting an organic gas as lumped SOA precursor surrogate proportional to anthropogenic or biomass burning CO emissions according to the observed ratio between SOA and CO in aged air, and reacting this surrogate with OH into a single non-volatile species that condenses to form SOA. An emission factor of 0.08 g of the lumped SOA precursor per g of CO and a rate constant with OH of 1.25 × 10−11 cm3 molecule−1 s−1 reproduce the observed average SOA mass within 30 % in the urban area and downwind. When a 2.5 times slower rate is used (5 × 10−12 cm3 molecule−1 s−1) the predicted SOA amount and temporal evolution is nearly identical to the results obtained with SOA formation from semi-volatile and intermediate volatility primary organic vapors according to the Robinson et al. (2007) formulation. Our simplified method has the advantage of being much less computationally expensive than Robinson-type methods, and can be used in regions where the emissions of SOA precursors are not yet available. As the aged SOA/ΔCO ratios are rather consistent globally for anthropogenic pollution, this parameterization could be reasonably tested in and applied to other regions. The evolution of oxygen-to-carbon ratio was also empirically modeled and the predicted levels were found to be in reasonable agreement with observations. The potential enhancement of biogenic SOA by anthropogenic pollution, which has been suggested to play a major role in global SOA formation, is also tested using two simple parameterizations. Our results suggest that the pollution enhancement of biogenic SOA could provide additional SOA, but does not however explain the concentrations or the spatial and temporal variations of measured SOA mass in the vicinity of Mexico City, which appears to be controlled by anthropogenic sources. The contribution of the biomass burning to the predicted SOA is less than 10% during the studied period.

scholarly journals Modeling the transport of very short-lived substances into the tropical upper troposphere and lower stratosphere

2009 ◽  
Vol 9 (5) ◽  
pp. 18511-18543 ◽  
Author(s):  
J. Aschmann ◽  
B. M. Sinnhuber ◽  
E. L. Atlas ◽  
S. M. Schauffler
Keyword(s):  
Large Scale ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Three Dimensional ◽  
Chemical Transport Model ◽  
Heating Rates ◽  
Model Calculations ◽  
Upper Troposphere ◽  
Mass Fluxes ◽  
Tropical Upper Troposphere

Abstract. The transport of very short-lived substances into the tropical upper troposphere and lower stratosphere is investigated by a three-dimensional chemical transport model using archived convective updraft mass fluxes (or detrainment rates) from the European Centre for Medium-Range Weather Forecast's ERA-Interim reanalysis. Large-scale vertical velocities are calculated from diabatic heating rates. With this approach we explicitly model the large scale subsidence in the tropical troposphere with convection taking place in fast and isolated updraft events. The model calculations agree generally well with observations of bromoform and methyl iodide from aircraft campaigns and with ozone and water vapor from sonde and satellite observations. Using a simplified treatment of dehydration and bromine product gas washout we give a range of 1.6 to 3 ppt for the contribution of bromoform to stratospheric bromine, assuming a uniform source in the boundary layer of 1 ppt. We show that the most effective region for VSLS transport into the stratosphere is the West Pacific, accounting for about 55% of the bromine from bromoform transported into the stratosphere under the supposition of a uniformly distributed source.

scholarly journals Towards an online-coupled chemistry-climate model: evaluation of trace gases and aerosols in COSMO-ART

2011 ◽  
Vol 4 (4) ◽  
pp. 1077-1102 ◽  
Author(s):  
C. Knote ◽  
D. Brunner ◽  
H. Vogel ◽  
J. Allan ◽  
A. Asmi ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Size Distribution ◽  
Urban Areas ◽  
Climate Model ◽  
Transport Model ◽  
Climate Impacts ◽  
Chemistry Transport Model ◽  
Pm2.5 And Pm10 ◽  
Phase Chemistry ◽  
Aerosol Chemical Composition

Abstract. The online-coupled, regional chemistry transport model COSMO-ART is evaluated for periods in all seasons against several measurement datasets to assess its ability to represent gaseous pollutants and ambient aerosol characteristics over the European domain. Measurements used in the comparison include long-term station observations, satellite and ground-based remote sensing products, and complex datasets of aerosol chemical composition and number size distribution from recent field campaigns. This is the first time these comprehensive measurements of aerosol characteristics in Europe are used to evaluate a regional chemistry transport model. We show a detailed analysis of the simulated size-resolved chemical composition under different meteorological conditions. Mean, variability and spatial distribution of the concentrations of O3 and NOx are well reproduced. SO2 is found to be overestimated, simulated PM2.5 and PM10 levels are on average underestimated, as is AOD. We find indications of an overestimation of shipping emissions. Time evolution of aerosol chemical composition is captured, although some biases are found in relative composition. Nitrate aerosol components are on average overestimated, and sulfates underestimated. The accuracy of simulated organics depends strongly on season and location. While strongly underestimated during summer, organic mass is comparable in spring and autumn. We see indications for an overestimated fractional contribution of primary organic matter in urban areas and an underestimation of SOA at many locations. Aerosol number concentrations compare well with measurements for larger size ranges, but overestimations of particle number concentration with factors of 2–5 are found for particles smaller than 50 nm. Size distribution characteristics are often close to measurements, but show discrepancies at polluted sites. Suggestions for further improvement of the modeling system consist of the inclusion of a revised secondary organic aerosols scheme, aqueous-phase chemistry and improved aerosol boundary conditions. Our work sets the basis for subsequent studies of aerosol characteristics and climate impacts with COSMO-ART, and highlights areas where improvements are necessary for current regional modeling systems in general.

scholarly journals A Methodology for Estimating the Parameters in Three-Dimensional Cohesive Sediment Transport Models by Assimilating In Situ Observations with the Adjoint Method

2017 ◽  
Vol 34 (7) ◽  
pp. 1469-1482 ◽  
Author(s):  
Daosheng Wang ◽  
Jicai Zhang ◽  
Ya Ping Wang ◽  
Xianqing Lv ◽  
Yang Yang ◽  
...  
Keyword(s):  
Sediment Transport ◽  
Adjoint Method ◽  
Settling Velocity ◽  
Transport Model ◽  
Three Dimensional ◽  
Temporal Variations ◽  
Cohesive Sediment ◽  
Cohesive Sediment Transport ◽  
Resuspension Rate

AbstractThe model parameters in the suspended cohesive sediment transport model are quite important for the accurate simulation of suspended sediment concentrations (SSCs). Based on a three-dimensional cohesive sediment transport model and its adjoint model, the in situ observed SSCs at four stations are assimilated to simulate the SSCs and to estimate the parameters in Hangzhou Bay in China. Numerical experimental results show that the adjoint method can efficiently improve the simulation results, which can benefit the prediction of SSCs. The time series of the modeled SSCs present a clear semidiurnal variation, in which the maximal SSCs occur during the flood tide and near the high water level due to the large current speeds. Sensitivity experiments prove that the estimated results of the settling velocity and resuspension rate, especially the temporal variations, are robust to the model settings. The temporal variations of the estimated settling velocity are negatively correlated with the tidal elevation. The main reason is that the mean size of the suspended sediments can be reduced during the flood tide, which consequently decreases the settling velocity according to Stokes’s law, and it is opposite in the ebb tide. The temporal variations of the estimated resuspension rate and the current speeds have a significantly positive correlation, which accords with the dynamics of the resuspension rate. The temporal variations of the settling velocity and resuspension rate are reasonable from the viewpoint of physics, indicating the adjoint method can be an effective tool for estimating the parameters in the sediment transport models.

scholarly journals Technical Note: A new SIze REsolved Aerosol Model (SIREAM)

2007 ◽  
Vol 7 (6) ◽  
pp. 1537-1547 ◽  
Author(s):  
E. Debry ◽  
K. Fahey ◽  
K. Sartelet ◽  
B. Sportisse ◽  
M. Tombette
Keyword(s):  
Size Distribution ◽  
Transport Model ◽  
Three Dimensional ◽  
Technical Note ◽  
Aerosol Size Distribution ◽  
Short Paper ◽  
Chemistry Transport Model ◽  
Dynamical Mass ◽  
Aerosol Model ◽  
Transfer Method

Abstract. We briefly present in this short paper a new SIze REsolved Aerosol Model (SIREAM) which simulates the evolution of atmospheric aerosol by solving the General Dynamic Equation (GDE). SIREAM segregates the aerosol size distribution into sections and solves the GDE by splitting coagulation and condensation/evaporation-nucleation. A quasi-stationary sectional approach is used to describe the size distribution change due to condensation/evaporation, and a hybrid equilibrium/dynamical mass-transfer method has been developed to lower the computational burden. SIREAM uses the same physical parameterizations as those used in the Modal Aerosol Model, MAM Sartelet et al. (2006). It is hosted in the modeling system Polyphemus Mallet et al., 2007, but can be linked to any other three-dimensional Chemistry-Transport Model.

scholarly journals Technical Note: A new SIze REsolved Aerosol Model (SIREAM)

2006 ◽  
Vol 6 (6) ◽  
pp. 11845-11875 ◽  
Author(s):  
E. Debry ◽  
K. Fahey ◽  
K. Sartelet ◽  
B. Sportisse ◽  
M. Tombette
Keyword(s):  
Size Distribution ◽  
Atmospheric Aerosol ◽  
Transport Model ◽  
Three Dimensional ◽  
Technical Note ◽  
Aerosol Size Distribution ◽  
Short Paper ◽  
Chemistry Transport Model ◽  
Aerosol Model ◽  
General Dynamic

Abstract. We briefly present in this short paper a new SIze REsolved Aerosol Model (SIREAM) which simulates the evolution of atmospheric aerosol by solving the General Dynamic Equation (GDE). SIREAM segregates the aerosol size distribution into sections and solves the GDE by splitting coagulation and condensation/evaporation. A moving sectional approach is used to describe the size distribution change due to condensation/evaporation and a hybrid method has been developed to lower the computational burden. SIREAM uses the same physical parameterizations as those used in the Modal Aerosol Model, MAM sartelet05development. It is hosted in the modeling system POLYPHEMUS (Mallet et al., 2006) but can be linked to any other three-dimensional Chemistry-Transport Model.

scholarly journals Composite study of aerosol export events from East Asia and North America

2012 ◽  
Vol 12 (8) ◽  
pp. 21977-22022 ◽  
Author(s):  
Y. Luan ◽  
L. Jaeglé
Keyword(s):  
Boundary Layer ◽  
North America ◽  
East Asia ◽  
Transport Model ◽  
Lower Troposphere ◽  
Temporal Variations ◽  
The Arctic ◽  
Chemical Transport Model ◽  
Mean Values ◽  
Warm Conveyor Belts

Abstract. We use satellite observations of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectrometer (MODIS) together with the GEOS-Chem global chemical transport model to contrast export of aerosols from East Asia and North America during 2004–2010. The GEOS-Chem model reproduces the spatial distribution and temporal variations of Asian aerosol outflow generally well, although a low bias (−30%) is found in the model fine mode AOD. We use the model to identify 244 aerosol pollution export events from E. Asia and 251 export events from N. America over our 7-yr study period. When these events are composited by season, we find that the AOD in the outflow is enhanced by 50–100% relative to seasonal mean values. The composite Asian plume splits into one branch going poleward towards the Arctic, with the other crossing the Pacific in 6–8 days. A fraction of the aerosols is trapped in the subtropical Pacific High. The N. American plume travels to the northeast Atlantic, reaching Europe after 4–5 days. Part of the composite plume turns anticyclonically in the Azores High, where it slowly decays. Both the Asian and N. American export events are favored by a dipole structure in sea-level pressure anomalies, associated with mid-latitude cyclone activity over the respective source regions. The observed AOD in the E. Asian outflow exhibits stronger seasonality, with a spring maximum, than the N. American outflow, with a weak summer maximum. The large spring AOD in the Asian outflow is the result of enhanced sulfate and dust aerosol concentrations, but is also due to a larger export efficiency of sulfate and SO2 from the Asian boundary layer relative to the N. American boundary layer. While the N. American sulfate outflow is mostly found in the lower troposphere (1–3 km altitude), the Asian sulfate outflow occurs at higher altitudes (2–6 km). In the Asian outflow 42–59% of the sulfate column is present above 2 km altitude, with only 24–35% in the N. American outflow. We link this to the factor of 2–5 lower precipitation in the warm conveyor belts (WCB) of midlatitude cyclones over E. Asia compared to N. America. This relative lack of precipitation makes Asian WCB very efficient for injecting aerosols in the middle troposphere.

scholarly journals Description and evaluation of a detailed gas-phase chemistry scheme in the TM5-MP global chemistry transport model (r112)

2020 ◽  
Author(s):  
Stelios Myriokefalitakis ◽  
Nikos Daskalakis ◽  
Angelos Gkouvousis ◽  
Andreas Hilboll ◽  
Twan van Noije ◽  
...  
Keyword(s):  
Gas Phase ◽  
Transport Model ◽  
Vertical Mixing ◽  
Three Dimensional ◽  
Chemical Mechanism ◽  
Aerosol Formation ◽  
Chemistry Transport Model ◽  
Mixing Ratios ◽  
Time Requirements ◽  
Phase Chemistry

Abstract. This work documents and evaluates the tropospheric gas-phase chemical mechanism MOGUNTIA in the three-dimensional chemistry transport model TM5-MP. Compared to the modified CB05 chemical mechanism previously used in the model, the MOGUNTIA includes a detailed representation of the light hydrocarbons (C1-C4) and isoprene, along with a simplified chemistry representation of terpenes and aromatics. Another feature implemented in TM5-MP for this work is the use of the Rosenbrock solver in the chemistry code, which can replace the classical Euler Backward Integration method of the model. Global budgets of ozone (O3), carbon monoxide (CO), hydroxyl radicals (OH), nitrogen oxides (NOX) and volatile organic compounds (VOCs) are here analyzed and their mixing ratios are compared with a series of surface, aircraft and satellite observations for the year 2006. Both mechanisms appear to be able to represent satisfactorily observed mixing ratios of important trace gases, with the MOGUNTIA chemistry configuration yielding lower biases compared to measurements in most of the cases. However, the two chemical mechanisms fail to reproduce the observed mixing ratios of light VOCs, indicating insufficient primary emission source strengths, too weak vertical mixing in the boundary layer, and/or a low bias in the secondary contribution of C2-C3 organics via VOC atmospheric oxidation. Relative computational memory and time requirements of the different model configurations are also compared and discussed. Overall, compared to other chemistry schemes in use in global CTMs, the MOGUNTIA scheme simulates a large suite of oxygenated VOCs that are observed in the atmosphere at significant levels and are involved in aerosol formation, expanding, thus, the applications of TM5-MP.

scholarly journals Assimilation of TES CO into a global CTM: first results

2006 ◽  
Vol 6 (6) ◽  
pp. 11727-11743 ◽  
Author(s):  
N. A. D. Richards ◽  
Q. Li ◽  
K. W. Bowman ◽  
J. R. Worden ◽  
S. S. Kulawik ◽  
...  
Keyword(s):  
Transport Model ◽  
Model Simulation ◽  
Three Dimensional ◽  
Model Bias ◽  
Upper Troposphere ◽  
First Results ◽  
Assimilation Scheme ◽  
Co Observations ◽  
Good Agreement

Abstract. We present results from the first assimilation of carbon monoxide (CO) observations from the Tropospheric Emission Spectrometer (TES) into a global three-dimensional (3-D) chemistry and transport model (CTM). A sequential sub-optimal Kalman filter assimilation scheme (Khattatov et al., 2000) was applied to assimilate TES CO profiles during November 2004 into the GEOS-Chem global 3-D CTM. The assimilation results were compared with MOPITT and MOZAIC observations. The assimilation significantly improves model simulation of CO in the middle to upper troposphere, where the MOPITT versus model bias was reduced by up to two-thirds. Assimilation results show higher levels of CO in the southern tropics, consistent with MOPITT observations. We find good agreement between the TES assimilated model estimates of CO and in situ measurements from the MOZAIC program, which shows a negative bias of up to 10 ppbv in middle and upper tropospheric TES CO. The results demonstrate how assimilation can be used for non-coincident validation of TES CO profile retrievals.

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