scholarly journals Sensitivity of chemical transport model simulations to the duration of chemical and transport operators: a case study with GEOS-Chem v10-01

2015 ◽  
Vol 8 (11) ◽  
pp. 9589-9616
Author(s):  
S. Philip ◽  
R. V. Martin ◽  
C. A. Keller
Keyword(s):  
Spatial Resolution ◽  
Temporal Resolution ◽  
Transport Model ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Transport Models ◽  
Simulation Accuracy ◽  
Chemical Transport Models ◽  
Order Of Magnitude ◽  
Simulation Error

Abstract. Chemical transport models involve considerable computational expense. Fine temporal resolution offers accuracy at the expense of computation time. Assessment is needed of the sensitivity of simulation accuracy to the duration of chemical and transport operators. We conduct a series of simulations with the GEOS-Chem chemical transport model at different temporal and spatial resolutions to examine the sensitivity of simulated atmospheric composition to temporal resolution. Subsequently, we compare the tracers simulated with operator durations from 10 to 60 min as typically used by global chemical transport models, and identify the timesteps that optimize both computational expense and simulation accuracy. We found that longer transport timesteps increase concentrations of emitted species such as nitrogen oxides and carbon monoxide since a more homogeneous distribution reduces loss through chemical reactions and dry deposition. The increased concentrations of ozone precursors increase ozone production at longer transport timesteps. Longer chemical timesteps decrease sulfate and ammonium but increase nitrate due to feedbacks with in-cloud sulfur dioxide oxidation and aerosol thermodynamics. The simulation duration decreases by an order of magnitude from fine (5 min) to coarse (60 min) temporal resolution. We assess the change in simulation accuracy with resolution by comparing the root mean square difference in ground-level concentrations of nitrogen oxides, ozone, carbon monoxide and secondary inorganic aerosols with a finer temporal or spatial resolution taken as truth. Simulation error for these species increases by more than a factor of 5 from the shortest (5 min) to longest (60 min) temporal resolution. Chemical timesteps twice that of the transport timestep offer more simulation accuracy per unit computation. However, simulation error from coarser spatial resolution generally exceeds that from longer timesteps; e.g. degrading from 2° × 2.5° to 4° × 5° increases error by an order of magnitude. We recommend prioritizing fine spatial resolution before considering different temporal resolutions in offline chemical transport models. We encourage the chemical transport model users to specify in publications the durations of operators due to their effects on simulation accuracy.

scholarly journals Skill-Testing Chemical Transport Models across Contrasting Atmospheric Mixing States Using Radon-222

2018 ◽  
Author(s):  
Scott D. Chambers ◽  
Elise-Andree Guérette ◽  
Khalia Monk ◽  
Alan D. Griffiths ◽  
Yang Zhang ◽  
...  
Keyword(s):  
Air Quality ◽  
Diurnal Cycle ◽  
Transport Model ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Transport Models ◽  
Potential Health ◽  
Meteorological Model ◽  
Model Skill ◽  
Chemical Transport Models

We propose a new technique to prepare statistically-robust benchmarking data for evaluating chemical transport model meteorology and air quality parameters within the urban boundary layer. The approach employs atmospheric class-typing, using nocturnal radon measurements to assign atmospheric mixing classes, and can be applied temporally (across the diurnal cycle), or spatially (to create angular distributions of pollutants as a top-down constraint on emissions inventories). In this study only a short (<1-month) campaign is used, but grouping of the relative mixing classes based on nocturnal mean radon concentrations can be adjusted according to dataset length (i.e., number of days per category), or desired range of within-class variability. Calculating hourly distributions of observed and simulated values across diurnal composites of each class-type helps to: (i) bridge the gap between scales of simulation and observation, (ii) represent the variability associated with spatial and temporal heterogeneity of sources and meteorology without being confused by it, and (iii) provide an objective way to group results over whole diurnal cycles that separates ‘natural complicating factors’ (synoptic non-stationarity, rainfall, mesoscale motions, extreme stability, etc.) from problems related to parameterizations, or between-model differences. We demonstrate the utility of this technique using output from a suite of seven contemporary regional forecast and chemical transport models. Meteorological model skill varied across the diurnal cycle for all models, with an additional dependence on the atmospheric mixing class that varied between models. From an air quality perspective, model skill regarding the duration and magnitude of morning and evening “rush hour” pollution events varied strongly as a function of mixing class. Model skill was typically the lowest when public exposure would have been the highest, which has important implications for assessing potential health risks in new and rapidly evolving urban regions, and also for prioritizing the areas of model improvement for future applications.

scholarly journals On the ability of chemical transport models to simulate the vertical structure of the N<sub>2</sub>O, NO<sub>2</sub> and HNO<sub>3</sub> species in the mid-latitude stratosphere

2005 ◽  
Vol 5 (6) ◽  
pp. 12373-12401
Author(s):  
G. Berthet ◽  
N. Huret ◽  
F. Lefèvre ◽  
G. Moreau ◽  
C. Robert ◽  
...  
Keyword(s):  
Transport Model ◽  
Three Dimensional ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Transport Models ◽  
One Dimensional ◽  
Chemical Transport Models ◽  
Dimensional Version ◽  
The Impact

Abstract. In this paper we study the impact of the modelling of N2O on the simulation of NO2 and HNO3 by comparing in situ vertical profiles measured at mid-latitudes with the results of the Reprobus 3-D CTM (Three-dimensional Chemical Transport Model) computed with the kinetic parameters from the JPL recommendation in 2002. The analysis of the measured in situ profile of N2O shows particular features indicating different air mass origins. The measured N2O, NO2 and HNO3 profiles are not satisfyingly reproduced by the CTM when computed using the current 6-hourly ECMWF operational analysis. Improving the simulation of N2O transport allows us to calculate quantities of NO2 and HNO3 in reasonable agreement with observations. This is achieved using 3-hourly winds obtained from ECMWF forecasts. The best agreement is obtained by constraining a one-dimensional version of the model with the observed N2O. This study shows that modelling the NOy partitioning with better accuracy relies at least on a correct simulation of N2O and thus of total NOy.

scholarly journals Sensitivity of chemistry-transport model simulations to the duration of chemical and transport operators: a case study with GEOS-Chem v10-01

2016 ◽  
Vol 9 (5) ◽  
pp. 1683-1695 ◽  
Author(s):  
Sajeev Philip ◽  
Randall V. Martin ◽  
Christoph A. Keller
Keyword(s):  
Carbon Monoxide ◽  
Nitrogen Oxides ◽  
Spatial Resolution ◽  
Transport Model ◽  
Transport Models ◽  
Chemistry Transport Model ◽  
Simulation Accuracy ◽  
Transport Operator ◽  
Computational Expense ◽  
Simulation Error

Abstract. Chemistry-transport models involve considerable computational expense. Fine temporal resolution offers accuracy at the expense of computation time. Assessment is needed of the sensitivity of simulation accuracy to the duration of chemical and transport operators. We conduct a series of simulations with the GEOS-Chem chemistry-transport model at different temporal and spatial resolutions to examine the sensitivity of simulated atmospheric composition to operator duration. Subsequently, we compare the species simulated with operator durations from 10 to 60 min as typically used by global chemistry-transport models, and identify the operator durations that optimize both computational expense and simulation accuracy. We find that longer continuous transport operator duration increases concentrations of emitted species such as nitrogen oxides and carbon monoxide since a more homogeneous distribution reduces loss through chemical reactions and dry deposition. The increased concentrations of ozone precursors increase ozone production with longer transport operator duration. Longer chemical operator duration decreases sulfate and ammonium but increases nitrate due to feedbacks with in-cloud sulfur dioxide oxidation and aerosol thermodynamics. The simulation duration decreases by up to a factor of 5 from fine (5 min) to coarse (60 min) operator duration. We assess the change in simulation accuracy with resolution by comparing the root mean square difference in ground-level concentrations of nitrogen oxides, secondary inorganic aerosols, ozone and carbon monoxide with a finer temporal or spatial resolution taken as “truth”. Relative simulation error for these species increases by more than a factor of 5 from the shortest (5 min) to longest (60 min) operator duration. Chemical operator duration twice that of the transport operator duration offers more simulation accuracy per unit computation. However, the relative simulation error from coarser spatial resolution generally exceeds that from longer operator duration; e.g., degrading from 2°  ×  2.5° to 4°  ×  5° increases error by an order of magnitude. We recommend prioritizing fine spatial resolution before considering different operator durations in offline chemistry-transport models. We encourage chemistry-transport model users to specify in publications the durations of operators due to their effects on simulation accuracy.

scholarly journals On the ability of chemical transport models to simulate the vertical structure of the N<sub>2</sub>O, NO<sub>2</sub> and HNO<sub>3</sub> species in the mid-latitude stratosphere

2006 ◽  
Vol 6 (6) ◽  
pp. 1599-1609 ◽  
Author(s):  
G. Berthet ◽  
N. Huret ◽  
F. Lefèvre ◽  
G. Moreau ◽  
C. Robert ◽  
...  
Keyword(s):  
Transport Model ◽  
Three Dimensional ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Transport Models ◽  
One Dimensional ◽  
Chemical Transport Models ◽  
Dimensional Version ◽  
The Impact

Abstract. In this paper we study the impact of the modelling of N2O on the simulation of NO2 and HNO3 by comparing in situ vertical profiles measured at mid-latitudes with the results of the Reprobus 3-D CTM (Three-dimensional Chemical Transport Model) computed with the kinetic parameters from the JPL recommendation in 2002. The analysis of the measured in situ profile of N2O shows particular features indicating different air mass origins. The measured N2O, NO2 and HNO3 profiles are not satisfyingly reproduced by the CTM when computed using the current 6-hourly ECMWF operational analysis. Improving the simulation of N2O transport allows us to calculate quantities of NO2 and HNO3 in reasonable agreement with observations. This is achieved using 3-hourly winds obtained from ECMWF forecasts. The best agreement is obtained by constraining a one-dimensional version of the model with the observed N2O. This study shows that the modelling of the NOy partitioning with better accuracy relies at least on a correct simulation of N2O and thus of total NOy.

scholarly journals Skill-Testing Chemical Transport Models across Contrasting Atmospheric Mixing States Using Radon-222

Atmosphere ◽  
2019 ◽  
Vol 10 (1) ◽  
pp. 25 ◽  
Author(s):  
Scott Chambers ◽  
Elise-Andree Guérette ◽  
Khalia Monk ◽  
Alan Griffiths ◽  
Yang Zhang ◽  
...  
Keyword(s):  
Air Quality ◽  
Diurnal Cycle ◽  
Transport Model ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Transport Models ◽  
Potential Health ◽  
Meteorological Model ◽  
Model Skill ◽  
Chemical Transport Models

We propose a new technique to prepare statistically-robust benchmarking data for evaluating chemical transport model meteorology and air quality parameters within the urban boundary layer. The approach employs atmospheric class-typing, using nocturnal radon measurements to assign atmospheric mixing classes, and can be applied temporally (across the diurnal cycle), or spatially (to create angular distributions of pollutants as a top-down constraint on emissions inventories). In this study only a short (<1-month) campaign is used, but grouping of the relative mixing classes based on nocturnal mean radon concentrations can be adjusted according to dataset length (i.e., number of days per category), or desired range of within-class variability. Calculating hourly distributions of observed and simulated values across diurnal composites of each class-type helps to: (i) bridge the gap between scales of simulation and observation, (ii) represent the variability associated with spatial and temporal heterogeneity of sources and meteorology without being confused by it, and (iii) provide an objective way to group results over whole diurnal cycles that separates ‘natural complicating factors’ (synoptic non-stationarity, rainfall, mesoscale motions, extreme stability, etc.) from problems related to parameterizations, or between-model differences. We demonstrate the utility of this technique using output from a suite of seven contemporary regional forecast and chemical transport models. Meteorological model skill varied across the diurnal cycle for all models, with an additional dependence on the atmospheric mixing class that varied between models. From an air quality perspective, model skill regarding the duration and magnitude of morning and evening “rush hour” pollution events varied strongly as a function of mixing class. Model skill was typically the lowest when public exposure would have been the highest, which has important implications for assessing potential health risks in new and rapidly evolving urban regions, and also for prioritizing the areas of model improvement for future applications.

scholarly journals Data Assimilation as a Tool to Improve Chemical Transport Models Performance in Developing Countries

2021 ◽  
Author(s):  
Santiago Lopez-Restrepo ◽  
Andrés Yarce Botero ◽  
Olga Lucia Quintero ◽  
Nicolás Pinel ◽  
Jhon Edinson Hinestroza ◽  
...  
Keyword(s):  
Particulate Matter ◽  
Data Assimilation ◽  
Transport Model ◽  
Population Expansion ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Tropical Andes ◽  
Urban Centers ◽  
Transport Models ◽  
Chemical Transport Models

Particulate matter (PM) is one of the most problematic pollutants in urban air. The effects of PM on human health, associated especially with PM of ≤2.5μm in diameter, include asthma, lung cancer and cardiovascular disease. Consequently, major urban centers commonly monitor PM2.5 as part of their air quality management strategies. The Chemical Transport models allow for a permanent monitoring and prediction of pollutant behavior for all the regions of interest, different to the sensor network where the concentration is just available in specific points. In this chapter a data assimilation system for the LOTOS-EUROS chemical transport model has been implemented to improve the simulation and forecast of Particulate Matter in a densely populated urban valley of the tropical Andes. The Aburrá Valley in Colombia was used as a case study, given data availability and current environmental issues related to population expansion. Using different experiments and observations sources, we shown how the Data Assimilation can improve the model representation of pollutants.

scholarly journals Implementation of state-of-the-art ternary new-particle formation scheme to the regional chemical transport model PMCAMx-UF in Europe

2016 ◽  
Vol 9 (8) ◽  
pp. 2741-2754 ◽  
Author(s):  
Elham Baranizadeh ◽  
Benjamin N. Murphy ◽  
Jan Julin ◽  
Saeed Falahat ◽  
Carly L. Reddington ◽  
...  
Keyword(s):  
Transport Model ◽  
Three Dimensional ◽  
Chemical Transport ◽  
Particle Formation ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
New Particle Formation ◽  
Chemical Transport Model ◽  
Order Of Magnitude ◽  
Adjustment Scheme

Abstract. The particle formation scheme within PMCAMx-UF, a three-dimensional chemical transport model, was updated with particle formation rates for the ternary H2SO4–NH3–H2O pathway simulated by the Atmospheric Cluster Dynamics Code (ACDC) using quantum chemical input data. The model was applied over Europe for May 2008, during which the EUCAARI-LONGREX (European Aerosol Cloud Climate and Air Quality Interactions–Long-Range Experiment) campaign was carried out, providing aircraft vertical profiles of aerosol number concentrations. The updated model reproduces the observed number concentrations of particles larger than 4 nm within 1 order of magnitude throughout the atmospheric column. This agreement is encouraging considering the fact that no semi-empirical fitting was needed to obtain realistic particle formation rates. The cloud adjustment scheme for modifying the photolysis rate profiles within PMCAMx-UF was also updated with the TUV (Tropospheric Ultraviolet and Visible) radiative-transfer model. Results show that, although the effect of the new cloud adjustment scheme on total number concentrations is small, enhanced new-particle formation is predicted near cloudy regions. This is due to the enhanced radiation above and in the vicinity of the clouds, which in turn leads to higher production of sulfuric acid. The sensitivity of the results to including emissions from natural sources is also discussed.

scholarly journals Mixing times of organic molecules within secondary organic aerosol particles: a global planetary boundary layer perspective

2017 ◽  
Author(s):  
Adrian M. Maclean ◽  
Christopher L. Butenhoff ◽  
James W. Grayson ◽  
Kelley Barsanti ◽  
Jose L. Jimenez ◽  
...  
Keyword(s):  
Organic Molecules ◽  
Secondary Organic Aerosol ◽  
Transport Model ◽  
Laboratory Data ◽  
Chemical Transport ◽  
Organic Aerosol ◽  
Mixing Times ◽  
Chemical Transport Model ◽  
Transport Models ◽  
Lack Of Information

Abstract. When simulating the formation and life cycle of secondary organic aerosol (SOA) with chemical transport models, it is often assumed that organic molecules are well mixed within SOA particles on the time scale of 1 h. While this assumption has been debated vigorously in the literature, the issue remains unresolved in part due to a lack of information on the mixing times within SOA particles as a function of both temperature and relative humidity. Using laboratory data, meteorological fields and a chemical transport model, we determine how often mixing times are

scholarly journals Tagged ozone mechanism for MOZART-4, CAM-chem and other chemical transport models

2012 ◽  
Vol 5 (6) ◽  
pp. 1531-1542 ◽  
Author(s):  
L. K. Emmons ◽  
P. G. Hess ◽  
J.-F. Lamarque ◽  
G. G. Pfister
Keyword(s):  
Transport Model ◽  
Stratospheric Ozone ◽  
Chemical Transport ◽  
Chemical Mechanism ◽  
Chemical Transport Model ◽  
Transport Models ◽  
Chemical Tracers ◽  
Source Contributions ◽  
The Difference ◽  
No Emissions

Abstract. A procedure for tagging ozone produced from NO sources through updates to an existing chemical mechanism is described, and results from its implementation in the Model for Ozone and Related chemical Tracers (MOZART-4), a global chemical transport model, are presented. Artificial tracers are added to the mechanism, thus, not affecting the standard chemistry. The results are linear in the troposphere, i.e., the sum of ozone from individual tagged sources equals the ozone from all sources to within 3% in zonal mean monthly averages. In addition, the tagged ozone is shown to equal the standard ozone, when all tropospheric sources are tagged and stratospheric input is turned off. The stratospheric ozone contribution to the troposphere determined from the difference between total ozone and ozone from all tagged sources is significantly less than estimates using a traditional stratospheric ozone tracer (8 vs. 20 ppbv at the surface). The commonly used technique of perturbing NO emissions by 20% in a region to determine its ozone contribution is compared to the tagging technique, showing that the tagged ozone is 2–4 times the ozone contribution that was deduced from perturbing emissions. The ozone tagging described here is useful for identifying source contributions based on NO emissions in a given state of the atmosphere, such as for quantifying the ozone budget.

High resolution Aerosol Radiative Effects over Europe using detailed optical properties from the Chemical Transport Model PMCAMx

2020 ◽  
Author(s):  
Marios Bruno Korras Carraca ◽  
Dimitris Manetas ◽  
David Patoulias ◽  
Spyros Pandis ◽  
Nikolaos Hatzianastassiou ◽  
...  
Keyword(s):  
Optical Properties ◽  
Temporal Resolution ◽  
Biomass Burning ◽  
Transport Model ◽  
Aerosol Particles ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Aerosol Optical Properties ◽  
The Earth ◽  
Spatio Temporal

&lt;p&gt;Natural and anthropogenic aerosol particles are major drivers of the Earth&amp;#8217;s radiation budget, which they affect directly (through scattering and absorption) and indirectly (through modification of cloud scattering and precipitation properties), while they semi-directly influence atmospheric stability and convection, mainly through modification of solar radiation absorption by the atmosphere. Despite the important climatic role of aerosols, large uncertainties in their radiative effects remain due to limited knowledge of the aerosol spatio-temporal distribution and physico-chemical properties. The interaction of aerosols with radiation is strongly dependent on their optical properties, which in turn are controlled by the particles&amp;#8217; size distribution, shape, chemical composition and mixing state. In order to accurately estimate the magnitude of the aerosol direct radiative effect (DRE), detailed knowledge of their optical properties with high spatial and temporal resolution is required.&lt;/p&gt;&lt;p&gt;The European continent is a region of particular interest for studying atmospheric aerosol effects, because of the presence of&amp;#160; numerous and varying sources of particles and their precursors, such as industries, large urban centers and biomass burning, especially when combined with high levels of solar insolation during summer. In this study, the aerosol DRE over Europe is examined using the FORTH deterministic spectral radiative transfer model (RTM) and aerosol data from the chemical transport model PMCAMx. Chemically and size resolved aerosol concentrations predicted by PMCAMx are combined with a Mie model to calculate key aerosol optical properties (i.e. vertically resolved aerosol optical depth, single scattering albedo and asymmetry parameter) that are necessary to compute aerosol DRE using the RTM. The Mie model takes into account concentrations of organics, black carbon, sulfate, nitrate, ammonium, chlorine, sodium, water, and crustal material, and calculates aerosol optical properties assuming that the aerosol particles of the same size are internally mixed. The DRE is estimated at the Earth&amp;#8217;s surface, within the atmospheric column and at the top of the atmosphere (TOA), at high spatial and temporal resolution (36 &amp;#215; 36 km grids, 27 vertical layers, hourly), during June and July 2012.&lt;/p&gt;&lt;p&gt;Initial modelling results reveal that DREs exhibit significant spatio-temporal variability, due to the heterogeneity of source emissions rates, mostly with regard to wildfires, and the varying synoptic conditions. Emphasis is thus given to biomass burning aerosols, which are among the most significant radiative forcing agents in Europe during summer. Their relative forcing is computed by performing model computations with and without biomass burning emissions.&lt;/p&gt;

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