scholarly journals The Chemistry of Atmosphere-Forest Exchange (CAFE) Model – Part 1: Model description and characterization

2010 ◽  
Vol 10 (9) ◽  
pp. 21721-21790
Author(s):  
G. M. Wolfe ◽  
J. A. Thornton

Abstract. We present the Chemistry of Atmosphere-Forest Exchange (CAFE) model, a vertically-resolved 1-D chemical transport model designed to probe the details of near-surface reactive gas exchange. CAFE integrates all key processes, including turbulent diffusion, emission, deposition and chemistry, throughout the forest canopy and mixed layer. It is the first model of its kind to incorporate the Master Chemical Mechanism (MCM) and a suite of reactions for the oxidation of monoterpenes and sesquiterpenes, providing a more comprehensive description of the oxidative chemistry occurring within and above the forest. We use CAFE to simulate a young Ponderosa pine forest in the Sierra Nevada, CA. Utilizing meteorological constraints from the BEARPEX-2007 field campaign, we assess the sensitivity of modeled fluxes to parameterizations of diffusion, laminar sublayer resistance and radiation extinction. To characterize the general chemical environment of this forest, we also present modeled mixing ratio profiles of biogenic hydrocarbons, hydrogen oxides and reactive nitrogen. The vertical profiles of these species demonstrate a range of structures and gradients that reflect the interplay of physical and chemical processes within the forest canopy, which can influence net exchange.

2011 ◽  
Vol 11 (1) ◽  
pp. 77-101 ◽  
Author(s):  
G. M. Wolfe ◽  
J. A. Thornton

Abstract. We present the Chemistry of Atmosphere-Forest Exchange (CAFE) model, a vertically-resolved 1-D chemical transport model designed to probe the details of near-surface reactive gas exchange. CAFE integrates all key processes, including turbulent diffusion, emission, deposition and chemistry, throughout the forest canopy and mixed layer. CAFE utilizes the Master Chemical Mechanism (MCM) and is the first model of its kind to incorporate a suite of reactions for the oxidation of monoterpenes and sesquiterpenes, providing a more comprehensive description of the oxidative chemistry occurring within and above the forest. We use CAFE to simulate a young Ponderosa pine forest in the Sierra Nevada, CA. Utilizing meteorological constraints from the BEARPEX-2007 field campaign, we assess the sensitivity of modeled fluxes to parameterizations of diffusion, laminar sublayer resistance and radiation extinction. To characterize the general chemical environment of this forest, we also present modeled mixing ratio profiles of biogenic hydrocarbons, hydrogen oxides and reactive nitrogen. The vertical profiles of these species demonstrate a range of structures and gradients that reflect the interplay of physical and chemical processes within the forest canopy, which can influence net exchange.


2010 ◽  
Vol 10 (9) ◽  
pp. 21791-21866
Author(s):  
G. M. Wolfe ◽  
J. A. Thornton ◽  
N. C. Bouvier-Brown ◽  
A. H. Goldstein ◽  
J.-H. Park ◽  
...  

Abstract. In a companion paper, we have introduced the Chemistry of Atmosphere-Forest Exchange (CAFE) model, a vertically-resolved 1-D chemical transport model designed to probe the details of near-surface reactive gas exchange. Here, we use CAFE to interpret noontime observations from the 2007 phase of the Biosphere Effects on Aerosols and Photochemistry Experiment (BEARPEX-2007), conducted at a young Ponderosa pine plantation in the western Sierra Nevada. The model reproduces many features of the BEARPEX-2007 data and offers new insights into the forest-atmosphere exchange of reactive molecules at this location. Nitrogen oxide (NOx = NO + NO2) fluxes are driven by soil emissions of NO, while the partitioning between NO and NO2 fluxes is sensitive to in-canopy photochemical gradients. Enhanced thermolysis at the ground increases downward acyl peroxy nitrate (APN) fluxes by as much as 50%, in general agreement with previous findings. APN fluxes are also influenced by in-canopy chemical production, especially when their formation is tied closely to oxidation of BVOC emissions. Gross dry N deposition is typically dominated by nitric acid, though other reactive nitrogen (NOy) species can comprise up to 28% of the N deposition budget under cooler conditions. Upward NO2 fluxes cause the net above-canopy NOy flux to be ~30% lower than the gross depositional flux. Model-measurement comparison of hydrogen peroxide mixing ratios suggests this molecule deposits at the aerodynamic limit. CAFE under-predicts ozone fluxes by ~20%, which may indicate additional in-canopy chemical losses that are missing from the current model.


2013 ◽  
Vol 6 (1) ◽  
pp. 1173-1222 ◽  
Author(s):  
K. M. Longo ◽  
S. R. Freitas ◽  
M. Pirre ◽  
V. Marécal ◽  
L. F. Rodrigues ◽  
...  

Abstract. The Coupled Chemistry Aerosol-Tracer Transport model to the Brazilian developments on the Regional Atmospheric Modeling System (CCATT–BRAMS, version 4.5) is an online regional chemical transport model designed for local and regional studies of atmospheric chemistry from surface to the lower stratosphere suitable both for operational and research purposes. It includes gaseous/aqueous chemistry, photochemistry, scavenging and dry deposition. The CCATT–BRAMS model takes advantages of the BRAMS specific development for the tropics/subtropics and of the recent availability of preprocessing tools for chemical mechanisms and of fast codes for photolysis rates. BRAMS includes state-of-the-art physical parameterizations and dynamic formulations to simulate atmospheric circulations of scales down to meters. The online coupling between meteorology and chemistry allows the system to be used for simultaneous atmospheric weather and chemical composition forecasts as well as potential feedbacks between them. The entire system comprises three preprocessing software tools for chemical mechanism (which are user defined), aerosol and trace gases emission fields and atmospheric and chemistry fields for initial and boundary conditions. In this paper, the model description is provided along evaluations performed using observational data obtained from ground-based stations, instruments aboard of aircrafts and retrieval from space remote sensing. The evaluation takes into account model application on different scales from megacities and Amazon Basin up to intercontinental region of the Southern Hemisphere.


2016 ◽  
Author(s):  
Sarah A. Monks ◽  
Stephen R. Arnold ◽  
Michael J. Hollaway ◽  
Richard J. Pope ◽  
Chris Wilson ◽  
...  

Abstract. The TOMCAT 3-D chemical transport model has been updated with the emissions and chemical degradation of ethene, propene, toluene, butane and monoterpenes. The full tropospheric chemical mechanism is described and the model is evaluated against a range of surface, balloon, aircraft and satellite measurements. The model is generally able to capture the main spatial and seasonal features of high and low concentrations of carbon monoxide (CO), ozone (O3), volatile organic compounds (VOCs) and reactive nitrogen. However, model biases are found, some of which are common to chemistry models and some that are specific to TOMCAT and warrant further investigation. Simulated O3 is found to generally lie within the range of ozonesonde observations and shows good agreement with surface sites. The most notable exceptions to this are during winter at high latitudes, when O3 is underestimated, and during summer over North America, when O3 is overestimated. Global Ozone Monitoring Experiment-2 (GOME-2) comparisons suggest that TOMCAT sub-column tropospheric O3 in DJF may also be underestimated outside of the Arctic, particularly near tropical regions. TOMCAT CO is negatively biased during winter and spring in the Northern Hemisphere (NH) when compared to ground-based observations and MOPITT (Measurements Of Pollution In The Troposphere) satellite data. In contrast, CO is positively biased throughout the year in the Southern Hemisphere (SH). The negative bias in the NH is a common feature in chemistry models and TOMCAT lies well within the range of biases found in other models, while the TOMCAT SH positive bias is at the upper range of positive biases reported in other models. Using two simulations with different boundary conditions highlighted the sensitivity of model performance to the chosen emission dataset when simulating VOCs, nitrogen oxides (NOx) and peroxyacetyl nitrate (PAN). VOC measurements show winter/spring negative biases in C2-C3 alkanes and alkenes, which is likely driven by underestimated anthropogenic emissions. TOMCAT is able to capture the seasonal minima and maxima of PAN and HNO3. However, comparisons to an aircraft climatology show that PAN may be overestimated in winter and HNO3 may be overestimated in winter and spring in regions over North America. The model showed different biases in NOx, depending on location, with evidence of underestimated Asian emissions contributing to negative model biases over China and underestimated fire emissions contributing to negative biases in the SH. TOMCAT global mean tropospheric hydroxyl radical (OH) concentrations are higher than estimates inferred from observations of methyl chloroform, but similar to, or lower than, multi-model mean concentrations reported in recent model intercomparison studies. TOMCAT shows peak OH concentrations in the tropical lower troposphere, unlike other models, which show peak concentrations in the tropical upper troposphere. This is likely to affect the lifetime and transport of important trace gases and warrants further investigation.


1999 ◽  
Vol 104 (D9) ◽  
pp. 11755-11781 ◽  
Author(s):  
Eugene V. Rozanov ◽  
Vladimir A. Zubov ◽  
Michael E. Schlesinger ◽  
Fanglin Yang ◽  
Natalia G. Andronova

2015 ◽  
Vol 15 (12) ◽  
pp. 17251-17281 ◽  
Author(s):  
J. Xu ◽  
R. V. Martin ◽  
A. van Donkelaar ◽  
J. Kim ◽  
M. Choi ◽  
...  

Abstract. We determine and interpret fine particulate matter (PM2.5) concentrations in East China for January to December 2013 at a horizontal resolution of 6 km from aerosol optical depth (AOD) retrieved from the Korean Geostationary Ocean Color Imager (GOCI) satellite instrument. We implement a set of filters to minimize cloud contamination in GOCI AOD. Evaluation of filtered GOCI AOD with AOD from the Aerosol Robotic Network (AERONET) indicates significant agreement with mean fractional bias (MFB) in Beijing of 6.7 % and northern Taiwan of −1.2 %. We use a global chemical transport model (GEOS-Chem) to relate the total column AOD to the near-surface PM2.5. The simulated PM2.5/AOD ratio exhibits high consistency with ground-based measurements (MFB = −0.52–8.0 %). We evaluate the satellite-derived PM2.5 vs. the ground-level PM2.5 in 2013 measured by the China Environmental Monitoring Center. Significant agreement is found between GOCI-derived PM2.5 and in-situ observations in both annual averages (r = 0.81, N = 494) and monthly averages (MFB = 13.1 %), indicating GOCI provides valuable data for air quality studies in Northeast Asia. The GEOS-Chem simulated chemical speciation of GOCI-derived PM2.5 reveals that secondary inorganics (SO42−, NO3−, NH4+) and organic matter are the most significant components. Biofuel emissions in northern China for heating are responsible for an increase in the concentration of organic matter in winter. The population-weighted GOCI-derived PM2.5 over East China for 2013 is 53.8 μg m−3, threatening the health and life expectancy of its 600 million residents.


2011 ◽  
Vol 11 (4) ◽  
pp. 13099-13139 ◽  
Author(s):  
G. González Abad ◽  
N. D. C. Allen ◽  
P. F. Bernath ◽  
C. D. Boone ◽  
S. D. McLeod ◽  
...  

Abstract. Near global upper tropospheric concentrations of carbon monoxide (CO), ethane (C2H6) and ethyne (C2H2) from ACE (Atmospheric Chemistry Experiment) Fourier transform spectrometer on board the Canadian satellite SCISAT-1 are presented and compared with the output from the Chemical Transport Model (CTM) GEOS-Chem. The retrievals of ethane and ethyne from ACE have been improved for this paper by using new sets of microwindows compared with those for previous versions of ACE data. With the improved ethyne retrieval we have been able to produce a near global upper tropospheric distribution of C2H2 from space. Carbon monoxide, ethane and ethyne concentrations retrieved using ACE spectra show the expected seasonality linked to variations in the anthropogenic emissions and destruction rates as well as seasonal biomass burning activity. The GEOS-Chem model was run using the dicarbonyl chemistry suite, an extended chemical mechanism in which ethyne is treated explicitly. Seasonal cycles observed from satellite data are well reproduced by the model output, however the simulated CO concentrations are found to be systematically biased low over the Northern Hemisphere. An average negative global mean bias of 12% and 7% of the model relative to the satellite observations has been found for CO and C2H6 respectively and a positive global mean bias of 1% has been found for C2H2. ACE data are compared for validation purposes with MkIV spectrometer data and Global Tropospheric Experiment (GTE) TRACE-A campaign data showing good agreement with all of them.


2008 ◽  
Vol 8 (5) ◽  
pp. 16981-17036 ◽  
Author(s):  
T. Stavrakou ◽  
J.-F. Müller ◽  
I. De Smedt ◽  
M. Van Roozendael ◽  
G. R. van der Werf ◽  
...  

Abstract. A new one-decade dataset of formaldehyde (HCHO) columns retrieved from GOME and SCIAMACHY is compared with HCHO columns simulated by an updated version of the IMAGES global chemical transport model. This model version includes an optimized chemical scheme with respect to HCHO production, where the short-term and final HCHO yields from pyrogenically emitted non-methane volatile organic compounds (NMVOCs) are estimated from the Master Chemical Mechanism (MCM) and an explicit speciation profile of pyrogenic emissions. The model is driven by the Global Fire Emissions Database (GFED) version 1 or 2 for biomass burning, whereas biogenic emissions are provided either by the Global Emissions Inventory Activity (GEIA), or by a newly developed inventory based on the Model of Emissions of Gases and Aerosols from Nature (MEGAN) algorithms driven by meteorological fields from the European Centre for Medium-Range Weather Forecasts (ECMWF). The comparisons focus on tropical ecosystems, North America and China, which experience strong biogenic and biomass burning NMVOC emissions reflected in the enhanced measured HCHO columns. These comparisons aim at testing the ability of the model to reproduce the observed features of the HCHO distribution on the global scale and at providing a first assessment of the performance of the current emission inventories. The high correlation coefficients (r>0.8) between the observed and simulated columns over most regions indicate a very good consistency between the model, the implemented inventories and the HCHO dataset. The use of the MEGAN-ECMWF inventory improves the model/data agreement in almost all regions, but biases persist over parts of Africa and the Northern Australia. Although neither GFED version is consistent with the data over all regions, a better match is achieved over Indonesia and Southern Africa when GFEDv2 is used, but GFEDv1 succeeds better in getting the correct seasonal patterns and intensities of the fire episodes over the Amazon basin, as reflected by the higher correlations calculated in this region.


2012 ◽  
Vol 5 (6) ◽  
pp. 1531-1542 ◽  
Author(s):  
L. K. Emmons ◽  
P. G. Hess ◽  
J.-F. Lamarque ◽  
G. G. Pfister

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.


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