Abstract. The Model for Ozone and Related chemical Tracers, version 4 (MOZART-4) is an offline global chemical transport model particularly suited for studies of the troposphere. The updates of the model from its previous version MOZART-2 are described, including an expansion of the chemical mechanism to include more detailed hydrocarbon chemistry and bulk aerosols. Online calculations of a number of processes, such as dry deposition, emissions of isoprene and monoterpenes and photolysis frequencies, are now included. Results from an eight-year simulation (2000)(2001)(2002)(2003)(2004)(2005)(2006)(2007) are presented and evaluated. The MOZART-4 source code and standard input files are available for download from the NCAR Community Data Portal (http://cdp.ucar.edu).
Abstract. The Fire INventory from NCAR version 1.0 (FINNv1) provides daily, 1 km resolution, global estimates of the trace gas and particle emissions from open burning of biomass, which includes wildfire, agricultural fires, and prescribed burning and does not include biofuel use and trash burning. Emission factors used in the calculations have been updated with recent data, particularly for the non-methane organic compounds (NMOC). The resulting global annual NMOC emission estimates are as much as a factor of 5 greater than some prior estimates. Chemical speciation profiles, necessary to allocate the total NMOC emission estimates to lumped species for use by chemical transport models, are provided for three widely used chemical mechanisms: SAPRC99, GEOS-CHEM, and MOZART-4. Using these profiles, FINNv1 also provides global estimates of key organic compounds, including formaldehyde and methanol. Uncertainties in the emissions estimates arise from several of the method steps. The use of fire hot spots, assumed area burned, land cover maps, biomass consumption estimates, and emission factors all introduce error into the model estimates. The uncertainty in the FINNv1 emission estimates are about a factor of two; but, the global estimates agree reasonably well with other global inventories of biomass burning emissions for CO, CO 2 , and other species with less variable emission factors. FINNv1 emission estimates have been developed specifically for modeling atmospheric chemistry and air quality in a consistent framework at scales from local to global. The product is unique because of the high temporalCorrespondence to: C. Wiedinmyer (christin@ucar.edu) and spatial resolution, global coverage, and the number of species estimated. FINNv1 can be used for both hindcast and forecast or near-real time model applications and the results are being critically evaluated with models and observations whenever possible.
[1] We have developed a global three-dimensional chemical transport model called Model of Ozone and Related Chemical Tracers (MOZART), version 2. This model, which will be made available to the community, is built on the framework of the National Center for Atmospheric Research (NCAR) Model of Atmospheric Transport and Chemistry (MATCH) and can easily be driven with various meteorological inputs and model resolutions. In this work, we describe the standard configuration of the model, in which the model is driven by meteorological inputs every 3 hours from the middle atmosphere version of the NCAR Community Climate Model (MACCM3) and uses a 20-min time step and a horizontal resolution of 2.8°latitude  2.8°longitude with 34 vertical levels extending up to approximately 40 km. The model includes a detailed chemistry scheme for tropospheric ozone, nitrogen oxides, and hydrocarbon chemistry, with 63 chemical species. Tracer advection is performed using a flux-form semi-Lagrangian scheme with a pressure fixer. Subgrid-scale convective and boundary layer parameterizations are included in the model. Surface emissions include sources from fossil fuel combustion, biofuel and biomass burning, biogenic and soil emissions, and oceanic emissions. Parameterizations of dry and wet deposition are included. Stratospheric concentrations of several long-lived species (including ozone) are constrained by relaxation toward climatological values. The distribution of tropospheric ozone is well simulated in the model, including seasonality and horizontal and vertical gradients. However, the model tends to overestimate ozone near the tropopause at high northern latitudes. Concentrations of nitrogen oxides (NO x ) and nitric acid (HNO 3 ) agree well with observed values, but peroxyacetylnitrate (PAN) is overestimated by the model in the upper troposphere at several locations. Carbon monoxide (CO) is simulated well at most locations, but the seasonal cycle is underestimated at some sites in the Northern Hemisphere. We find that in situ photochemical production and loss dominate the tropospheric ozone budget, over input from the stratosphere and dry deposition. Approximately 75% of the tropospheric production and loss of ozone occurs within the tropics, with large net production in the tropical upper troposphere. Tropospheric production and loss of ozone are three to four times greater in the northern extratropics than the southern extratropics. The global sources of CO consist of photochemical production (55%) and direct emissions (45%). The tropics dominate the chemistry of CO, accounting for about 75% of the tropospheric production and loss. The global budgets of tropospheric ozone and CO are generally consistent with the range found in recent studies. The lifetime of methane (9.5 years) and methylchloroform (5.7 years) versus oxidation by tropospheric hydroxyl radical (OH), two useful measures of the global abundance of OH, agree well with recent estimates. Concentrations of nonmethane hydrocarbons and oxygenated intermediates (carbony...
We discuss and evaluate the representation of atmospheric chemistry in the global Community Atmosphere Model (CAM) version 4, the atmospheric component of the Community Earth System Model (CESM). We present a variety of configurations for the representation of tropospheric and stratospheric chemistry, wet removal, and online and offline meteorology. Results from simulations illustrating these configurations are compared with surface, aircraft and satellite observations. Major biases include a negative bias in the high-latitude CO distribution, a positive bias in upper-tropospheric/lower-stratospheric ozone, and a positive bias in summertime surface ozone (over the United States and Europe). The tropospheric net chemical ozone production varies significantly between configurations, partly related to variations in stratosphere-troposphere exchange. Aerosol optical depth tends to be underestimated over most regions, while comparison with aerosol surface measurements over the United States indicate reasonable results for sulfate , especially in the online simulation. Other aerosol species exhibit significant biases. Overall, the model-data comparison indicates that the offline simulation driven by GEOS5 meteorological analyses provides the best simulation, possibly due in part to the increased vertical resolution (52 levels instead of 26 for online dynamics). The CAM-chem code as described in this paper, along with all the necessary datasets needed to perform the simulations described here, are available for download at <a href="http://www.cesm.ucar.edu">www.cesm.ucar.edu</a>
Organic peroxy radicals (often abbreviated RO(2)) play a central role in the chemistry of the Earth's lower atmosphere. Formed in the atmospheric oxidation of essentially every organic species emitted, their chemistry is part of the radical cycles that control the oxidative capacity of the atmosphere and lead to the formation of ozone, organic nitrates, organic acids, particulate matter and other so-called secondary pollutants. In this review, laboratory studies of this peroxy radical chemistry are detailed, as they pertain to the chemistry of the atmosphere. First, a brief discussion of methods used to detect the peroxy radicals in the laboratory is presented. Then, the basic reaction pathways - involving RO(2) unimolecular reactions and bimolecular reactions with atmospheric constituents such as NO, NO(2), NO(3), O(3), halogen oxides, HO(2), and other RO(2) species - are discussed. For each of these reaction pathways, basic reaction rates are presented, along with trends in reactivity with radical structure. Focus is placed on recent advances in detection methods and on recent advances in our understanding of radical cycling processes, particularly pertaining to the complex chemistry associated with the atmospheric oxidation of biogenic hydrocarbons.
[1] The Model for Ozone and Related Chemical Tracers, version 3 (MOZART-3), which represents the chemical and physical processes from the troposphere through the lower mesosphere, was used to evaluate the representation of long-lived tracers and ozone using three different meteorological fields. The meteorological fields are based on (1) the Whole Atmosphere Community Climate Model, version 1b (WACCM1b), (2) the European Centre for Medium-Range Weather Forecasts (ECMWF) operational analysis, and (3) a new reanalysis for year 2000 from ECMWF called EXP471. Model-derived tracers (methane, water vapor, and total inorganic nitrogen) and ozone are compared to data climatologies from satellites. Model mean age of air was also derived and compared to in situ CO 2 and SF 6 data. A detailed analysis of the chemical fields simulated by shows that even though the general features characterizing the three dynamical sets are rather similar, slight differences in winds and temperature can produce substantial differences in the calculated distributions of chemical tracers. The MOZART-3 simulations that use meteorological fields from WACCM1b and ECMWF EXP471 represented best the distribution of long-lived tracers and mean age of air in the stratosphere. There was a significant improvement using the ECMWF EXP471 reanalysis data product over the ECMWF operational data product. The effect of the quasi-biennial oscillation circulation on long-lived tracers and ozone is examined.
1. Scope -is the work directly or implicitly related to atmospheric composition? 2. Novelty -does the work provide a) a general and/or broader relevance (e.g. not a pure local study), b) new results or methods, and c) does it add significantly to the knowledge of atmospheric composition and its impacts?3. Quality -does the work contain high quality a) atmospheric observations, b) process studies, c) modeling exercises or d) data analysis?Will your paper be within the scope of Atmospheric Environment?We try to be flexible with novel scientific articles on issues of atmospheric composition even, if they are not directly related to atmospheric measurements (e.g. wind tunnel studies, dynamometer studies, remote sensing retrieval, etc). However, we are still cautious of purely mathematical derivations, preliminary results or insignificant case and local studies. The authors should make sure that the articles contain substantial contributions to the science of atmospheric composition before sending them for review.
The absorption spectrum of O2 and O2‐O2 collision pairs were measured over the wavelength range from 330 to 1140 nm using pressures of O2 from 1 to 55 atm at 298 K. Absorption cross sections, pressure dependences, band centers, and full widths at half maximum of the observed absorption bands centered at 343.4, 360.5, 380.2, 446.7, 477.3, 532.2, 577.2, 630.0, 688, 762, and 1065.2 nm are reported. The absorption bands centered at 360.5, 380.2, and 477.3 nm were also measured at 196 K and their temperature dependences were characterized.
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