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  • 1
    Publication Date: 2011-10-31
    Description: Presently only limited sets of tropospheric ammonia (NH3) measurements in the Earth's atmosphere have been reported from satellite and surface station measurements, despite the well-documented negative impact of NH3 on the environment and human health. Presented here is a detailed description of the satellite retrieval strategy and analysis for the Tropospheric Emission Spectrometer (TES) using simulations and measurements. These results show that: (i) the level of detectability for a representative boundary layer TES NH3 mixing ratio value is ~0.4 ppbv, which typically corresponds to a profile that contains a maximum level value of ~1 ppbv; (ii) TES NH3 retrievals generally provide at most one degree of freedom for signal (DOFS), with peak sensitivity between 700 and 900 mbar; (iii) TES NH3 retrievals show significant spatial and seasonal variability of NH3 globally; (iv) initial comparisons of TES observations with GEOS-CHEM estimates show TES values being higher overall. Important differences and similarities between modeled and observed seasonal and spatial trends are noted, with discrepancies indicating areas where the timing and magnitude of modeled NH3 emissions from agricultural sources, and to lesser extent biomass burning sources, need further study.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 2
    Publication Date: 2013-01-23
    Description: The Community Multiscale Air Quality (CMAQ) model version 4.7.1 was used to simulate mercury wet and dry deposition for a domain covering the continental United States (US). The simulations used MM5-derived meteorological input fields and the US Environmental Protection Agency (EPA) Clear Air Mercury Rule (CAMR) emissions inventory. Using sensitivity simulations with different boundary conditions and tracer simulations, this investigation focuses on the contributions of boundary concentrations to deposited mercury in the Southwest (SW) US. Concentrations of oxidized mercury species along the boundaries of the domain, in particular the upper layers of the domain, can make significant contributions to the simulated wet and dry deposition of mercury in the SW US. In order to better understand the contributions of boundary conditions to deposition, inert tracer simulations were conducted to quantify the relative amount of an atmospheric constituent transported across the boundaries of the domain at various altitudes and to quantify the amount that reaches and potentially deposits to the land surface in the SW US. Simulations using alternate sets of boundary concentrations, including estimates from global models (Goddard Earth Observing System-Chem (GEOS-Chem) and the Global/Regional Atmospheric Heavy Metals (GRAHM) model), and alternate meteorological input fields (for different years) are analyzed in this paper. CMAQ dry deposition in the SW US is sensitive to differences in the atmospheric dynamics and atmospheric mercury chemistry parameterizations between the global models used for boundary conditions.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 3
    Publication Date: 2011-05-26
    Description: Presently only limited sets of tropospheric ammonia (NH3) measurements in the Earth's atmosphere have been reported from satellite and surface station measurements, despite the well-documented negative impact of NH3 on the environment and human health. Presented here is a detailed description of the satellite retrieval strategy and analysis for the Tropospheric Emission Spectrometer (TES) using simulations and measurements. These results show that: (i) the level of detectability for a representative boundary layer TES NH3 mixing ratio value is ~0.3 ppbv, which typically corresponds to a profile that contains a maximum level value of ~1 ppbv; (ii) TES NH3 retrievals provide at most one degree of freedom for signal (DOFS), with peak sensitivity between 700 and 900 mbar; (iii) TES NH3 retrievals show significant spatial and seasonal variability of NH3 globally; (iv) Initial comparisons of TES observations with GEOS-CHEM estimates show TES values being higher overall. Important differences and similarities between modeled and observed seasonal and spatial trends are noted, with discrepancies indicating areas where the timing and magnitude of modeled NH3 emissions from agricultural sources, and to lesser extent biomass burning sources, need further study.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 4
    Publication Date: 2012-04-20
    Description: The Community Multiscale Air Quality (CMAQ) model version 4.7.1 was used to simulate mercury wet and dry deposition for a domain covering the contiguous United States (US). The simulations used MM5-derived meteorological input fields and the US Environmental Protection Agency (EPA) Clear Air Mercury Rule (CAMR) emissions inventory. Using sensitivity simulations with different boundary conditions and tracer simulations, this investigation focuses on the contributions of boundary concentrations to deposited mercury in the Southwest (SW) US. Concentrations of oxidized mercury species along the boundaries of the domain, in particular the upper layers of the domain, can make significant contributions to the simulated wet and dry deposition of mercury in the SW US. In order to better understand the contributions of boundary conditions to deposition, inert tracer simulations were conducted to quantify the relative amount of an atmospheric constituent transported across the boundaries of the domain at various altitudes and to quantify the amount that reaches and potentially deposits to the land surface in the SW US. Simulations using alternate sets of boundary concentrations, including estimates from global models (Goddard Earth Observing System-Chem (GEOS-Chem) and the Global/Regional Atmospheric Heavy Metals (GRAHM) model), and alternate meteorological input fields (for different years) are analyzed in this paper. CMAQ dry deposition in the SW US is sensitive to differences in the atmospheric dynamics and atmospheric mercury chemistry parameterizations between the global models used for boundary conditions.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 5
  • 6
  • 7
    Publication Date: 2012-08-23
    Description: Atmospheric ammonia (NH3) is the primary atmospheric base and an important precursor for inorganic particulate matter and when deposited NH3 contributes to surface water eutrophication, soil acidification and decline in species biodiversity. Flux measurements indicate that the air-surface exchange of NH3 is bi-directional. However, the effects of bi-directional exchange, soil biogeochemistry and human activity are not parameterized in air quality models. The US Environmental Protection Agency (EPA)'s Community Multiscale Air-Quality (CMAQ) model with bi-directional NH3 exchange has been coupled with the United States Department of Agriculture (USDA)'s Environmental Policy Integrated Climate (EPIC) agro-ecosystem model's nitrogen geochemistry algorithms. CMAQ with bi-directional NH3 exchange coupled to EPIC connects agricultural cropping management practices to emissions and atmospheric concentrations of reduced nitrogen and models the biogeochemical feedback on NH3 air-surface exchange. This coupled modeling system reduced the biases and error in NHx (NH3 + NH4+) wet deposition and in ambient aerosol concentrations in an annual 2002 Continental US (CONUS) domain simulation when compared to a 2002 annual simulation of CMAQ without bi-directional exchange. Fertilizer emissions estimated in CMAQ 5.0 with bi-directional exchange exhibits markedly different seasonal dynamics than the US EPA's National Emissions Inventory (NEI), with lower emissions in the spring and fall and higher emissions in July.
    Print ISSN: 1810-6277
    Electronic ISSN: 1810-6285
    Topics: Biology , Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 8
    Publication Date: 2013-03-21
    Description: Atmospheric ammonia (NH3) dominates global emissions of total reactive nitrogen (Nr), while emissions from agricultural production systems contribute about two thirds of global NH3 emissions; the remaining third emanates from oceans, natural vegetation, humans, wild animals and biomass burning. On land, NH3 emitted from the various sources eventually returns to the biosphere by dry deposition to sink areas, predominantly semi-natural vegetation, and by wet and dry deposition as ammonium (NH4+) to all surfaces. However, the land/atmosphere exchange of gaseous NH3 is in fact bi-directional over unfertilized as well as fertilized ecosystems, with periods and areas of emission and deposition alternating in time (diurnal, seasonal) and space (patchwork landscapes). The exchange is controlled by a range of environmental factors, including meteorology, surface layer turbulence, thermodynamics, air and surface heterogeneous-phase chemistry, canopy geometry, plant development stage, leaf age, organic matter decomposition, soil microbial turnover, and, in agricultural systems, by fertilizer application rate, fertilizer type, soil type, crop type, and agricultural management practices. We review the range of processes controlling NH3 emission and uptake in the different parts of the soil-canopy-atmosphere continuum, with NH3 emission potentials defined at the substrate and leaf levels by different [NH4+] / [H+] ratios (Γ). Surface/atmosphere exchange models for NH3 are necessary to compute the temporal and spatial patterns of emissions and deposition at the soil, plant, field, landscape, regional and global scales, in order to assess the multiple environmental impacts of air-borne and deposited NH3 and NH4+. Models of soil/vegetation/atmosphereem NH3 exchange are reviewed from the substrate and leaf scales to the global scale. They range from simple steady-state, "big leaf" canopy resistance models, to dynamic, multi-layer, multi-process, multi-chemical species schemes. Their level of complexity depends on their purpose, the spatial scale at which they are applied, the current level of parameterisation, and the availability of the input data they require. State-of-the-art solutions for determining the emission/sink Γ potentials through the soil/canopy system include coupled, interactive chemical transport models (CTM) and soil/ecosystem modelling at the regional scale. However, it remains a matter for debate to what extent realistic options for future regional and global models should be based on process-based mechanistic versus empirical and regression-type models. Further discussion is needed on the extent and timescale by which new approaches can be used, such as integration with ecosystem models and satellite observations.
    Print ISSN: 1810-6277
    Electronic ISSN: 1810-6285
    Topics: Biology , Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 9
    Publication Date: 2012-05-29
    Description: While nitrogen (N) is an essential element for life, human population growth and demands for energy, transportation and food can lead to excess nitrogen in the environment. A modeling framework is described and implemented, to promote a more integrated, process-based and system-level approach to the estimation of ammonia (NH3) emissions resulting from the application of inorganic nitrogen fertilizers to agricultural soils in the United States. The United States Department of Agriculture (USDA) Environmental Policy Integrated Climate (EPIC) model is used to simulate plant demand-driven fertilizer applications to commercial cropland throughout the continental US. This information is coupled with a process-based air quality model to produce continental-scale NH3 emission estimates. Regional cropland NH3 emissions are driven by the timing and amount of fertilizer applied, local meteorology, and ambient air concentrations. An evaluation of EPIC-simulated crop management activities associated with fertilizer application at planting compared with similar USDA state-level event estimates shows temporally progressive spatial patterns that agree well with one another. EPIC annual inorganic fertilizer application amounts also agree well with reported spatial patterns produced by others, but domain-wide the EPIC values are biased about 6 % low. Preliminary application of the integrated fertilizer application and air quality modeling system produces a modified geospatial pattern of seasonal NH3 emissions that improves current simulations of observed atmospheric nitrate concentrations. This modeling framework provides a more dynamic, flexible, and spatially and temporally resolved estimate of NH3 emissions than previous factor-based NH3 inventories, and will facilitate evaluation of alternative nitrogen and air quality policy and adaptation strategies associated with future climate and land use changes.
    Print ISSN: 1810-6277
    Electronic ISSN: 1810-6285
    Topics: Biology , Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 10
    Publication Date: 2012-06-28
    Description: Recent incorporation of coupled soil biogeochemical and bi-directional NH3 air-surface exchange algorithms into regional air quality models holds promise for further reducing uncertainty in estimates of NH3 emissions from fertilized soils. While this represents a significant advancement over previous approaches, the evaluation and improvement of such modeling systems for fertilized crops requires process level field measurements over extended periods of time that capture the range of soil, vegetation, and atmospheric conditions that drive short term (i.e., post fertilization) and total growing seasonNH3 fluxes. This study examines the processes of NH3 air-surface exchange in a fertilized corn (Zea mays) canopy over the majority of a growing season to characterize soil emissions after fertilization and investigate soil-canopy interactions. Micrometeorological flux measurements above the canopy, measurements of soil, leaf apoplast and dew/guttation chemistry, and a combination of in-canopy measurements, inverse source/sink, and resistance modeling were employed. Over a period of approximately 10 weeks following fertilization, daily mean and median net canopy-scale fluxes yielded cumulative total N losses of 8.4% and 6.1%, respectively, of the 134 kg N ha−1 surface applied to the soil as urea ammonium nitrate (UAN). During the first month after fertilization, daily mean emission fluxes were positively correlated with soil temperature and soil volumetric water. Diurnally, maximum hourly average fluxes of ≈700 ng N m−2 s−1 occurred near mid-day, coincident with the daily maximum in friction velocity. Net emission was still observed 5 to 10 weeks after fertilization, although mid-day peak fluxes had declined to ≈125 ng N m−2 s−1 A key finding of the surface chemistry measurements was the observation of high pH (7.0 – 8.5) in leaf dew/guttation, which reduced the ability of the canopy to recapture soil emissions during wet periods. In-canopy measurements near peak LAI indicated that the concentration of NH3 just above the soil surface was highly positively correlated with soil volumetric water, which likely reflects the influence of soil moisture on resistance to gaseous diffusion through the soil profile and hydrolysis of remaining urea. Inverse source/sink and resistance modeling indicated that the canopy recaptured ≈73% of soil emissions near peak LAI. Stomatal uptake may account for 12–34% of total uptake by foliage during the day compared to 66–88% deposited to the cuticle. Future process-level NH3 studies in fertilized cropping systems should focus on the temporal dynamics of net emission to the atmosphere from fertilization to peak LAI and improvement of soil and cuticular resistance parameterizations.
    Print ISSN: 1810-6277
    Electronic ISSN: 1810-6285
    Topics: Biology , Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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