ALBERT

Description: A natural emissions inventory for the continental United States and surrounding territories is needed in order to use the US Environmental Protection Agency Community Multiscale Air Quality (CMAQ) Model for simulating natural air quality. The CMAQ air modeling system (including the Sparse Matrix Operator Kernel Emissions (SMOKE) emissions processing system) currently estimates non-methane volatile organic compound (NMVOC) emissions from biogenic sources, nitrogen oxide (NOx) emissions from soils, ammonia from animals, several types of particulate and reactive gas emissions from fires, as well as sea salt emissions. However, there are several emission categories that are not commonly treated by the standard CMAQ Model system. Most notable among these are nitrogen oxide emissions from lightning, reduced sulfur emissions from oceans, geothermal features and other continental sources, windblown dust particulate, and reactive chlorine gas emissions linked with sea salt chloride. A review of past emissions modeling work and existing global emissions data bases provides information and data necessary for preparing a more complete natural emissions data base for CMAQ applications. A model-ready natural emissions data base is developed to complement the anthropogenic emissions inventory used by the VISTAS Regional Planning Organization in its work analyzing regional haze based on the year 2002. This new data base covers a modeling domain that includes the continental United States plus large portions of Canada, Mexico and surrounding oceans. Comparing July 2002 source data reveals that natural emissions account for 16% of total gaseous sulfur (sulfur dioxide, dimethylsulfide and hydrogen sulfide), 44% of total NOx, 80% of reactive carbonaceous gases (NMVOCs and carbon monoxide), 28% of ammonia, 96% of total chlorine (hydrochloric acid, nitryl chloride and sea salt chloride), and 84% of fine particles (i.e., those smaller than 2.5 μm in size) released into the atmosphere. The seasonality and relative importance of the various natural emissions categories are described.

Description: Sulfur aerosols impact human health, ecosystems, agriculture, and global and regional climate. A new annual estimate of anthropogenic global and regional sulfur dioxide emissions has been constructed spanning the period 1850–2005 using a bottom-up mass balance method, calibrated to country-level inventory data. Global emissions peaked in the early 1970s and decreased until 2000, with an increase in recent years due to increased emissions in China, international shipping, and developing countries in general. An uncertainty analysis was conducted including both random and systemic uncertainties. The overall global uncertainty in sulfur dioxide emissions is relatively small, but regional uncertainties ranged up to 30%. The largest contributors to uncertainty at present are emissions from China and international shipping. Emissions were distributed on a 0.5° grid by sector for use in coordinated climate model experiments.

Description: The calibration of field instruments used to measure concentrations of OH and HO2 worldwide have traditionally relied on a single method utilising the photolysis of water vapour in air in a flow tube at atmospheric pressure. Here the calibration of two FAGE (Fluorescence Assay by Gaseous Expansion) apparatuses designed for HOx (OH and HO2) measurements have been investigated as a function of external pressure and temperature, using two different laser systems. The conventional method of generating known concentrations of HOx from H2O vapour photolysis in a turbulent flowtube impinging just outside the FAGE sample inlet has been used to study instrument sensitivity as a function of internal fluorescence cell pressure (1.8–3.8 mbar). An increase in the calibration constants COH and CHO2 with pressure was observed and an empirical linear regression of the data was used to describe the trends, with ΔCOH = (17 ± 11)% and ΔCHO2 = (31.6 ± 4.4)% increase per mbar air (uncertainties quoted to 2σ). Presented here are the first direct measurements of the FAGE calibration constants as a function of external pressure (440–1000 mbar) in a controlled environment using the University of Leeds HIRAC chamber (Highly Instrumented Reactor for Atmospheric Chemistry). Two methods were used: the temporal decay of hydrocarbons for calibration of OH, and the kinetics of the second-order recombination of HO2 for HO2 calibrations. Over comparable conditions for the FAGE cell, the two alternative methods are in good agreement with the conventional method, with the average ratio of calibration factors (conventional : alternative) across the entire pressure range COH(conv)/COH(alt) = 1.19 ± 0.26 and CHO2(conv)/CHO2(alt) = 0.96 ± 0.18 (2σ). These alternative calibration methods currently have comparable systematic uncertainties than the conventional method: ~28% and ~41% for the alternative OH and HO2 calibration methods respectively compared to 35% for the H2O vapour photolysis method; ways in which these can be reduced in the future are discussed. The good agreement between the very different methods of calibration leads to increased confidence in HOx field measurements and particularly in aircraft based HOx measurements, where there are substantial variations in external pressure, and assumptions are made regarding loss rates on inlets as a function of pressure.

Description: We present and discuss a new dataset of gridded emissions covering the historical period (1850–2000) in decadal increments at a horizontal resolution of 0.5° in latitude and longitude. The primary purpose of this inventory is to provide consistent gridded emissions of reactive gases and aerosols for use in chemistry model simulations needed by climate models for the Climate Model Intercomparison Program #5 (CMIP5) in support of the Intergovernmental Panel on Climate Change (IPCC) Fifth Assessment report (AR5). Our best estimate for the year 2000 inventory represents a combination of existing regional and global inventories to capture the best information available at this point; 40 regions and 12 sectors are used to combine the various sources. The historical reconstruction of each emitted compound, for each region and sector, is then forced to agree with our 2000 estimate, ensuring continuity between past and 2000 emissions. Simulations from two chemistry-climate models are used to test the ability of the emission dataset described here to capture long-term changes in atmospheric ozone, carbon monoxide and aerosol distributions. The simulated long-term change in the Northern mid-latitudes surface and mid-troposphere ozone is not quite as rapid as observed. However, stations outside this latitude band show much better agreement in both present-day and long-term trend. The model simulations indicate that the concentration of carbon monoxide is underestimated at the Mace Head station; however, the long-term trend over the limited observational period seems to be reasonably well captured. The simulated sulfate and black carbon deposition over Greenland is in very good agreement with the ice-core observations spanning the simulation period. Finally, aerosol optical depth and additional aerosol diagnostics are shown to be in good agreement with previously published estimates and observations.

Description: The REgents PARk and Tower Environmental Experiment (REPARTEE) comprised two campaigns in London in October 2006 and October/November 2007. The experiment design involved measurements at a heavily trafficked roadside site, two urban background sites and an elevated site at 160–190 m above ground on the BT Tower, supplemented in the second campaign by Doppler lidar measurements of atmospheric vertical structure. A wide range of measurements of airborne particle physical metrics and chemical composition were made as well as measurements of a considerable range of gas phase species and the fluxes of both particulate and gas phase substances. Significant findings include (a) demonstration of the evaporation of traffic-generated nanoparticles during both horizontal and vertical atmospheric transport; (b) generation of a large base of information on the fluxes of nanoparticles, accumulation mode particles and specific chemical components of the aerosol and a range of gas phase species, as well as the elucidation of key processes and comparison with emissions inventories; (c) quantification of vertical gradients in selected aerosol and trace gas species which has demonstrated the important role of regional transport in influencing concentrations of sulphate, nitrate and secondary organic compounds within the atmosphere of London; (d) generation of new data on the atmospheric structure and turbulence above London, including the estimation of mixed layer depths; (e) provision of new data on trace gas dispersion in the urban atmosphere through the release of purposeful tracers; (f) the determination of spatial differences in aerosol particle size distributions and their interpretation in terms of sources and physico-chemical transformations; (g) studies of the nocturnal oxidation of nitrogen oxides and of the diurnal behaviour of nitrate aerosol in the urban atmosphere, and (h) new information on the chemical composition and source apportionment of particulate matter size fractions in the atmosphere of London derived both from bulk chemical analysis and aerosol mass spectrometry with two instrument types.

Description: A natural emissions inventory for the continental United States and surrounding territories is needed in order to use the US Environmental Protection Agency Community Multiscale Air Quality (CMAQ) Model for simulating natural air quality. The CMAQ air modeling system (including the Sparse Matrix Operator Kernel Emissions (SMOKE) emissions processing system) currently estimates volatile organic compound (VOC) emissions from biogenic sources, nitrogen oxide (NOx) emissions from soils, ammonia from animals, several types of particulate and reactive gas emissions from fires, as well as windblown dust and sea salt emissions. However, there are several emission categories that are not commonly treated by the standard CMAQ Model system. Most notable among these are nitrogen oxide emissions from lightning, reduced sulfur emissions from oceans, geothermal features and other continental sources, and reactive chlorine gas emissions linked with sea salt chloride. A review of past emissions modeling work and existing global emissions data bases provides information and data necessary for preparing a more complete natural emissions data base for CMAQ applications. A model-ready natural emissions data base is developed to complement the anthropogenic emissions inventory used by the VISTAS Regional Planning Organization in its work analyzing regional haze based on the year 2002. This new data base covers a modeling domain that includes the continental United States plus large portions of Canada, Mexico and surrounding oceans. Comparing July 2002 source data reveals that natural emissions account for 16% of total gaseous sulfur (sulfur dioxide, dimethylsulfide and hydrogen sulfide), 44% of total NOx, 80% of reactive carbonaceous gases (VOCs and carbon monoxide), 28% of ammonia, 96% of total chlorine (hydrochloric acid, nitryl chloride and sea salt chloride), and 84% of fine particles (i.e., those smaller than 2.5 μm in size) released into the atmosphere. The seasonality and relative importance of the various natural emissions categories are described.

Description: We examine past and future carbon emissions from global croplands, considering land-use change, changes in crop productivity, tillage practices, and residue removal. We find that emissions over the historical period are sensitive to the assumed productivity of arable land that is not planted in a given year and the assumed fraction of soil carbon that is released during land conversion. The role of this "other" arable land, both at present and over the historical period, is not well understood and should be examined further. The carbon balance of croplands over 21st century depends on changes in management practices, particularly the adoption of conservation tillage and the potential removal of residue for use as energy feedstocks. We find that croplands will not become large carbon sinks in the future, however, unless most crop residue is left on fields. Given the relatively low carbon "penalty" incurred by removal, residue use for energy feedstocks may be the preferred option.

Description: We examine historical and future land-use emissions using a simple mechanistic carbon-cycle model with regional and ecosystem specific parameterizations. Our central estimate of net terrestrial land-use change emissions, exclusive of climate feedbacks, is 250 Gt C over the last three hundred years. This estimate is most sensitive to assumptions for pre-industrial forest and soil carbon densities. We also find that estimates are sensitive to the treatment of crop and pasture lands. These sensitivities also translate into differences in future terrestrial uptake in the RCP4.5 land-use scenario. This estimate of future uptake is lower than the native values from the GCAM integrated assessment model result due to lower net reforestation in the RCP4.5 gridded land-use data product.

Description: Carbonaceous and sulfur aerosols have a substantial global and regional influence on climate, resulting in a net cooling to date, in addition to their impact on health and ecosystems. The magnitude of this influence has changed substantially over the past and is expected to continue to change into the future. An integrated picture of the changing climatic influence of black carbon, organic carbon and sulfate over the period 1850 through 2100, focusing on uncertainty, is presented using updated historical inventories and a coordinated set of emission projections. We describe, in detail, the aerosol emissions from the Representative Concentration Pathway (RCP) 4.5 scenario and its associated reference scenario. While aerosols have had a substantial impact on climate over the past century, we show that, by the end of the 21st century aerosols will likely be only a minor contributor to radiative forcing due to increases in greenhouse gas forcing and a net global decrease in pollutant emissions. This outcome is even more certain under a successful implementation of a policy to limit greenhouse gas emissions as low-carbon energy technologies that do not emit appreciable aerosol or SO2 are deployed.