122 research outputs found
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Regional Visibility Statistics in the United States: Natural and Transboundary Pollution Influences, and Implications for the Regional Haze Rule
The Regional Haze Rule of the US Environmental Protection Agency mandates reduction in US anthropogenic emissions to achieve linear improvement of visibility in wilderness areas over the 2004–18 period toward an endpoint of natural visibility conditions by 2064. Linear improvement is to apply to the mean visibility degradation on the statistically 20% worst days, measured as a Haze Index in units of deciviews (log of aerosol extinction). We use a global chemical transport model (GEOS-Chem) with 1°×1° horizontal resolution to simulate present-day visibility statistics in the USA, compare them to observations from the Interagency Monitoring of Protected Visual Environments (IMPROVE) surface network, and provide natural and background visibility statistics for application of the Regional Haze Rule. Background is defined by suppression of US anthropogenic emissions but allowance for present-day foreign emissions and associated import of pollution. Our model is highly successful at reproducing the observed variability of visibility statistics for present-day conditions, including the low tail of the frequency distribution that is most representative of natural or background conditions. We find considerable spatial and temporal variability in natural visibility over the USA, especially due to fires in the west. A major uncertainty in estimating natural visibility is the sensitivity of biogenic organic aerosol formation to the availability of preexisting anthropogenic aerosol. Background visibility is more variable than natural visibility and the 20% worst days show large contributions from Canadian and Mexican pollution. Asian pollution, while degrading mean background visibility, is relatively less important on the worst days. Recognizing the influence of uncontrollable transboundary pollution in the Regional Haze Rule would substantially decrease the schedule of emission reductions required in the 2004–18 implementation phase. Meaningful application of the Rule in the future will require projections of future trends in foreign anthropogenic emissions, wildfire frequency, and climate variablesEarth and Planetary SciencesEngineering and Applied Science
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The Role of the Ocean in the Global Atmospheric Budget of Acetone
[1] Acetone is one of the most abundant carbonyl compounds in the atmosphere and it plays an important role in atmospheric chemistry. The role of the ocean in the global atmospheric acetone budget is highly uncertain, with past studies reaching opposite conclusions as to whether the ocean is a source or sink. Here we use a global 3-D chemical transport model (GEOS-Chem) simulation of atmospheric acetone to evaluate the role of air-sea exchange in the global budget. Inclusion of updated (slower) photolysis loss in the model means that a large net ocean source is not needed to explain observed acetone in marine air. We find that a simulation with a fixed seawater acetone concentration of 15 nM based on observations can reproduce the observed global patterns of atmospheric concentrations and air-sea fluxes. The Northern Hemisphere oceans are a net sink for acetone while the tropical oceans are a net source. On a global scale the ocean is in near-equilibrium with the atmosphere. Prescribing an ocean concentration of acetone as a boundary condition in the model assumes that ocean concentrations are controlled by internal production and loss, rather than by air-sea exchange. An implication is that the ocean plays a major role in controlling atmospheric acetone. This hypothesis needs to be tested by better quantification of oceanic acetone sources and sinks.Engineering and Applied Science
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Regional CO Pollution in China Simulated by the High-Resolution Nested-Grid GEOS-Chem Model
An updated version of the nested-grid GEOS-Chem model is developed allowing for higher horizontal (0.5°×0.667°) and vertical resolution as compared to global models. CO transport over a heavily polluted region, the Beijing-Tianjin-Hebei (BTH) city cluster in China, and the pattern of outflow from East China in summertime are investigated. Comparison of the nested-grid with global models indicates that the fine-resolution nested-grid model is capable of resolving individual cities with high associated emission intensities. The nested-grid model indicates the presence of a high CO column density over the Sichuan Basin in summer, attributable to the low-level stationary vortex associated with the Basin's topographical features. The nested-grid model provides good agreement also with measurements from a suburban monitoring site in Beijing during summer 2005. Tagged CO simulation results suggest that regional emissions make significant contributions to elevated CO levels over Beijing on polluted days and that the southeastward moving cyclones bringing northwest winds to Beijing are the key meteorological mechanisms responsible for dispersion of pollution over Beijing in summer. Overall CO fluxes to the NW Pacific from Asia are found to decrease by a factor of 3–4 from spring to summer. Much of the seasonal change is driven by decreasing fluxes from India and Southeast Asia in summer, while fluxes from East China are only 30% lower in summer than in spring. Compared to spring, summertime outflow from Chinese source regions is strongest at higher latitudes (north of 35° N). The deeper convection in summer transporting CO to higher altitudes where export is more efficient is largely responsible for enhanced export in summer.Engineering and Applied Science
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Why Are There Large Differences Between Models in Global Budgets of Tropospheric Ozone?
Global 3-D tropospheric chemistry models in the literature show large differences in global budget terms for tropospheric ozone. The ozone production rate in the troposphere, P(O x ), varies from 2300 to 5300 Tg yr−1 across models describing the present-day atmosphere. The ensemble mean of P(O x ) in models from the post-2000 literature is 35% higher than that compiled in the Intergovernmental Panel on Climate Change (IPCC) Third Assessment Report (TAR). Simulations conducted with the GEOS-Chem model using two different assimilated meteorological data sets for 2001 (GEOS-3 and GEOS-4), as well as 3 years of GISS GCM meteorology, show P(O x ) values in the range 4250–4700 Tg yr−1; the differences appear mostly because of clouds. Examination of the evolution of P(O x ) over the GEOS-Chem model history shows major effects from changes in heterogeneous chemistry, the lightning NOx source, and the yield of organic nitrates from isoprene oxidation. Multivariate statistical analysis of model budgets in the literature indicates that 74% of the variance in P(O x ) across models can be explained by differences in NOx emissions, inclusion of nonmethane volatile organic compounds (NMVOCs, mostly biogenic isoprene), and ozone influx from stratosphere-troposphere exchange (STE). Higher NOx emissions, more widespread inclusion of NMVOC chemistry, and weaker STE in the more recent models increase ozone production; however, the effect of NMVOCs does not appear generally sensitive to the magnitude of emissions within the range typically used in models (500–900 Tg C yr−1). We find in GEOS-Chem that P(O x ) saturates when NMVOC emissions exceed 200 Tg C yr−1 because of formation of organic nitrates from isoprene oxidation, providing an important sink for NOx.Earth and Planetary SciencesEngineering and Applied Science
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Asian chemical outflow to the Pacific in spring: Origins, pathways, and budgets
We analyze the Asian outflow of CO, ozone, and nitrogen oxides (NOx) to the Pacific in spring by using the GEOS-CHEM global three-dimensional model of tropospheric chemistry and simulating the Pacific Exploratory Mission-West (PEM-West B) aircraft mission in February–March 1994. The GEOS-CHEM model uses assimilated meteorological fields from the NASA Goddard Earth Observing System (GEOS). It reproduces relatively well the main features of tropospheric ozone, CO, and reactive nitrogen species observed in PEM-West B, including latitudinal and vertical gradients of the Asian pollution outflow over the western Pacific although simulated concentrations of CO tend to be too low (possibly because biogenic sources are underestimated). We use CO as a long-lived tracer to diagnose the processes contributing to the outflow. The highest concentrations in the outflow are in the boundary layer (0–2 km), but the strongest outflow fluxes are in the lower free troposphere (2–5 km) and reflect episodic lifting of pollution over central and eastern China ahead of eastward moving cold fronts. This frontal lifting, followed by westerly transport in the lower free troposphere, is the principal process responsible for export of both anthropogenic and biomass burning pollution from Asia. Anthropogenic emissions from Europe and biomass burning emissions from Africa make also major contributions to the Asian outflow over the western Pacific; European sources dominate in the lower troposphere north of 40°N, while African sources are important in the upper troposphere at low latitudes. For the period of PEM-West B (February–March) we estimate that fossil fuel combustion and biomass burning make comparable contributions to the budgets of CO, ozone, and NOx. in the Asian outflow. We find that 13% of NOx emitted in Asia is exported as NOx or PAN, a smaller fraction than for the United States because of higher aerosol concentrations that promote heterogeneous conversion of NOx to HNO3. Production and export of ozone from Asia in spring is much greater than from the United States because of the higher photochemical activity.Engineering and Applied Science
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Sulfate Formation in Sea-Salt Aerosols: Constraints from Oxygen Isotopes
We use observations of the mass-independent oxygen isotopic composition (Δ17O) of sulfate in the marine boundary layer (MBL) to quantify the sulfate source from aqueous SO2 (S(IV)) oxidation by O3 in alkaline sea-salt aerosols. Oxidation by O3 imparts a large Δ17O signature to the resulting sulfate (8.8‰) relative to oxidation by H2O2 (0.9‰) or by OH or O2 (0‰). Ship data from two Indian Ocean Experiment (INDOEX) cruises in the Indian Ocean indicate Δ17O values usually 70%) and increases MBL sulfate concentrations by typically >10% (up to 30%). Globally, this mechanism contributes 9% of atmospheric sulfate production and 1% of the sulfate burden. The impact on H2SO4 (g) formation and implications for the potential formation of new particles in the MBL warrants inclusion in models examining the radiative effects of sulfate aerosols.Earth and Planetary SciencesEngineering and Applied Science
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An Improved Global Model for Air-Sea Exchange of Mercury: High Concentrations over the North Atlantic
We develop an improved treatment of the surface ocean in the GEOS-Chem global 3-D biogeochemical model for mercury (Hg). We replace the globally uniform subsurface ocean Hg concentrations used in the original model with basin-specific values based on measurements. Updated chemical mechanisms for Hg0/HgII redox reactions in the surface ocean include both photochemical and biological processes, and we improved the parametrization of particle-associated Hg scavenging. Modeled aqueous Hg concentrations are consistent with limited surface water observations. Results more accurately reproduce high-observed MBL concentrations over the North Atlantic (NA) and the associated seasonal trends. High seasonal evasion in the NA is driven by inputs from Hg enriched subsurface waters through entrainment and Ekman pumping. Globally, subsurface waters account for 40% of Hg inputs to the ocean mixed layer, and 60% is from atmospheric deposition. Although globally the ocean is a net sink for 3.8 Mmol Hg y−1, the NA is a net source to the atmosphere, potentially due to enrichment of subsurface waters with legacy Hg from historical anthropogenic sources.Engineering and Applied Science
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North American Pollution Outflow and the Trapping of Convectively Lifted Pollution by Upper-Level Anticyclone
We examine the major outflow pathways for North American pollution to the Atlantic in summer by conducting a 4-year simulation with the GEOS-CHEM global chemical transport model, including a coupled ozone-aerosol simulation with 1° × 1° horizontal resolution for summer 2000. The outflow is driven principally by cyclones tracking eastward across North America at 45–55°N, every 5 days on average. Anthropogenic and fire effluents from western North America are mostly transported north and east, eventually merging with the eastern U.S. pollution outflow to the Atlantic. A semipermanent upper-level anticyclone traps the convective outflow and allows it to age in the upper troposphere over the United States for several days. Rapid ozone production takes place in this outflow, driven in part by anthropogenic and lightning NO x and in part by HO x radicals produced from convectively lifted CH2O that originates from biogenic isoprene. This mechanism could explain ozonesonde observations of elevated ozone in the upper troposphere over the southeastern United States. Asian and European pollution influences in the North American outflow to the Atlantic are found to be dispersed into the background and do not generate distinct plumes. Satellite observations of CO columns from MOPITT and of aerosol optical depths (AODs) from MODIS provide useful mapping of outflow events, despite their restriction to clear-sky scenes.Earth and Planetary Science
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