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The response of streams to changes in atmospheric deposition of sulfur and nitrogen in the Adirondack Mountains

Acidic deposition is the result of upwind sulfur (S) and nitrogen (N) emissions into the atmosphere from human activities. Environmental impacts from acidic deposition across forested landscapes include acidification of soil and drainage water, depletion of available soil nutrient bases, and impacts to and changes in forest and aquatic species composition and biodiversity. Acidic deposition can mobilize aluminum (Al) from soil-to-soil solution and subsequently to drainage water in forms that can be toxic to aquatic life. When exposed to decreasing levels of acidic deposition, which has been occurring in New York since the late 1970s, some soils and drainage waters have become gradually less acidic. Remaining questions relate to effects on stream resources, anticipated resource recovery under increasingly lower levels of deposition, and the levels of deposition (target loads, TLs) needed to reach a range of stream ecosystem recovery targets. Environmental scientists commonly estimate thresholds of air pollutant emissions and resulting atmospheric deposition at which adverse ecological effects are manifested. This analysis is often done using critical loads (CL) and/or TLs, using approaches that account for the spatial and temporal aspects of acidification and recovery. Exceedance represents the extent to which current levels of acidic deposition exceed the level expected to cause ecological harm. The research reported here is intended to help address S and N deposition TLs and ecosystem recovery of Adirondack streams, a resource that has been less thoroughly investigated than lakes. The overarching goal of this work is to highlight key considerations that will help inform decision-makers and ecosystem managers who are responsible for environmental policy in New York State and beyond. Salient aspects of stream TL modeling are discussed with an aim of informing not only scientists, but also policymakers, ecosystem managers, and nonscientists who are required to make decisions related to the effects of acidic deposition on natural ecosystems. Analyses reported herein quantify relations among chemical indicators and metrics of fish community health and biodiversity in streams of the Adirondack Park. This information is used to indicate levels of atmospheric deposition necessary to alleviate harmful effects on fish populations. Results of this investigation provide a framework that can be applied to better understand how modeled stream acid neutralizing capacity (ANC) values that are developed to support TL investigations can be adjusted to reflect high-flow ANC values that may be associated with toxic conditions. Since process models are often calibrated to a low-flow or average flow condition, the magnitude and spatial extent of TL exceedances increase substantially when episodic acidification is considered.

New York

Influence of land-atmosphere feedbacks on temperature and precipitation extremes in the GLACE-CMIP5 ensemble

We examine how soil moisture variability and trends affect the simulation of temperature and precipitation extremes in six global climate models using the experimental protocol of the Global Land-Atmosphere Coupling Experiment of the Coupled Model Intercomparison Project, Phase 5 (GLACE-CMIP5). This protocol enables separate examinations of the influences of soil moisture variability and trends on the intensity, frequency, and duration of climate extremes by the end of the 21st century under a business-as-usual (Representative Concentration Pathway 8.5) emission scenario. Removing soil moisture variability significantly reduces temperature extremes over most continental surfaces, while wet precipitation extremes are enhanced in the tropics. Projected drying trends in soil moisture lead to increases in intensity, frequency, and duration of temperature extremes by the end of the 21st century. Wet precipitation extremes are decreased in the tropics with soil moisture trends in the simulations, while dry extremes are enhanced in some regions, in particular the Mediterranean and Australia. However, the ensemble results mask considerable differences in the soil moisture trends simulated by the six climate models. We find that the large differences between the models in soil moisture trends, which are related to an unknown combination of differences in atmospheric forcing (precipitation, net radiation), flux partitioning at the land surface, and how soil moisture is parameterized, imply considerable uncertainty in future changes in climate extremes.

Journal of Geophysical Research D: Atmospheres

Variations of weekly atmospheric deposition for multiple collectors at a site on the shore of Lake Okeechobee, Florida

Eight wet/dry precipitation collectors were modified to house four additional dryfall collectors and one bulk precipitation collector to sample atmospheric deposition for 12 weeks in a small area on the southwestern shore of Lake Okeechobee; sample contamination, primarily by insects, reduced the comparison to the last nine weeks. The deposition was determined for Ca2+, Na+, Cl-, and SO42- and nutrients including total phosphorus, orthophosphate, total ammonia plus organic nitrogen, and nitrite plus nitrate. In general, deposition was lower and less variable in wet precipitation than in bulk precipitation. The higher variability of the bulk precipitation was attributed to local contamination, particularly by dust and insects. Each wet/dry precipitation collector was fitted with dryfall collectors that consisted of the dry-side bucket on a wet/dry collector, which was preloaded with distilled and deionized water, and four glass dish collectors; two of the glass dishes were preloaded with water and the other two remained dry. The deposition to the dry dish collectors was not comparable in adjacent collectors for any constituent; however, the deposition in the adjacent water-loaded dishes was comparable for most major constituents, except nutrients. A comparison of Ortho-P deposition with Total-P indicated that the P collected by the dryfall collectors was predominantly reactive, which also was reflected in the bulk deposition, whereas that in the wet deposition was mostly nonreactive. The large variability in deposition of P among the bulk and dryfall collectors suggests that alternative methods must be used to evaluate the P sources and processes of atmospheric transfer.

Atmospheric Environment

Atmospheric mercury and fine particulate matter in coastal New England: implications for mercury and trace element sources in the northeastern United States

Intensive sampling of ambient atmospheric fine particulate matter was conducted at Woods Hole, Massachusetts over a four-month period from 3 April to 29 July, 2008, in conjunction with year-long deployment of the USGS Mobile Mercury Lab. Results were obtained for trace elements in fine particulate matter concurrently with determination of ambient atmospheric mercury speciation and concentrations of ancillary gasses (SO 2 , NO x , and O 3 ). For particulate matter, trace element enrichment factors greater than 10 relative to crustal background values were found for As, Bi, Cd, Cu, Hg, Pb, Sb, V, and Zn, indicating contribution of these elements by anthropogenic sources. For other elements, enrichments are consistent with natural marine (Na, Ca, Mg, Sr) or crustal (Ba, Ce, Co, Cs, Fe, Ga, La, Rb, Sc, Th, Ti, U, Y) sources, respectively. Positive matrix factorization was used together with concentration weighted air-mass back trajectories to better define element sources and their locations. Our analysis, based on events exhibiting the 10% highest PM 2.5 contributions for each source category, identifies coal-fired power stations concentrated in the U.S. Ohio Valley, metal smelting in eastern Canada, and marine and crustal sources showing surprisingly similar back trajectories, at times each sampling Atlantic coastal airsheds. This pattern is consistent with contribution of Saharan dust by a summer maximum at the latitude of Florida and northward transport up the Atlantic Coast by clockwise circulation of the summer Bermuda High. Results for mercury speciation show diurnal production of RGM by photochemical oxidation of Hg° in a marine environment, and periodic traverse of the study area by correlated RGM-SO 2 (NO x ) plumes, indicative of coal combustion sources.

Massachusetts

Iron dissolution and speciation in atmospheric mineral dust: Metal-metal synergistic and antagonistic effects

Under acidic atmospheric conditions, iron leached from atmospheric mineral dust may influence the distribution of bioavailable iron at a global scale. However, the effects of non-Fe-containing minerals on iron dissolution remain unknown. This work describes metal-metal synergistic and antagonistic effects on iron dissolution that go beyond aggregation and ionic strength effects in mineral dust mixtures. In this study, we investigated iron mobilization by proton-promoted dissolution in natural mineral dust samples from the Kalahari Desert (SZ1) and Australian Red Dawn event (RO), along with one iron oxide proxy, hematite. The total iron dissolution in natural dust samples highly corresponds with the respective amount of Ti, rather than their particle sizes or Fe contents. The dust sample with high Ti content, SZ1, also showed a higher fraction of dissolved Fe(II), under dark conditions. These observations are in good agreement with the dissolution data for hematite artificially mixed with metal oxides. Total iron dissolution in hematite, mixed with TiO 2 , is 1.5- and 2-fold higher compared to that of just hematite under dark and light conditions, respectively. However, dissolution of hematite is suppressed when mixed with Al 2 O 3 and CaO. Under dark conditions, furthermore, dissolved Fe(II) fraction is enhanced for hematite when mixed with TiO 2 compared to that of other mixtures or hematite alone. Yet, dissolved Fe(II) is lower in hematite mixed with TiO 2 under light conditions compared to that of hematite alone, suggesting photo-oxidation of Fe(II) by reactive oxygen species, such as OH radicals.

Atmospheric Environment

Chamber measurement of surface-atmosphere trace gas exchange: Numerical evaluation of dependence on soil interfacial layer, and source/sink products

We employed a three-dimensional finite difference gas diffusion model to simulate the performance of chambers used to measure surface-atmosphere tace gas exchange. We found that systematic errors often result from conventional chamber design and deployment protocols, as well as key assumptions behind the estimation of trace gas exchange rates from observed concentration data. Specifically, our simulationshowed that (1) when a chamber significantly alters atmospheric mixing processes operating near the soil surface, it also nearly instantaneously enhances or suppresses the postdeployment gas exchange rate, (2) any change resulting in greater soil gas diffusivity, or greater partitioning of the diffusing gas to solid or liquid soil fractions, increases the potential for chamber-induced measurement error, and (3) all such errors are independent of the magnitude, kinetics, and/or distribution of trace gas sources, but greater for trace gas sinks with the same initial absolute flux. Finally, and most importantly, we found that our results apply to steady state as well as non-steady-state chambers, because the slow rate of gas diffusion in soil inhibits recovery of the former from their initial non-steady-state condition. Over a range of representative conditions, the error in steady state chamber estimates of the trace gas flux varied from -30 to +32%, while estimates computed by linear regression from non-steadystate chamber concentrations were 2 to 31% too small. Although such errors are relatively small in comparison to the temporal and spatial variability characteristic of trace gas exchange, they bias the summary statistics for each experiment as well as larger scale trace gas flux estimates based on them.

Journal of Geophysical Research D: Atmospheres

Reconstructed historical land cover and biophysical parameters for studies of land-atmosphere interactions within the eastern United States

Over the past 350 years, the eastern half of the United States experienced extensive land cover changes. These began with land clearing in the 1600s, continued with widespread deforestation, wetland drainage, and intensive land use by 1920, and then evolved to the present-day landscape of forest regrowth, intensive agriculture, urban expansion, and landscape fragmentation. Such changes alter biophysical properties that are key determinants of land-atmosphere interactions (water, energy, and carbon exchanges). To understand the potential implications of these land use transformations, we developed and analyzed 20-km land cover and biophysical parameter data sets for the eastern United States at 1650, 1850, 1920, and 1992 time slices. Our approach combined potential vegetation, county-level census data, soils data, resource statistics, a Landsat-derived land cover classification, and published historical information on land cover and land use. We reconstructed land use intensity maps for each time slice and characterized the land cover condition. We combined these land use data with a mutually consistent set of biophysical parameter classes, to characterize the historical diversity and distribution of land surface properties. Time series maps of land surface albedo, leaf area index, a deciduousness index, canopy height, surface roughness, and potential saturated soils in 1650, 1850, 1920, and 1992 illustrate the profound effects of land use change on biophysical properties of the land surface. Although much of the eastern forest has returned, the average biophysical parameters for recent landscapes remain markedly different from those of earlier periods. Understanding the consequences of these historical changes will require land-atmosphere interactions modeling experiments.

Journal of Geophysical Research D: Atmospheres

Diurnal and vertical variability of the sensible heat and carbon dioxide budgets in the atmospheric surface layer

The diurnal and vertical variability of heat and carbon dioxide (CO2) in the atmospheric surface layer are studied by analyzing measurements from a 213 in tower in Cabauw (Netherlands). Observations of thermodynamic variables and CO2 mixing ratio as well as vertical profiles of the turbulent fluxes are used to retrieve the contribution of the budget terms in the scalar conservation equation. On the basis of the daytime evolution of turbulent fluxes, we calculate the budget terms by assuming that turbulent fluxes follow a linear profile with height. This assumption is carefully tested and the deviation ftom linearity is quantified. The budget calculation allows us to assess the importance of advection of heat and CO2 during day hours for three selected days. It is found that, under nonadvective conditions, the diurnal variability of temperature and CO2 is well reproduced from the flux divergence measurements. Consequently, the vertical transport due to the turbulent flux plays a major role in the daytime evolution of both scalars and the advection is a relatively small contribution. During the analyzed days with a strong contribution of advection of either heat or carbon dioxide, the flux divergence is still an important contribution to the budget. For heat, the quantification of the advection contribution is in close agreement with results from a numerical model. For carbon dioxide, we qualitatively corroborate the results with a Lagrangian transport model. Our estimation of advection is compared with, traditional estimations based on the Net Ecosystem-atmosphere Exchange (NEE). Copyright 2008 by the American Geophysical Union.

Journal of Geophysical Research D: Atmospheres

Flood runoff in relation to water vapor transport by atmospheric rivers over the western United States, 1949–2015

Atmospheric rivers (ARs) have a significant role in generating floods across the western United States. We analyze daily streamflow for water years 1949 to 2015 from 5,477 gages in relation to water vapor transport by ARs using a 6 h chronology resolved to 2.5° latitude and longitude. The probability that an AR will generate 50 mm/d of runoff in a river on the Pacific Coast increases from 12% when daily mean water vapor transport, DVT , is greater than 300 kg m −1 s −1 to 54% when DVT > 600 kg m −1 s −1 . Extreme runoff, represented by the 99th quantile of daily values, doubles from 80 mm/d at DVT = 300 kg m −1 s −1 to 160 mm/d at DVT = 500 kg m −1 s −1 . Forecasts and predictions of water vapor transport by atmospheric rivers can support flood risk assessment and estimates of future flood frequencies and magnitude in the western United States.

Geophysical Research Letters

The GFDL global atmosphere and land model AM4.0/LM4.0: 1. Simulation characteristics with prescribed SSTs

In this two‐part paper, a description is provided of a version of the AM4.0/LM4.0 atmosphere/land model that will serve as a base for a new set of climate and Earth system models (CM4 and ESM4) under development at NOAA's Geophysical Fluid Dynamics Laboratory (GFDL). This version, with roughly 100 km horizontal resolution and 33 levels in the vertical, contains an aerosol model that generates aerosol fields from emissions and a “light” chemistry mechanism designed to support the aerosol model but with prescribed ozone. In Part 1, the quality of the simulation in AMIP (Atmospheric Model Intercomparison Project) mode—with prescribed sea surface temperatures (SSTs) and sea‐ice distribution—is described and compared with previous GFDL models and with the CMIP5 archive of AMIP simulations. The model's Cess sensitivity (response in the top‐of‐atmosphere radiative flux to uniform warming of SSTs) and effective radiative forcing are also presented. In Part 2, the model formulation is described more fully and key sensitivities to aspects of the model formulation are discussed, along with the approach to model tuning.

Journal of Advances in Modeling Earth Systems

Seasonal Sea-Level Variations in San Francisco Bay in Response to Atmospheric Forcing, 1980

The seasonal response of sea level in San Francisco Bay (SFB) to atmospheric forcing during 1980 is investigated. The relations between sea-level data from the Northern Reach, Central Bay and South Bay, and forcing by local wind stresses, sea level pressure (SLP), runoff and the large scale sea level pressure field are examined in detail. The analyses show that the sea-level elevations and slopes respond to the along-shore wind stress T(V) at most times of the year, and to the cross-shore wind stress T(N) during two transition periods in spring and autumn. River runoff raises the sea-level elevation during winter. It is shown that winter precipitation in the SFB area is mainly attributed to the atmospheric circulation associated with the Alcutian Low, which transports the warm, moist air into the Bay area. A multiple linear regression model is employed to estimate the independent contributions of barometric pressure and wind stress to adjusted sea level. These calculations have a simple dynamical interpretation which confirms the importance of along-shore wind to both sea level and north-south slope within the Bay.

Estuarine, Coastal and Shelf Science

Groundwater Dating with Atmospheric Halogenated Compounds

"Atmospheric environmental releases refer to the emission of stable, long-lived compounds of solely anthropogenic origin into the atmosphere and the use of the compounds to estimate dates of their incorporation into groundwater."

Book chapter

Improved mapping of National Atmospheric Deposition Program wet-deposition in complex terrain using PRISM-gridded data sets

High-elevation regions in the United States lack detailed atmospheric wet-deposition data. The National Atmospheric Deposition Program/National Trends Network (NADP/NTN) measures and reports precipitation amounts and chemical constituent concentration and deposition data for the United States on annual isopleth maps using inverse distance weighted (IDW) interpolation methods. This interpolation for unsampled areas does not account for topographic influences. Therefore, NADP/NTN isopleth maps lack detail and potentially underestimate wet deposition in high-elevation regions. The NADP/NTN wet-deposition maps may be improved using precipitation grids generated by other networks. The Parameter-elevation Regressions on Independent Slopes Model (PRISM) produces digital grids of precipitation estimates from many precipitation-monitoring networks and incorporates influences of topographical and geographical features. Because NADP/NTN ion concentrations do not vary with elevation as much as precipitation depths, PRISM is used with unadjusted NADP/NTN data in this paper to calculate ion wet deposition in complex terrain to yield more accurate and detailed isopleth deposition maps in complex terrain. PRISM precipitation estimates generally exceed NADP/NTN precipitation estimates for coastal and mountainous regions in the western United States. NADP/NTN precipitation estimates generally exceed PRISM precipitation estimates for leeward mountainous regions in Washington, Oregon, and Nevada, where abrupt changes in precipitation depths induced by topography are not depicted by IDW interpolation. PRISM-based deposition estimates for nitrate can exceed NADP/NTN estimates by more than 100% for mountainous regions in the western United States.

Environmental Monitoring and Assessment

Diatom changes in two Uinta mountain lakes, Utah, USA: Responses to anthropogenic and natural atmospheric inputs

Diatom assemblages in sediments from two subalpine lakes in the Uinta Mountains, Utah, show asynchronous changes that are related to both anthropogenic and natural inputs of dust. These lakes are downwind of sources of atmospheric inputs originating from mining, industrial, urban, agricultural and natural sources that are distributed within tens to hundreds of kilometers west and south of the Uinta Mountains. Sediment cores were retrieved from Marshall and Hidden lakes to determine the impacts of atmospheric pollution, especially metals. Paleolimnological techniques, including elemental analyses and 210 Pb and 239+240 Pu dating, indicate that both lakes began receiving eolian inputs from anthropogenic sources in the late 1800s with the greatest increases occurring after the early 1900s. Over the last century, sediments in Marshall Lake, which is closer to the Wasatch Front and receives more precipitation than Hidden Lake, received twice the concentrations of metals and phosphorus as Hidden Lake. Comparison of diatom and elemental data reveals coeval changes in geochemistry and diatom assemblages at Marshall Lake, but not at Hidden Lake; however, a major shift in diatom assemblages occurs at Hidden Lake in the seventeenth century. The change in diatoms at Marshall Lake is marked by the near disappearance of Cyclotella stelligera and C. pseudostelligera and an increase in benthic, metal-tolerant diatoms. This change is similar to changes in other lakes that have been attributed to metal pollution. The marked change in diatom assemblages at Hidden Lake indicates a shift in lake-water pH from somewhat acidic to circumneutral. We hypothesize that this change in pH is related to drought-induced changes in input of carbonate-rich desert dust.

Utah

Measurement of atmospheric mercury species with manual sampling and analysis methods in a case study in Indiana

Ground-level concentrations of three atmospheric mercury species were measured using manual sampling and analysis to provide data for estimates of mercury dry deposition. Three monitoring stations were operated simultaneously during winter, spring, and summer 2004, adjacent to three mercury wet-deposition monitoring stations in northern, central, and southern Indiana. The monitoring locations differed in land-use setting and annual mercury-emissions level from nearby sources. A timer-controlled air-sampling system that contained a three-part sampling train was used to isolate reactive gaseous mercury, particulate-bound mercury, and elemental mercury. The sampling trains were exchanged every 6 days, and the mercury species were quantified in a laboratory. A quality-assurance study indicated the sampling trains could be held at least 120 h without a significant change in reactive gaseous or particulate-bound mercury concentrations. The manual sampling method was able to provide valid mercury concentrations in 90 to 95% of samples. Statistical differences in mercury concentrations were observed during the project. Concentrations of reactive gaseous and elemental mercury were higher in the daytime samples than in the nighttime samples. Concentrations of reactive gaseous mercury were higher in winter than in summer and were highest at the urban monitoring location. The results of this case study indicated manual sampling and analysis could be a reliable method for measurement of atmospheric mercury species and has the capability for supplying representative concentrations in an effective manner from a long-term deposition-monitoring network. ?? 2007 Springer Science+Business Media B.V.

Water, Air, & Soil Pollution

Composition and sources of atmospheric dusts in snow at 3200 meters in the St. Elias Range, southeastern Alaska, USA

Dusts in snow from the accumulation zone in the St. Elias Range appear from their chemical compositions to have come from terranes of rocks of ferromagnesian composition. These dusts, with respect to their composition and to the moderate degree of variation that occurs through a depositional year, are similar those deposited in Greenland. The high portion of the St. Elias Range is isolated from dominance by any local dust source terranes, because of altitude and the extent of the surrounding glacierized and snow-covered region. In Greenland the altitude is typically lower, but local sources are even less likely to dominate the character of the dusts deposited into the ice record there. The similar compositions and moderate compositional variations of dusts from these two places bear on the question of whether the dusts that are transported over long distances by the atmosphere under modern and glacial-period conditions are uniform and representative of a broad regional or even hemispheric background dust. The dusts in the snow were measured by means of a suite of major, minor, and trace rock-forming metals chosen to give information about rock types, their constituent minerals, degree of degradation (weathering), and energies of atmospheric uptake from source. The variations in amounts of rock dust through the year in the St. Elias Range snowpack have no time-stratigraphic correspondence to the also large variations in concentrations of other species that are not constituents of rock-derived dusts, such the anions chloride, sulfate, and nitrate; the highs and lows of the two types of materials are apparently completely independent. The structure revealed by the moderately fine-scale sampling of the present study (≈ 10 increments/y) serves as a background for the interpretation of analysis of ice core samples, in which annual layers may be too compressed to permit analysis of sub-annual samples.

Alaska

Mass spectrometric analysis of organic compounds, water and volatile constituents in the atmosphere and surface of Mars: The Viking Mars Lander

An experiment centering around a mass spectrometer is described, which is aimed at the identification of organic substances present in the top 10 cm of the surface of Mars and an analysis of the atmosphere for major and minor constituents as well as isotopic abundances. In addition, an indication of the abundance of water in the surface and some information concerning the mineralogy can be obtained by monitoring the gases produced upon heating the soil sample. The organic material will simply be expelled by heating to 150°, 300°, and 500° into the carrier gas stream of a gas chromatograph interfaced to the mass spectrometer or by slowly heating the sample in direct communication with the spectrometer. It is planned to analyze a total of up to nine soil samples in order to study diurnal and seasonal variations. The system is designed to give useful data even for minor constituents if the total of organics should be as low as 5ppm. The spectrometer covers the mass range of 12–200 with adequate resolution. The results of these experiments, which are deliberately designed to cover a wide spectrum of possibilities independent of terrestrial models, are expected to produce a good picture of the planet's organic chemistry and its possible biological significance as well as allow conclusions regarding the history of the planet's atmosphere.

Icarus

Atmospheric lead deposition to Okefenokee Swamp, Georgia, USA

Contamination of the environment from atmospheric deposition during the twentieth century is pervasive even in areas ostensibly considered pristine or remote from point sources. In this study, Pb concentrations in a 210 Pb-dated peat core collected from the Okefenokee Swamp, GA were used to assess historical contaminant input via atmospheric deposition. Lead isotope ratios were determined by dynamic reaction cell ICP-MS (DRC-ICP-MS). Increases in Pb concentration occurred in the late nineteenth century and a marked rise in Pb concentrations pre-dated the widespread use of leaded gasoline within the US. The 206 Pb/ 207 Pb ratios of 1.19 during this period were consistent with coal combustion emissions. A later increase in Pb concentration, concurrent with a trend toward more radiogenic 06 Pb/ 207 Pb ratios in gasoline is consistent with an increased input of Pb from leaded gasoline emissions remain a major source of Pb to the Okefenokee.

Georgia