Source apportionment of atmospheric trace gases and particulate matter--Comparison of log-ratio and traditional approaches
No abstract available.
Conference Paper↗
SEARCH · Geology Reports
Results for “Atmosphere - Ocean”
Search indexed USGS publications on groundwater, aquifers, geologic maps, mineral resources and earthquakes. Explore source records by subject and place.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
Mercury in Indiana watersheds: Retrospective for 2001–2006
Information about total mercury and methylmercury concentrations in water samples and mercury concentrations in fish-tissue samples was summarized for 26 watersheds in Indiana that drain most of the land area of the State. Mercury levels were interpreted with information on streamflow, atmospheric mercury deposition, mercury emissions to the atmosphere, mercury in wastewater, and landscape characteristics. Unfiltered total mercury concentrations in 411 water samples from streams in the 26 watersheds had a median of 2.32 nanograms per liter (ng/L) and a maximum of 28.2 ng/L. When these concentrations were compared to Indiana water-quality criteria for mercury, 5.4 percent exceeded the 12-ng/L chronic-aquatic criterion, 59 percent exceeded the 1.8-ng/L Great Lakes human-health criterion, and 72.5 percent exceeded the 1.3-ng/L Great Lakes wildlife criterion. Mercury concentrations in water were related to streamflow, and the highest mercury concentrations were associated with the highest streamflows. On average, 67 percent of total mercury in streams was in a particulate form, and particulate mercury concentrations were significantly lower downstream from dams than at monitoring stations not affected by dams. Methylmercury is the organic fraction of total mercury and is the form of mercury that accumulates and magnifies in food chains. It is made from inorganic mercury by natural processes under specific conditions. Unfiltered methylmercury concentrations in 411 water samples had a median of 0.10 ng/L and a maximum of 0.66 ng/L. Methylmercury was a median 3.7 percent and maximum 64.8 percent of the total mercury in 252 samples for which methylmercury was reported. The percentages of methylmercury in water samples were significantly higher downstream from dams than at other monitoring stations. Nearly all of the total mercury detected in fish tissue was assumed to be methylmercury. Fish-tissue samples from the 26 watersheds had wet-weight mercury concentrations that exceeded the 0.3 milligram per kilogram (mg/kg) U.S. Environmental Protection Agency (USEPA) methylmercury criterion in 12.4 percent of the 1,731 samples. The median wet-weight concentration in the fish-tissue samples was 0.13 mg/kg, and the maximum was 1.07 mg/kg. A coarse-scale analysis of all fish-tissue data in each watershed and a fine-scale analysis of data within 5 kilometers (km) of the downstream end of each watershed showed similar results overall. Mercury concentrations in fish-tissue samples were highest in the White River watershed in southern Indiana and the Fall Creek watershed in central Indiana. In fish-tissue samples within 5 km of the downstream end of a watershed, the USEPA methylmercury criterion was exceeded by 45 percent of mercury concentrations from the White River watershed and 40 percent of the mercury concentration from the Fall Creek watershed. A clear relation between mercury concentrations in fish-tissue samples and methylmercury concentrations in water was not observed in the data from watersheds in Indiana. Average annual atmospheric mercury wet-deposition rates were mapped with data at 156 locations in Indiana and four surrounding states for 2001–2006. These maps revealed an area in southeastern Indiana with high mercury wet-deposition rates—from 15 to 19 micrograms per square meter per year (µg/m 2 /yr). Annual atmospheric mercury dry-deposition rates were estimated with an inferential method by using concentrations of mercury species in air samples at three locations in Indiana. Mercury dry deposition-rates were 5.6 to 13.6 µg/m 2 /yr and were 0.49 to 1.4 times mercury wet-deposition rates. Total mercury concentrations were detected in 96 percent of 402 samples of wastewater effluent from 50 publicly owned treatment works in the watersheds; the median concentration was 3.0 ng/L, and the maximum was 88 ng/L. When these concentrations were compared to Indiana water-quality criteria for mercury, 12 percent exceeded the 12-ng/L chronic-aquatic criterion, 68 percent exceeded the 1.8-ng/L Great Lakes human-health criterion, and 81 percent exceeded the 1.3-ng/L Great Lakes wildlife criterion. Annual stream mercury yields were calculated with a model by using the mercury concentrations in water samples and daily average streamflows for 2002–2006, normalized to the watershed drainage areas. The average annual total mercury stream yields ranged from 0.73 to 45.2 µg/m 2 /yr and were highest in two White River watersheds in central Indiana. Median methylmercury stream yield was 1.9 percent of the median total mercury stream yield. In most watersheds, average annual stream yields of total mercury were a fraction of the combined average annual atmospheric mercury wet-deposition and estimated annual dry-deposition loading rates, indicating that much of the stream mercury was attributable to atmospheric deposition. In two watersheds, average annual stream yields of total mercury were approximately twice the atmospheric mercury loading, indicating that some of the stream mercury apparently was not attributable to atmospheric deposition. Rather, some of the stream mercury yield potentially was contributed by mercury in wastewater discharges. Land-cover type corresponded with the mercury levels in three watersheds: (1) A watershed of the White River in central Indiana with a high percentage of urban land cover had some of the highest total mercury concentrations and stream mercury yields. The urban land cover and numerous permitted wastewater outfalls with mercury in treated effluent potentially contributed mercury to this watershed. (2) A monitoring station on the Maumee River in northeastern Indiana, downstream from a large area of urban land cover, recorded the highest stream mercury concentrations. The urban land cover and mercury detected in treated effluent potentially contributed to the high mercury concentrations at this station. (3) A watershed of the Patoka River in southern Indiana with a high percentage of forest land cover had the highest atmospheric mercury dry-deposition rate. The high dry-deposition rate from the forest land cover potentially contributed to the high mercury concentrations in this watershed. From a retrospective view, mercury concentrations in Indiana watersheds routinely exceeded criteria protective of humans and commonly exceeded criteria protective of wildlife. Atmospheric mercury wet deposition was a predominant factor, but not the single factor, affecting mercury in Indiana watersheds. Mercury in wastewater discharges and atmospheric mercury dry deposition apparently contributed a substantial part of the mercury yield from some watersheds. Dams and impoundments increased the percentage of methylmercury in downstream waters. Long-term monitoring of mercury in wet and dry atmospheric deposition, and in streams and reservoirs, coordinated with monitoring of mercury in fish, will be needed to detect whether mercury levels in Indiana watersheds change in the future.
Indiana↗
Global methane budget 2000-2020
Understanding and quantifying the global methane (CH 4 ) budget is important for assessing realistic pathways to mitigate climate change. CH 4 is the second most important human-influenced greenhouse gas in terms of climate forcing after carbon dioxide (CO 2 ), and both emissions and atmospheric concentrations of CH 4 have continued to increase since 2007 after a temporary pause. The relative importance of CH 4 emissions compared to those of CO 2 for temperature change is related to its shorter atmospheric lifetime, stronger radiative effect, and acceleration in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in quantifying the factors responsible for the observed atmospheric growth rate arise from diverse, geographically overlapping CH 4 sources and from the uncertain magnitude and temporal change in the destruction of CH 4 by short-lived and highly variable hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to improve, synthesise, and update the global CH 4 budget regularly and to stimulate new research on the methane cycle. Following Saunois et al. (2016, 2020), we present here the third version of the living review paper dedicated to the decadal CH 4 budget, integrating results of top-down CH 4 emission estimates (based on in situ and Greenhouse Gases Observing SATellite (GOSAT) atmospheric observations and an ensemble of atmospheric inverse-model results) and bottom-up estimates (based on process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). We present a budget for the most recent 2010–2019 calendar decade (the latest period for which full data sets are available), for the previous decade of 2000–2009 and for the year 2020. The revision of the bottom-up budget in this 2025 edition benefits from important progress in estimating inland freshwater emissions, with better counting of emissions from lakes and ponds, reservoirs, and streams and rivers. This budget also reduces double counting across freshwater and wetland emissions and, for the first time, includes an estimate of the potential double counting that may exist (average of 23 Tg CH 4 yr −1 ). Bottom-up approaches show that the combined wetland and inland freshwater emissions average 248 [159–369] Tg CH 4 yr −1 for the 2010–2019 decade. Natural fluxes are perturbed by human activities through climate, eutrophication, and land use. In this budget, we also estimate, for the first time, this anthropogenic component contributing to wetland and inland freshwater emissions. Newly available gridded products also allowed us to derive an almost complete latitudinal and regional budget based on bottom-up approaches. For the 2010–2019 decade, global CH 4 emissions are estimated by atmospheric inversions (top-down) to be 575 Tg CH 4 yr −1 (range 553–586, corresponding to the minimum and maximum estimates of the model ensemble). Of this amount, 369 Tg CH 4 yr −1 or ∼ 65 % is attributed to direct anthropogenic sources in the fossil, agriculture, and waste and anthropogenic biomass burning (range 350–391 Tg CH 4 yr −1 or 63 %–68 %). For the 2000–2009 period, the atmospheric inversions give a slightly lower total emission than for 2010–2019, by 32 Tg CH 4 yr −1 (range 9–40). The 2020 emission rate is the highest of the period and reaches 608 Tg CH 4 yr −1 (range 581–627), which is 12 % higher than the average emissions in the 2000s. Since 2012, global direct anthropogenic CH 4 emission trends have been tracking scenarios that assume no or minimal climate mitigation policies proposed by the Intergovernmental Panel on Climate Change (shared socio-economic pathways SSP5 and SSP3). Bottom-up methods suggest 16 % (94 Tg CH 4 yr −1 ) larger global emissions (669 Tg CH 4 yr −1 , range 512–849) than top-down inversion methods for the 2010–2019 period. The discrepancy between the bottom-up and the top-down budgets has been greatly reduced compared to the previous differences (167 and 156 Tg CH 4 yr −1 in Saunois et al. (2016, 2020) respectively), and for the first time uncertainties in bottom-up and top-down budgets overlap. Although differences have been reduced between inversions and bottom-up, the most important source of uncertainty in the global CH 4 budget is still attributable to natural emissions, especially those from wetlands and inland freshwaters. The tropospheric loss of methane, as the main contributor to methane lifetime, has been estimated at 563 [510–663] Tg CH 4 yr −1 based on chemistry–climate models. These values are slightly larger than for 2000–2009 due to the impact of the rise in atmospheric methane and remaining large uncertainty ( ∼ 25 %). The total sink of CH 4 is estimated at 633 [507–796] Tg CH 4 yr −1 by the bottom-up approaches and at 554 [550–567] Tg CH 4 yr −1 by top-down approaches. However, most of the top-down models use the same OH distribution, which introduces less uncertainty to the global budget than is likely justified. For 2010–2019, agriculture and waste contributed an estimated 228 [213–242] Tg CH 4 yr −1 in the top-down budget and 211 [195–231] Tg CH 4 yr −1 in the bottom-up budget. Fossil fuel emissions contributed 115 [100–124] Tg CH 4 yr −1 in the top-down budget and 120 [117–125] Tg CH 4 yr −1 in the bottom-up budget. Biomass and biofuel burning contributed 27 [26–27] Tg CH 4 yr −1 in the top-down budget and 28 [21–39] Tg CH 4 yr −1 in the bottom-up budget. We identify five major priorities for improving the CH 4 budget: (i) producing a global, high-resolution map of water-saturated soils and inundated areas emitting CH 4 based on a robust classification of different types of emitting ecosystems; (ii) further development of process-based models for inland-water emissions; (iii) intensification of CH 4 observations at local (e.g. FLUXNET-CH 4 measurements, urban-scale monitoring, satellite imagery with pointing capabilities) to regional scales (surface networks and global remote sensing measurements from satellites) to constrain both bottom-up models and atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) integration of 3D variational inversion systems using isotopic and/or co-emitted species such as ethane as well as information in the bottom-up inventories on anthropogenic super-emitters detected by remote sensing (mainly oil and gas sector but also coal, agriculture, and landfills) to improve source partitioning.
Earth System Science Data↗
Acid Rain
Although acid rain is fading as a political issue in the United States and funds for research in this area have largely disappeared, the acidity of rain in the Eastern United States has not changed significantly over the last decade, and it continues to be a serious environmental problem. Acid deposition (commonly called acid rain) is a term applied to all forms of atmospheric deposition of acidic substances - rain, snow, fog, acidic dry particulates, aerosols, and acid-forming gases. Water in the atmosphere reacts with certain atmospheric gases to become acidic. For example, water reacts with carbon dioxide in the atmosphere to produce a solution with a pH of about 5.6. Gases that produce acids in the presence of water in the atmosphere include carbon dioxide (which converts to carbonic acid), oxides of sulfur and nitrogen (which convert to sulfuric and nitric acids}, and hydrogen chloride (which converts to hydrochloric acid). These acid-producing gases are released to the atmosphere through natural processes, such as volcanic emissions, lightning, forest fires, and decay of organic matter. Accordingly, precipitation is slightly acidic, with a pH of 5.0 to 5.7 even in undeveloped areas. In industrialized areas, most of the acid-producing gases are released to the atmosphere from burning fossil fuels. Major emitters of acid-producing gases include power plants, industrial operations, and motor vehicles. Acid-producing gases can be transported through the atmosphere for hundreds of miles before being converted to acids and deposited as acid rain. Because acids tend to build up in the atmosphere between storms, the most acidic rain falls at the beginning of a storm, and as the rain continues, the acids "wash out" of the atmosphere.
Conference Paper↗
Occurrence of nitrous oxide in the central High Plains aquifer, 1999
Nitrogen-enriched groundwater has been proposed as an important anthropogenic source of atmospheric nitrous oxide (N2O), yet few measurements of N2O in large aquifer systems have been made. Concentrations of N2O in water samples collected from the 124 000 km2 central High Plains aquifer in 1999 ranged from < 1 to 940 nM, with a median concentration of 29 nM (n = 123). Eighty percent of the N20 concentrations exceeded the aqueous concentration expected from equilibration with atmospheric N2O. Measurements of N2O, NO3-, and 3H in unsaturated-zone sediments, recently recharged groundwater, and older groundwater indicate that concentrations of N2O in groundwater increased over time and will likely continue to increase in the future as N-enriched water recharges the aquifer. Large concentrations of O2 and NO3- and small concentrations of NH4+ and dissolved organic carbon in the aquifer indicate that N2O in the central High Plains aquifer was produced primarily by nitrification. Calculations indicate that the flux of N2O from the central High Plains aquifer to the atmosphere from well pumping and groundwater discharge to streams was not a significant source of atmospheric N2O.Nitrogen-enriched groundwater has been proposed as an important anthropogenic source of atmospheric nitrous oxide (N2O), yet few measurements of N2O in large aquifer systems have been made. Concentrations of N2O in water samples collected from the 124000 km2 central High Plains aquifer in 1999 ranged from < 1 to 940 nM, with a median concentration of 29 nM (n = 123). Eighty percent of the N2O concentrations exceeded the aqueous concentration expected from equilibration with atmospheric N2O. Measurements of N2O, NO3-, and 3H in unsaturated-zone sediments, recently recharged groundwater, and older groundwater indicate that concentrations of N2O in groundwater increased over time and will likely continue to increase in the future as N-enriched water recharges the aquifer. Large concentrations of O2 and NO3- and small concentrations of NH4+ and dissolved organic carbon in the aquifer indicate that N2O in the central High Plains aquifer was produced primarily by nitrification. Calculations indicate that the flux of N2O from the central High Plains aquifer to the atmosphere from well pumping and groundwater discharge to streams was not a significant source of atmospheric N2O.Water samples were collected from 92 domestic wells, 16 monitoring wells and 15 public-supply wells in the High Plains Aquifer in 1999, and concentrations of nitrous oxide were measured. The groundwater concentrations ranged from less than 1 to 940 nM. Concentrations expressed as a percent of saturation in water ranged from less than 10 to 9690%. A significant decrease was noted in N2O concentrations with increasing depth of the well screen below the water table, and a significant positive correlation was found between the concentrations of N2O and nitrate. The small area-averaged N2O emission rate for the aquifer indicated that it was not an important component of the atmospheric N2O budget, but the importance could increase as groundwater N2O concentrations increase.
Environmental Science & Technology↗
Perchlorate in pleistocene and holocene groundwater in North-Central New Mexico
Groundwater from remote parts of the Middle Rio Grande Basin in north-central New Mexico has perchlorate (ClO 4 - ) concentrations of 0.12−1.8 μg/L. Because the water samples are mostly preanthropogenic in age (0−28 000 years) and there are no industrial sources in the study area, a natural source of the ClO 4 - is likely. Most of the samples have Br - , Cl - , and SO 4 2 - concentrations that are similar to those of modern bulk atmospheric deposition with evapotranspiration (ET) factors of about 7−40. Most of the ET values for Pleistocene recharge were nearly twice that for Holocene recharge. The NO 3 - /Cl - and ClO 4 - /Cl - ratios are more variable than those of Br - /Cl - or SO 4 2 - /Cl - . Samples thought to have recharged under the most arid conditions in the Holocene have relatively high NO 3 - /Cl - ratios and low δ 15 N values (+1 per mil (‰)) similar to those of modern bulk atmospheric N deposition. The δ 18 O values of the NO 3 - (−4 to 0 ‰) indicate that atmospheric NO 3 - was not transmitted directly to the groundwater but may have been cycled in the soils before infiltrating. Samples with nearly atmospheric NO 3 - /Cl - ratios have relatively high ClO 4 - concentrations (1.0−1.8 μg/L) with a nearly constant ClO 4 - /Cl - mole ratio of (1.4 ± 0.1) × 10 - 4 , which would be consistent with an average ClO 4 - concentration of 0.093 ± 0.005 μg/L in bulk atmospheric deposition during the late Holocene in north-central NM. Samples thought to have recharged under wetter conditions have higher δ 15 N values (+3 to +8 ‰), lower NO 3 - /Cl - ratios, and lower ClO 4 - /Cl - ratios than the ones most likely to preserve an atmospheric signal. Processes in the soils that may have depleted atmospherically derived NO 3 - also may have depleted ClO 4 - to varying degrees prior to recharge. If these interpretations are correct, then ClO 4 - concentrations of atmospheric origin as high as 4 μg/L are possible in preanthropogenic groundwater in parts of the Southwest where ET approaches a factor of 40. Higher ClO 4 - concentrations in uncontaminated groundwater could occur in recharge beneath arid areas where ET is greater than 40, where long-term accumulations of atmospheric salts are leached suddenly from dry soils, or where other (nonatmospheric) natural sources of ClO 4 - exist.
Environmental Science & Technology↗
Implementing a dual-spectrometer approach for improved surface reflectance estimation
Surface reflectance measurement is an integral part of the vicarious calibration of satellite sensors and the validation of satellite-derived top-of-atmosphere (TOA) and surface reflectance products. A well-known practice for estimating surface reflectance is to conduct a field campaign with a spectrometer and a calibration panel, which is labor-intensive and expensive. To address this issue, the Radiometric Calibration Network, RadCalNet, has been developed, which automatically collects surface reflectance over several selected sites. Neither of these approaches can continuously track the atmosphere, which limits their ability to compensate for atmospheric transmittance change during target measurement. This paper presents the dual-spectrometer approach that uses a stationary spectrometer dedicated to continuously tracking changes in atmospheric transmittance by staring at a calibrated reference panel while the mobile spectrometer measures the target. Simultaneous measurement of the reflectance panel and target help to transfer calibration from the stationary spectrometer to the mobile spectrometer and synchronize the measurements. In this manner, atmospheric transmittance changes during target measurement can be tracked and used to reduce the variability of the target surface reflectance. This paper uses field measurement data from combined field campaigns between different calibration groups at Brookings, South Dakota, and Landsat 8 and Landsat 9 underfly efforts over Coconino National Forest, Arizona, and Guymon, Oklahoma. Preliminary results show that even in a clear sky condition, where atmospheric transmittance changes are minimal, the precision of target surface reflectance estimated using the dual-spectrometer approach is 2–6% better than the single-spectrometer approach. The dual-spectrometer approach shows the potential for a substantial improvement in the precision of the target spectral profile when the atmospheric transmittance is changing rapidly during field measurement. Results show that during non-optimal atmospheric conditions, the dual-spectrometer approach improved the precision of the surface reflectance by 50–60% compared to the single-spectrometer approach across most spectral regions. The ability to estimate surface reflectance more precisely using the dual-spectrometer approach in different atmospheric conditions improves the vicarious calibration of optical satellite sensors and the validation of both TOA and surface reflectance products.
Remote Sensing↗
A synthesis of patterns of environmental mercury inputs, exposure and effects in New York State
Mercury (Hg) pollution is an environmental problem that adversely affects human and ecosystem health at local, regional, and global scales—including within New York State. More than two-thirds of the Hg currently released to the environment originates, either directly or indirectly, from human activities. Since the early 1800s, global atmospheric Hg concentrations have increased by three- to eight-fold over natural levels. In the U.S., atmospheric emissions and point-source releases to waterways increased following industrialization into the mid-1980s. Since then, water discharges have largely been curtailed. As a result, Hg emissions, atmospheric concentrations, and deposition over the past few decades have declined across the eastern U.S. Despite these decreases, Hg pollution persists. To inform policy efforts and to advance public understanding, the New York State Energy Research and Development Authority (NYSERDA) sponsored a scientific synthesis of information on Hg in New York State. This effort includes 23 papers focused on Hg in atmospheric deposition, water, fish, and wildlife published in Ecotoxicology . New York State experiences Hg contamination largely due to atmospheric deposition. Some landscapes are inherently sensitive to Hg inputs driven by the transport of inorganic Hg to zones of methylation, the conversion of inorganic Hg to methylmercury, and the bioaccumulation and biomagnification along food webs. Mercury concentrations exceed human and ecological risk thresholds in many areas of New York State, particularly the Adirondacks, Catskills, and parts of Long Island. Mercury concentrations in some biota have declined in the Eastern Great Lakes Lowlands and the Northeastern Highlands over the last four decades, concurrent with decreases in water releases and air emissions from regional and U.S. sources. However, widespread changes have not occurred in other ecoregions of New York State. While the timing and magnitude of the response of Hg levels in biota varies, policies expected to further diminish Hg emissions should continue to decrease Hg concentrations in food webs, yielding benefits to the fish, wildlife, and people of New York State. Anticipated improvements in the Hg status of aquatic ecosystems are likely to be greatest for inland surface waters and should be roughly proportional to declines in atmospheric Hg deposition. Efforts that advance recovery from Hg pollution in recent years have yielded significant progress, but Hg remains a pollutant of concern. Indeed, due to this extensive compilation of Hg observations in biota, it appears that the extent and intensity of the contamination on the New York landscape and waterscape is greater than previously recognized. Understanding the extent of Hg contamination and recovery following decreases in atmospheric Hg deposition will require further study, underscoring the need to continue existing monitoring efforts.
New York↗
Carbon balance of the terrestrial biosphere in the twentieth century: analyses of CO 2 , climate and land use effects with four process-based ecosystem models
The concurrent effects of increasing atmospheric CO 2 concentration, climate variability, and cropland establishment and abandonment on terrestrial carbon storage between 1920 and 1992 were assessed using a standard simulation protocol with four process-based terrestrial biosphere models. Over the long-term(1920–1992), the simulations yielded a time history of terrestrial uptake that is consistent (within the uncertainty) with a long-term analysis based on ice core and atmospheric CO 2 data. Up to 1958, three of four analyses indicated a net release of carbon from terrestrial ecosystems to the atmosphere caused by cropland establishment. After 1958, all analyses indicate a net uptake of carbon by terrestrial ecosystems, primarily because of the physiological effects of rapidly rising atmospheric CO 2 . During the 1980s the simulations indicate that terrestrial ecosystems stored between 0.3 and 1.5 Pg C yr−1, which is within the uncertainty of analysis based on CO 2 and O 2 budgets. Three of the four models indicated (in accordance with O 2 evidence) that the tropics were approximately neutral while a net sink existed in ecosystems north of the tropics. Although all of the models agree that the long-term effect of climate on carbon storage has been small relative to the effects of increasing atmospheric CO 2 and land use, the models disagree as to whether climate variability and change in the twentieth century has promoted carbon storage or release. Simulated interannual variability from 1958 generally reproduced the El Niño/Southern Oscillation (ENSO)-scale variability in the atmospheric CO 2 increase, but there were substantial differences in the magnitude of interannual variability simulated by the models. The analysis of the ability of the models to simulate the changing amplitude of the seasonal cycle of atmospheric CO 2 suggested that the observed trend may be a consequence of CO 2 effects, climate variability, land use changes, or a combination of these effects. The next steps for improving the process-based simulation of historical terrestrial carbon include (1) the transfer of insight gained from stand-level process studies to improve the sensitivity of simulated carbon storage responses to changes in CO 2 and climate, (2) improvements in the data sets used to drive the models so that they incorporate the timing, extent, and types of major disturbances, (3) the enhancement of the models so that they consider major crop types and management schemes, (4) development of data sets that identify the spatial extent of major crop types and management schemes through time, and (5) the consideration of the effects of anthropogenic nitrogen deposition. The evaluation of the performance of the models in the context of a more complete consideration of the factors influencing historical terrestrial carbon dynamics is important for reducing uncertainties in representing the role of terrestrial ecosystems in future projections of the Earth system.
Global Biogeochemical Cycles↗
An analysis of the global spatial variability of column-averaged CO 2 from SCIAMACHY and its implications for CO 2 sources and sinks
Satellite observations of carbon dioxide (CO 2 ) are important because of their potential for improving the scientific understanding of global carbon cycle processes and budgets. We present an analysis of the column-averaged dry air mole fractions of CO 2 (denoted XCO 2 ) of the Scanning Imaging Absorption Spectrometer for Atmospheric Cartography (SCIAMACHY) retrievals, which were derived from a satellite instrument with relatively long-term records (2003–2009) and with measurements sensitive to the near surface. The spatial-temporal distributions of remotely sensed XCO 2 have significant spatial heterogeneity with about 6–8% variations (367–397 ppm) during 2003–2009, challenging the traditional view that the spatial heterogeneity of atmospheric CO 2 is not significant enough (<4%) to have any large effect on terrestrial ecosystem carbon cycles. By comparison with surface measurements from the NOAA Earth System Research Laboratory (ESRL) GLOBALVIEW network, significant statistical relationships between XCO 2 and surface CO 2 were found for major ecosystems, with the exception of tropical forest. In addition, when compared with a simulated terrestrial carbon uptake from the Integrated Biosphere Simulator (IBIS) and the Emissions Database for Global Atmospheric Research (EDGAR) carbon emission inventory, the latitudinal gradient of XCO 2 seasonal amplitude was influenced by the combined effect of terrestrial carbon uptake, carbon emission, and atmospheric transport, suggesting no direct implications for terrestrial carbon sinks. From the investigation of the growth rate of XCO 2 we found that the increase of CO 2 concentration was dominated by temperature in the northern hemisphere (20–90°N) and by precipitation in the southern hemisphere (20–90°S), with the major contribution to global average occurring in the northern hemisphere. These findings indicated that the satellite measurements of atmospheric CO 2 improve not only the estimations of atmospheric inversion, but also the understanding of the terrestrial ecosystem carbon dynamics and its feedback to atmospheric CO 2 .
International Journal of Remote Sensing↗
Generation of liquid water on Mars through the melting of a dusty snowpack
The possibility that snowmelt could have provided liquid water for valley network formation early in the history of Mars is investigated using an optical-thermal model developed for dusty snowpacks at temperate latitudes. The heating of the postulated snow is assumed to be driven primarily by the absorption of solar radiation during clear sky conditions. Radiative heating rates are predicted as a function of depth and shown to be sensitive to the dust concentration and the size of the ice grains while the thermal conductivity is controlled by temperature, atmospheric pressure, and bulk density. Rates of metamorphism indicate that fresh fine-grained snow on Mars would evolve into moderately coarse snow during a single summer season. Results from global climate models are used to constrain the mean-annual surface temperatures for snow and the atmospheric exchange terms in the surface energy balance. Mean-annual temperatures within Martian snowpacks fail to reach the melting point for all atmospheric pressures below 1000 mbar despite a predicted temperature enhancement beneath the surface of the snowpacks. When seasonal and diurnal variations in the incident solar flux are included in the model, melting occurs at midday during the summer for a wide range of snow types and atmospheric pressures if the dust levels in the snow exceed 100 ppmw (parts per million by weight). The optimum dust concentration appears to be about 1000 ppmw. With this dust load, melting can occur in the upper few centimeters of a dense coarse-grained snow at atmospheric pressures as low as 7 mbar. Snowpack thickness and the thermal conductivity of the underlying substrate determine whether the generated snow-melt can penetrate to the snowpack base, survive basal ice formation, and subsequently become available for runoff. Under favorable conditions, liquid water becomes available for runoff at atmospheric pressures as low as 30 to 100 mbar if the substrate is composed of regolith, as is expected in the ancient cratered terrain of Mars.
Icarus↗
Steep spatial gradients of volcanic and marine sulfur in Hawaiian rainfall and ecosystems
Sulfur, a nutrient required by terrestrial ecosystems, is likely to be regulated by atmospheric processes in well-drained, upland settings because of its low concentration in most bedrock and generally poor retention by inorganic reactions within soils. Environmental controls on sulfur sources in unpolluted ecosystems have seldom been investigated in detail, even though the possibility of sulfur limiting primary production is much greater where atmospheric deposition of anthropogenic sulfur is low. Here we measure sulfur isotopic compositions of soils, vegetation and bulk atmospheric deposition from the Hawaiian Islands for the purpose of tracing sources of ecosystem sulfur. Hawaiian lava has a mantle-derived sulfur isotopic composition (δ 34 S VCDT) of − 0.8‰. Bulk deposition on the island of Maui had a δ 34 S VCDT that varied temporally, spanned a range from + 8.2 to + 19.7‰, and reflected isotopic mixing from three sources: sea-salt (+ 21.1‰), marine biogenic emissions (+ 15.6‰), and volcanic emissions from active vents on Kilauea Volcano (+ 0.8‰). A straightforward, weathering-driven transition in ecosystem sulfur sources could be interpreted in the shift from relatively low (0.0 to + 2.7‰) to relatively high (+ 17.8 to + 19.3‰) soil δ 34 S values along a 0.3 to 4100 ka soil age-gradient, and similar patterns in associated vegetation. However, sub-kilometer scale spatial variation in soil sulfur isotopic composition was found along soil transects assumed by age and mass balance to be dominated by atmospheric sulfur inputs. Soil sulfur isotopic compositions ranged from + 8.1 to + 20.3‰ and generally decreased with increasing elevation (0–2000 m), distance from the coast (0–12 km), and annual rainfall (180–5000 mm). Such trends reflect the spatial variation in marine versus volcanic inputs from atmospheric deposition. Broadly, these results illustrate how the sources and magnitude of atmospheric deposition can exert controls over ecosystem sulfur biogeochemistry across relatively small spatial scales.
Hawaii↗
Ecological factors decouple Great Lakes fish mercury concentrations trends decadal declines in mercury emissions
Atmospheric mercury (Hg) deposition has been declining in North America but remains the dominant delivery mechanism to the Great Lakes. The Lakes are highly efficient at bioaccumulating methylmercury, making the fish excellent sentinels for tracking shifts in atmospheric Hg deposition. Invasive mussels have altered biogeochemical processes, prey populations and fish dietary strategies asynchronously and to varied extents across the lower four lakes, impacting fish Hg exposure. To test if fish are adapting to new biogeochemical conditions, we analyzed a 40 year fish archive for carbon and nitrogen isotope ratios and amino acid-specific nitrogen isotope ratios. To assess Hg sources, we measured Hg isotope ratios. We reconstructed and compared energetic pathways that impact fish Hg concentrations to Hg-source trends. We found fish-Hg concentrations are declining but not monotonically due to ecological disturbances. Fish-Hg isotope values, unimpacted by ecological disturbance, confirm that sources of bioaccumulated Hg shift contemporaneously with changes in atmospheric Hg concentrations. Across Lakes, the degree of responsiveness to changes in atmospheric Hg concentrations mirrors the proportion of atmospheric-delivered Hg we previously modeled. Changes in both fish concentrations and fish isotope values outpace paleolimnetic reconstructions suggesting declines in atmospheric Hg concentrations impact fish Hg more than sediment.
Great Lakes↗
Effect of chronic nitrogen additions on soil nitrogen fractions in red spruce stands
The responses of temperate and boreal forest ecosystems to increased nitrogen (N) inputs have been varied, and the responses of soil N pools have been difficult to measure. In this study, fractions and pool sizes of N were determined in the forest floor of red spruce stands at four sites in the northeastern U.S. to evaluate the effect of increased N inputs on forest floor N. Two of the stands received 100 kg N ha-1 yr-1 for three years, one stand received 34 kg N ha-1 yr-1 for six years, and the remaining stand received only ambient N inputs. No differences in total N content or N fractions were measured in samples of the Oie and Oa horizons between treated and control plots in the three sites that received N amendments. The predominant N fraction in these samples was amino acid N (31-45 % of total N), followed by hydrolyzable unidentified N (16-31% of total N), acid- soluble N (18-22 % of total N), and NH4/+-N (9-13 % of total N). Rates of atmospheric deposition varied greatly among the four stands. Ammonium N and amino acid N concentrations in the Oie horizon were positively related to wet N deposition, with respective r2 values of 0.92 and 0.94 (n = 4, p < 0.05). These relationships were somewhat stronger than that observed between atmospheric wet N deposition and total N content of the forest floor, suggesting that these pools retain atmospherically deposited N. The NH4/+- N pool may represent atmospherically deposited N that is incorporated into organic matter, whereas the amino acid N pool could result from microbial immobilization of atmospheric N inputs. The response of forest floor N pools to applications of N may be masked, possibly by the large soil N pool, which has been increased by the long-term input of N from atmospheric deposition, thereby overwhelming the short-term treatments.
Water, Air, & Soil Pollution↗
Controls on nitrogen flux in alpine/subalpine watersheds of Colorado
High‐altitude watersheds in the Front Range of Colorado show symptoms of advanced stages of nitrogen excess, despite having less nitrogen in atmospheric deposition than other regions where watersheds retain nitrogen. In two alpine/subalpine subbasins of the Loch Vale watershed, atmospheric deposition of NO 3 − plus NH 4 + was 3.2–5.5 kg N ha −1 , and watershed export was 1.8–3.9 kg N ha −1 for water years 1992–1997. Annual N export increased in years with greater input of N, but most of the additional N was retained in the watershed, indicating that parts of the ecosystem are nitrogen‐limited. Dissolved inorganic nitrogen (DIN) concentrations were greatest in subsurface water of talus landscapes, where mineralization and nitrification augment high rates of atmospheric deposition of N. Tundra landscapes had moderately high DIN concentrations, whereas forest and wetland landscapes had low concentrations, indicating little export of nitrogen from these landscapes. Between the two subbasins the catchment of Icy Brook had greater retention of nitrogen than that of Andrews Creek because of landscape and hydrologic characteristics that favor greater N assimilation in both the terrestrial and aquatic ecosystems. These results suggest that export of N from alpine/subalpine watersheds is caused by a combination of direct flushing of N from atmospheric deposition and release of N from ecosystem biogeochemical processes (N cycling). Sensitivity of alpine ecosystems in the western United States to atmospheric deposition of N is a function of landscape heterogeneity, hydrologic flow paths, and climatic extremes that limit primary productivity and microbial activity, which, in turn, control retention and release of nitrogen. Conceptual and mechanistic models of N excess that have been developed for forested ecosystems need to be modified in order to predict the response of alpine ecosystems to future changes in climate and atmospheric deposition of N.
Water Resources Research↗
Quantifying non-thermal silicate weathering using Ge/Si and Si isotopes in rivers draining the Yellowstone Plateau Volcanic Field, USA
In active volcanic regions, high-temperature chemical reactions in the hydrothermal system consume CO 2 sourced from magma or from the deep crust, whereas reactions with silicates at shallow depths mainly consume atmospheric CO 2 . Numerous studies have quantified the load of dissolved solids in rivers that drain volcanic regions to determine chemical weathering rates and atmospheric CO 2 consumption rates. However, the balance between thermal and non-thermal components to riverine fluxes in these areas remains poorly constrained, hindering accurate estimates of atmospheric CO 2 consumption rates. Here we use the Ge/Si ratio and the stable silicon isotopes (δ 30 Si) as tracers for quantifying non-thermal silicon contributions in rivers draining the Yellowstone Plateau Volcanic Field, USA. The Ge/Si ratio (µmol.mol −1 ) was determined for seven thermal water samples (183 ± 22), eight rivers (35 ± 23) and six creeks flowing into Yellowstone Lake (5 ± 3) during base flow and during peak water discharge following snowmelt. The δ 30 Si value (‰) was determined for thermal waters (−0.09 ± 0.04), Yellowstone River at Yellowstone Lake outlet (1.91 ± 0.23) and creek samples (0.82 ± 0.29). The calculated atmospheric CO 2 consumption associated with non-thermal waters flowing through Yellowstone's rivers during peak discharge is ∼3.03 ton.km −2 .yr −1 , which is ∼2% of the annual mean atmospheric CO 2 consumption in other volcanic regions. This study highlights the significance of quantifying seasonal variations in chemical weathering rates for improving estimates of atmospheric CO 2 consumption rates in active volcanic regions.
Wyoming↗
Evidence for fluctuating wind in shaping an ancient Martian dune field: The Stimson formation at the Greenheugh pediment, Gale crater
Temporal fluctuations of wind strength and direction can influence aeolian bedform morphology and orientation, which can be encoded into the architecture of aeolian deposits. These strata represent a direct record of atmospheric processes and can be used to understand ancient Martian atmospheric processes as well as those on Earth. The strata can: give insight to ancient atmospheric circulation, how the atmosphere evolved in response to global changes in habitability, and how ancient processes differ from modern processes. The Stimson formation at the Greenheugh pediment (Gale crater) records evidence of fluctuating wind across multiple temporal scales. The strata can be subdivided into three intervals–Gleann Beag, Ladder, and Edinburgh intervals. Internally, the intervals record changes of dune morphology and orientation, correlatable to wind fluctuations at multiple temporal scales. The basal Gleann Beag interval comprises compound cross-strata, deposited by oblique compound dunes. These dunes record a bimodal wind regime, resulting in net sediment transport toward the north. The Ladder interval records a reversal of sediment transport to the south, where straight-crested simple-dunes shaped by a seasonally variable winds formed. Finally, the Edinburgh interval records sediment transport to the west, where a unimodal wind formed sinuous-crested simple dunes. These observations demonstrate active and variable atmospheric circulation in Gale crater during the accumulation of the Stimson dune field, at multiple temporal scales from seasonally driven winds to much longer time-frames, during the Hesperian. These observations can be used to further understand ancient atmospheric conditions and processes, at a high temporal resolution on Mars.
Journal of Geophysical Research - Planets↗
Possible solar noble-gas component in Hawaiian basalts
The noble-gas elemental and isotopic composition in the Earth is significantly different from that of the present atmosphere, and provides an important clue to the origin and history of the Earth and its atmosphere. Possible candidates for the noble-gas composition of the primordial Earth include a solar-like component, a planetary-like component (as observed in primitive meteorites) and a component similar in composition to the present atmosphere. In an attempt to identify the contributions of such components, we have measured isotope ratios of helium and neon in fresh basaltic glasses dredged from Loihi seamount and the East Rift Zone of Kilauea 1–3 . We find a systematic enrichment in 20 Ne and 21 Ne relative to 22 Ne, compared with atmospheric neon. The helium and neon isotope signatures observed in our samples can be explained by mixing of solar, present atmospheric, radiogenic and nucleogenic components. These data suggest that the noble-gas isotopic composition of the mantle source of the Hawaiian plume is different from that of the present atmosphere, and that it includes a significant solar-like component. We infer that this component was acquired during the formation of the Earth.
Hawaii↗