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8 recordsLinked to original sources
USGS2010

Patterns of mercury dispersion from local and regional emission sources, rural Central Wisconsin, USA

Simultaneous real-time changes in mercury (Hg) speciation-reactive gaseous Hg (RGM), elemental Hg (Hg??), and fine particulate Hg (Hg-PM 2.5 ), were determined from June to November 2007, in ambient air at three locations in rural Central Wisconsin. Known Hg emission sources within the airshed of the monitoring sites include: 1) a 1114 megawatt (MW) coal-fired electric utility generating station; 2) a Hg-bed chlor-alkali plant; and 3) a smaller (465 MW) coal-burning electric utility. Monitoring sites, showing sporadic elevation of RGM, Hg o and Hg-PM 2.5 , were positioned at distances of 25, 50 and 100 km northward of the larger electric utility. A series of RGM events were recorded at each site. The largest, on 23 September, occurred under prevailing southerly winds, with a maximum RGM value (56.8 pg m -3 ) measured at the 100 km site, and corresponding elevated SO 2 (10.41 ppbv; measured at 50 km site). The finding that RGM, Hg o , and Hg-PM 2.5 are not always highest at the 25 km site, closest to the large generating station, contradicts the idea that RGM decreases with distance from a large point source. This may be explained if: 1) the 100 km site was influenced by emissions from the chlor-alkali facility or by RGM from regional urban sources; 2) the emission stack height of the larger power plant promoted plume transport at an elevation where the Hg is carried over the closest site; or 3) RGM was being generated in the plume through oxidation of Hg o . Operational changes at each emitter since 2007 should reduce their Hg output, potentially allowing quantification of the environmental benefit in future studies.

Atmospheric Chemistry and Physics Discussions↗
USGS2010

Enhancement of the volcanogenic "bromine explosion" via reactive nitrogen chemistry (Kīlauea volcano, Hawai'i)

Since the first detection of bromine monoxide in volcanic plumes attention has focused on the atmospheric synthesis and impact of volcanogenic reactive halogens. We report here new measurements of BrO in the volcanic plume emitted from Kīlauea volcano – the first time reactive halogens have been observed in emissions from a hotspot volcano. Observations were carried out by ground-based Differential Optical Absorption Spectroscopy in 2007 and 2008 at Pu'u' O ' o crater, and at the 2008 magmatic vent that opened within Halema'uma'u crater. BrO was readily detected in the Halema'uma'u plume (average column amount of 3×1015 molec cm −2 ) and its abundance was strongly correlated with that of SO 2 . However, anticorrelation between NO 2 and SO 2 (and BrO) abundances in the same plume strongly suggest an active role of NO x in reactive halogen chemistry. The calculated SO 2 /BrO molar ratio of ~1600 is comparable to observations at other volcanoes, although the BrO mixing ratio is roughly double that observed elsewhere. While BrO was not observed in the Pu'u' O ' o plume this was probably merely a result of the detection limit of our measurements and based on understanding of the Summit and East Rift magmatic system we expect reactive halogens to be formed also in the Pu'u' O ' o emissions. If this is correct then based on the long term SO 2 flux from Pu'u' O ' o we calculate that Kīlauea emits ~480 Mg yr −1 of reactive bromine and may thus represent an important source to the tropical Pacific troposphere.

Hawaii↗
USGS2011

Changes in monoterpene mixing ratios during summer storms in rural New Hampshire (USA)

Monoterpenes are an important class of biogenic hydrocarbons that influence ambient air quality and are a principle source of secondary organic aerosol (SOA). Emitted from vegetation, monoterpenes are a product of photosynthesis and act as a response to a variety of environmental factors. Most parameterizations of monoterpene emissions are based on clear weather models that do not take into account episodic conditions that can drastically change production and release rates into the atmosphere. Here, the monoterpene dataset from the rural Thompson Farm measurement site in Durham, New Hampshire is examined in the context of a set of known severe storm events. While some storm systems had a negligible influence on ambient monoterpene mixing ratios, the average storm event increased mixing ratios by 0.59 ± 0.21 ppbv, a factor of 93 % above pre-storm levels. In some events, mixing ratios reached the 10’s of ppbv range and persisted overnight. These mixing ratios correspond to increases in the monoterpene emission rate, ranging from 120 to 1240 g km−2 h −1 compared to an estimated clear weather rate of 116 to 193 g km−2 h −1 . Considering the regularity of storm events over most forested areas, this could be an important factor to consider when modeling global monoterpene emissions and their resulting influence on the formation of organic aerosols.

New Hampshire↗
USGS2007

A new comprehensive approach to characterizing carbonaceous aerosol with an application to wintertime Fresno, California PM2.5

Fine particulate matter (PM2.5) samples were collected during a three week winter period in Fresno (CA). A composite sample was characterized by isolating several distinct fractions and characterizing them by infrared and nuclear magnetic resonance (NMR) spectroscopy. More than 80% of the organic matter in the aerosol samples was recovered and characterized. Only 35% of the organic matter was water soluble with another third soluble in dichloromethane and the remainder insoluble. Within the isolated water soluble material, hydrophobic acid and hydrophilic acids plus neutrals fractions contained the largest amounts of carbon. The hydrophobic acids fraction appears to contain significant amounts of lignin type structures, spectra of the hydrophilic acids plus neutrals fraction are indicative of carbohydrates and secondary organic material. The dichloromethane soluble fraction contains a variety of organic compound families typical of many previous studies of organic aerosol speciation, including alkanes, alkanols, alkanals and alkanoic acids. Finally the water and solvent insoluble fraction exhibits a strong aromaticity as one would expect from black or elemental carbon like material; however, these spectra also show a substantial amount of aliphaticity consistent with linear side chains on the aromatic structures.

Atmospheric Chemistry and Physics Discussions↗
USGS2025

Ultraviolet and visible remote sensing of volcanic gases

As magma rises in volcanic systems, volatile species exsolve from the silicate melt and are emitted as gases into the atmosphere. Measuring the magnitude and composition of gas emissions from volcanoes provides insights into processes occurring deep within the Earth and helps constrain the impact of volcanic degassing on atmospheric chemistry. Optical remote sensing techniques allow volcanic gas emissions to be characterized without the need to access hazardous areas near active volcanic vents. This paper reviews the state of the art in ultraviolet and visible volcanic gas remote sensing from the ground, air, and space. Special attention is given to discussing the physics of atmospheric radiative transfer on which these techniques are based. The functionality and limitations of different remote sensing instruments are examined, making clear that the ideal choice of instrumentation will depend on the volcanic system to which it is applied and the sought measurement parameters. Common algorithms for determining trace gas column densities, gas burdens, and volcanic emission rates from measurements of spectral radiance are outlined and compared, showing how some algorithms attempt to model the physics of the measurement while others maximize sensitivity. Several examples demonstrate how remote sensing measurements continue to advance our understanding of volcanic systems and their impact on the atmosphere. Finally, a few promising directions of inquiry are suggested that could lead to improvements in remote sensing instrumentation and analysis techniques. By combining spectroscopic and imaging techniques, improving our understanding of atmospheric radiative transfer, expanding the suite of target gases, and increasing the coverage and frequency of observations, we stand to significantly improve our ability to detect and quantify volcanic gas emissions and gain new insights into important Earth-system processes.

Journal of Volcanology and Geothermal Research↗
USGS2006

Methods for measuring denitrification: Diverse approaches to a difficult problem

Denitrification, the reduction of the nitrogen (N) oxides, nitrate (NO 3 − ) and nitrite (NO 2 − ), to the gases nitric oxide (NO), nitrous oxide (N 2 O), and dinitrogen (N 2 ), is important to primary production, water quality, and the chemistry and physics of the atmosphere at ecosystem, landscape, regional, and global scales. Unfortunately, this process is very difficult to measure, and existing methods are problematic for different reasons in different places at different times. In this paper, we review the major approaches that have been taken to measure denitrification in terrestrial and aquatic environments and discuss the strengths, weaknesses, and future prospects for the different methods. Methodological approaches covered include (1) acetylene-based methods, (2) 15 N tracers, (3) direct N 2 quantification, (4) N 2 :Ar ratio quantification, (5) mass balance approaches, (6) stoichiometric approaches, (7) methods based on stable isotopes, (8) in situ gradients with atmospheric environmental tracers, and (9) molecular approaches. Our review makes it clear that the prospects for improved quantification of denitrification vary greatly in different environments and at different scales. While current methodology allows for the production of accurate estimates of denitrification at scales relevant to water and air quality and ecosystem fertility questions in some systems (e.g., aquatic sediments, well-defined aquifers), methodology for other systems, especially upland terrestrial areas, still needs development. Comparison of mass balance and stoichiometric approaches that constrain estimates of denitrification at large scales with point measurements (made using multiple methods), in multiple systems, is likely to propel more improvement in denitrification methods over the next few years.

Ecological Applications↗
USGS2020

From pools to flow: The PROMISE framework for new insights on soil carbon cycling in a changing world

Soils represent the largest terrestrial reservoir of organic carbon, and the balance between soil organic carbon (SOC) formation and loss will drive powerful carbon‐climate feedbacks over the coming century. To date, efforts to predict SOC dynamics have rested on pool‐based models, which assume classes of SOC with internally homogenous physicochemical properties. However, emerging evidence suggests that soil carbon turnover is not dominantly controlled by the chemistry of carbon inputs, but rather by restrictions on microbial access to organic matter in the spatially heterogeneous soil environment. The dynamic processes that control the physicochemical protection of carbon translate poorly to pool‐based SOC models; as a result, we are challenged to mechanistically predict how environmental change will impact movement of carbon between soils and the atmosphere. Here, we propose a novel conceptual framework to explore controls on belowground carbon cycling: P robabilistic R epresentation of O rganic M atter I nteractions within the S oil E nvironment (PROMISE). In contrast to traditional model frameworks, PROMISE does not attempt to define carbon pools united by common thermodynamic or functional attributes. Rather, the PROMISE concept considers how SOC cycling rates are governed by the stochastic processes that influence the proximity between microbial decomposers and organic matter, with emphasis on their physical location in the soil matrix. We illustrate the applications of this framework with a new biogeochemical simulation model that traces the fate of individual carbon atoms as they interact with their environment, undergoing biochemical transformations and moving through the soil pore space. We also discuss how the PROMISE framework reshapes dialogue around issues related to SOC management in a changing world. We intend the PROMISE framework to spur the development of new hypotheses, analytical tools, and model structures across disciplines that will illuminate mechanistic controls on the flow of carbon between plant, soil, and atmospheric pools.

Global Change Biology↗
USGS2012

Structure, spectroscopy and dynamics of layered H2O and CO2 ices

Molecular dynamics simulations of structural, spectroscopic and dynamical properties of mixed water–carbon dioxide (H 2 O–CO 2 ) ices are discussed over temperature ranges relevant to atmospheric and astrophysical conditions. The simulations employ multipolar force fields to represent electrostatic interactions which are essential for spectroscopic and dynamical investigations. It is found that at the water/CO 2 interface the water surface acts as a template for the CO 2 component. The rotational reorientation times in both bulk phases agree well with experimental observations. A pronounced temperature effect on the CO 2 reorientation time is observed between 100 K and 200 K. At the interface, water reorientation times are nearly twice as long compared to water in the bulk. The spectroscopy of such ices is rich in the far-infrared region of the spectrum and can be related to translational and rotational modes. Furthermore, spectroscopic signatures mediated across the water/CO 2 interface are found in this frequency range (around 440 cm −1 ). These results will be particularly important for new airborne experiments such as planned for SOFIA.

Physical Chemistry Chemical Physics↗