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At least 109 records · Page 6

High sensitivity measurement of femtogram-level 238 Pu by thermal ionization mass spectrometry with correction of background 238 U

Low-concentration plutonium isotopic measurements provide a valuable fingerprint to identify possible material origins in the context of environmental contamination monitoring, environmental tracing, nuclear safeguards, nuclear forensics, and treaty monitoring. Thermal ionization mass spectrometry (TIMS) has long been recognized as one of the most sensitive techniques for plutonium isotopic measurement, but has not generally been utilized for 238 Pu determination, especially at low concentrations, due to an isobaric interference from 238 U, prevalent as background. Here, this work demonstrates a new analytical technique for correction of background 238 U from the 238 Pu counts collected during a TIMS analysis. The technique takes advantage of the higher ionization temperature of U relative to Pu and uses a 235 U tracer added after plutonium purification chemistry for 238 U semi-quantitative determination. This technique has been successfully applied to the determination of 238 Pu concentration and the 238 Pu/ 239 Pu ratio in sample types including single-isotope standards, isotopic certified reference materials, matrix-containing environmental reference materials, and simulated nuclear detonation debris. The results have been directly compared on a sample-by-sample basis to alpha spectrometry results. The detection limit by this new technique is 0.23 fg 238 Pu, which was previously unachievable by mass spectrometry and is possible in around 1 h of analysis time post-chemistry compared to weeks of required counting time by alpha spectrometry (at the same atom amount). We also present original, high precision data for Pu isotope concentrations in IAEA-384, Fangataufa Sediment, including 242 Pu results for the first time. The new technique allows measurement of a key isotope, 238 Pu, that was previously not measured in small environmental or nuclear forensics collections.

238Pu↗

The channel-source hypothesis: Empirical evidence for in-channel sourcing of dissolved organic carbon to explain hysteresis in a headwater mountain stream

Catchment hydrologists have long puzzled over the question: How can catchments rapidly generate storm flows and pulses of solutes in response to storm events? Conceptual models viewing catchments as composed of discrete source areas generating flow at unique time scales and with unique chemical characteristics have been used to explain the observed changes in flow and water chemistry. Surprisingly, those conceptual models usually do not treat the stream channel as one of the potential source areas. We propose the channel-source hypothesis in which the stream itself should be considered as a potential source with the same rigour as other contributing areas. We pose this in the spirit of the scientific use of the word: a hypothesis is not a proven idea but rather a provisional supposition serving as the basis for further study. We suggest that the channel should be considered as a potential source for dissolved organic carbon (DOC). Channels store substantial amounts of organic matter, and stream ecologists have long studied stream carbon cycling. From those studies, we know that leaching and decomposition can generate DOC from particulate organic carbon (POC). Further, POC is stored in channel ‘dead-zones’—regions of low flow velocity - that can be activated as flow velocity increases, thus releasing accumulated DOC during storms. All catchments are different; there is no reason to assume that channel sources are always important, in every catchment, in every storm. Thus, the channel-source hypothesis does not replace existing conceptual models. Instead, it adds another potential mechanism that may explain DOC dynamics observed in streams. The channel-source hypothesis has substantial implications for catchment studies examining sources of DOC in stream water or using DOC as a tracer to determine the locations of, and proportional contributions of, different source areas for streamflow generation.

54 ENVIRONMENTAL SCIENCES↗

On the Representation of Hyporheic Exchange in Models for Reactive Transport in Stream and River Corridors

Efforts to include more detailed representations of biogeochemical processes in basin-scale water quality simulation tools face the challenge of how to tractably represent mass exchange between the flowing channels of streams and rivers and biogeochemical hotspots in the hyporheic zones. Multiscale models that use relatively coarse representations of the channel network with subgrid models for mass exchange and reactions in the hyporheic zone have started to emerge to address that challenge. Two such multiscale models are considered here, one based on a stochastic Lagrangian travel time representation of advective pumping and one on multirate diffusive exchange. The two models are formally equivalent to well-established integrodifferential representations for transport of non-reacting tracers in steady stream flow, which have been very successful in reproducing stream tracer tests. Despite that equivalence, the two models are based on very different model structures and produce significantly different results in reactive transport. In a simple denitrification example, denitrification is two to three times greater for the advection-based model because the multirate diffusive model has direct connections between the stream channel and transient storage zones and an assumption of mixing in the transient storage zones that prevent oxygen levels from dropping to the point where denitrification can progress uninhibited. By contrast, the advection-based model produces distinct redox zonation, allowing for denitrification to proceed uninhibited on part of the hyporheic flowpaths. These results demonstrate that conservative tracer tests alone are inadequate for constraining representation of mass transfer in models for reactive transport in streams and rivers.

54 ENVIRONMENTAL SCIENCES↗

Investigating the Chemolithoautotrophic and Formate Metabolism of Nitrospira moscoviensis by Constraint-Based Metabolic Modeling and 13 C-Tracer Analysis

Nitrospira spp. are globally abundant nitrifying bacteria in soil and aquatic ecosystems and in wastewater treatment plants, where they control the oxidation of nitrite to nitrate. Despite their critical contribution to nitrogen cycling across diverse environments, detailed understanding of their metabolic network and prediction of their function under different environmental conditions remains a major challenge.

59 BASIC BIOLOGICAL SCIENCES↗

Studying Aerosol, Clouds, and Air Quality in the Coastal Urban Environment of Southeastern Texas

A multi-agency succession of field campaigns was conducted in southeastern Texas during July 2021 through October 2022 to study the complex interactions of aerosols, clouds and air pollution in the coastal urban environment. As part of the Tracking Aerosol Convection interactions Experiment (TRACER), the TRACER- Air Quality (TAQ) campaign the Experiment of Sea Breeze Convection, Aerosols, Precipitation and Environment (ESCAPE) and the Convective Cloud Urban Boundary Layer Experiment (CUBE), a combination of ground-based supersites and mobile laboratories, shipborne measurements and aircraft-based instrumentation were deployed. These diverse platforms collected high-resolution data to characterize the aerosol microphysics and chemistry, cloud and precipitation micro- and macro-physical properties, environmental thermodynamics and air quality-relevant constituents that are being used in follow-on analysis and modeling activities. We present the overall deployment setups, a summary of the campaign conditions and a sampling of early research results related to: (a) aerosol precursors in the urban environment, (b) influences of local meteorology on air pollution, (c) detailed observations of the sea breeze circulation, (d) retrieved supersaturation in convective updrafts, (e) characterizing the convective updraft lifecycle, (f) variability in lightning characteristics of convective storms and (g) urban influences on surface energy fluxes. The work concludes with discussion of future research activities highlighted by the TRACER model-intercomparison project to explore the representation of aerosol-convective interactions in high-resolution simulations.

54 ENVIRONMENTAL SCIENCES↗

TRACER Lightning Mapping Array Field Campaign Report

Our observational contribution to the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s Tracking Aerosol Convection Interactions Experiment (TRACER) was the deployment of additional Lightning Mapping Array sensors to provide enhanced capability to the Houston Lightning Mapping Array (HLMA) during the TRACER intensive operational period. To that end, the Texas Tech University personnel (Professor Bruning and Dr. Brunner, and graduate students Jessica Souza, David Singewald, Stephanie Weiss, and Matthew Miller) deployed two portable LMA antennae at locations G and B shown in the map below. The map also shows the predicted lightning flash detection efficiency in black contours, as well as color-shaded very-high-frequency (VHF) source detection efficiency, which roughly corresponds to the sensitivity to lightning channel detail. Feeds from these sensors were integrated in the HLMA processing in real-time and in post-processing, partially leveraging National Science Foundation support through the TRACER campaign that supported the core HLMA, operated by Timothy Logan.

54 ENVIRONMENTAL SCIENCES↗

TRACER CLAMPS1 Doppler Lidar VAD Data

These files contain 24 hour periods of data collected from the CLAMPS1 Halo Streamline XR Doppler lidar. The Doppler lidar conducts regular conical scans at a set elevation angle. These data are then passed through a typical VAD algorithm to retrieve horizontal wind speed and direction profiles. These data were collected during the TRACER project. For the TRACER campaign, the CLAMPS1 Doppler lidar collected PPI scans at 70 deg elevation every 20 minutes.

54 ENVIRONMENTAL SCIENCES↗

TRACER Radar b1 Data Processing: Corrections, Calibrations, and Processing Report

The U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility deployed the first ARM Mobile Facility (AMF1) to Houston, Texas for the Tracking Aerosol Convection Interactions Experiment (TRACER) field campaign. The TRACER campaign was conducted from October 1, 2021 to September 30, 2022, with an intensive operational period (IOP) from June 1 to September 30, 2022. To investigate the life cycles of convective cells in the polluted and humid urban environment of Houston, ARM deployed cloud and precipitation radars, including the C-band Scanning ARM Precipitation Radar (CSAPR2), the X/Ka-band Scanning ARM Cloud Radar (SACR), and the Ka-band ARM Zenith cloud Radar (KAZR), as shown in Figure 1. This report presents an analysis of radar data quality, hardware calibrations, and radar data corrections.

54 ENVIRONMENTAL SCIENCES↗

Spectro-Microscopic Investigation of the Aerosol Impact on Hydrological Processes

This project investigated physico-chemical characteristics of atmospheric particles collected during DOE ARM field campaigns and how they are involved in the hydrological cycle. Our efforts were focused on multi-modal chemical imaging and molecular characterization of atmospheric particles and snow samples collected during the Surface-Atmosphere Integrated Field Laboratory (SAIL) campaign and particle samples from the Tracking Aerosol Convection Interactions ExpeRiment (TRACER) campaign.

54 ENVIRONMENTAL SCIENCES↗

Simulated Dust Transport in the Convective Boundary Layer

Soil dusts are an important source of aerosol in agricultural regions and can affect the Earth's radiation budget through the modification of cloud properties, and in particular, through their ability to act as ice nucleating particles. In order to impact cloud properties, agricultural soil dusts need to be transported from the point of emission to cloud–relevant altitudes. Vertical transport within the planetary boundary layer is strongly controlled by turbulence and is challenging to represent accurately in regional and global models. Large–eddy simulations (LES) are run at resolutions capable of resolving most of the turbulent energy directly and can thus better simulate vertical transport. In this study, we leverage the LES ARM Symbiotic Simulation and Observation (LASSO) large–eddy simulations to simulate vertical transport of agricultural dust within the turbulent boundary layer using a modified version of the stochastic dispersion model FLEXPART–WRF. We find that the modified model is better capable of simulating particle transport due to turbulence, and that particle size was the greatest factor in determining particle lifetime. Individual meteorology and particle density had intermediate effects upon particle transport, while release height had little effect upon simulation results. Finally, we utilize a quasi–single column model (QSCM) approach to determine how our results compare to a parameterized treatment of turbulence. The QSCM simulations led to greater tracer transport out of the boundary layer, with ramifications for any studies utilizing a Lagrangian stochastic model to understand tracer dispersion. Furthermore, these results highlight the importance of accurately simulating turbulence for understanding particle transport.

54 ENVIRONMENTAL SCIENCES↗

TRACER CLAMPS1 AERI TROPoe Retrievals

These files contain 24 hour periods of retrieved thermodynamic profiles derived from observations collected by the CLAMPS1 Atmospheric Emitted Radiance Interferometer (AERI). The TROPoe algorithm is a python equivalent to the AERIoe algorithm (see Turner and Loehnert 2014; Turner and Blumberg 2019). These data were collected during the TRACER-CUBIC project. Due to issues with the CLAMPS1 microwave radiometer, only retrievals that used AERI data are available.

54 ENVIRONMENTAL SCIENCES↗

Influences of Environmental Relative Humidity and Horizontal Scale of Subcloud Ascent on Deep Convective Initiation

This study examines two factors impacting initiation of moist deep convection: free-tropospheric environmental relative humidity (φ E ) and horizontal scale of subcloud ascent (R sub ), the latter exerting a dominant control on cumulus cloud width. A simple theoretical model is used to formulate a “scale selection” hypothesis: that a minimum R sub is required for moist convection to go deep, and that this minimum scale decreases with increasing φ E . Specifically, the ratio of R 2 sub to saturation deficit (1 - φ E ) must exceed a certain threshold value that depends on cloud-layer environmental lapse rate. Idealized, large-eddy simulations of moist convection forced by horizontally varying surface fluxes show strong sensitivity of maximum cumulus height to both φ E and R sub consistent with the hypothesis. Increasing R sub by only 300–400 m can lead to a large increase (>5 km) in cloud height. A passive tracer analysis shows that the bulk fractional entrainment rate decreases rapidly with R sub but depends little on φ E . However, buoyancy dilution increases as either R sub or φ E decreases; buoyancy above the level of free convection is rapidly depleted in dry environments when R sub is small. While deep convective initiation occurs with an increase in relative humidity of the near environment from moistening by earlier convection, the importance of this moisture preconditioning is inconclusive as it is accompanied by an increase in R sub . Overall, it is concluded that small changes to R sub driven by external forcing or by convection itself could be a dominant regulator of deep convective initiation.

54 ENVIRONMENTAL SCIENCES↗

Investigating Mountain Watershed Headwater‐To‐Groundwater Connections, Water Sources, and Storage Selection Behavior With Dynamic‐Flux Particle Tracking

Abstract Climate change will impact mountain watershed streamflow both directly—with changing precipitation amounts and variability—and indirectly—through temperature shifts altering snowpack, melt, and evapotranspiration. To understand how these complex processes will affect ecosystem functioning and water resources, we need tools to distinguish connections between water sources (rain/snowmelt), groundwater storage, and exit fluxes (streamflow/evapotranspiration), and to determine how these connections change seasonally and as climate shifts. Here, we develop novel watershed‐scale approaches to understand water source, storage, and exit flux connections using a dynamic‐flux particle tracking model (EcoSLIM) applied in California's Cosumnes Watershed, which connects the Sierra Nevada and Central Valley. This work develops new visualizations and applications to provide mechanistic understanding that underpins the interpretation of isotopic field data at watershed scales to distinguish sources, flow paths, residence times, and storage selection. In our simulations, streamflow comes primarily from snow‐derived water while evapotranspiration generally comes from rain. Most streamflow starts above 1,000 m while evapotranspiration is sourced relatively evenly across the watershed and is generally younger than streamflow. Modeled streamflow consists primarily of water sourced from precipitation in the previous 5 years but before the current water year, while ET consists primarily of water from precipitation in the current water year. ET, and to a lesser extent streamflow, are both younger than water in groundwater storage. However, snowmelt‐derived streamflow preferentially discharges older water from snow‐derived storage. Dynamic‐flux particle tracking and new approaches presented here enable novel model‐tracer comparisons in large‐scale watersheds to better understand watershed behavior in a changing climate.

54 ENVIRONMENTAL SCIENCES↗

WellSTIC: A Cost-Effective Sensor for Performing Point Dilution Tests to Measure Groundwater Velocity in Shallow Aquifers

Many individual measurement points are required to characterize groundwater velocity within an aquifer. Groundwater velocity is most commonly measured using a network of >5 cm diameter monitoring wells, which, if not already present at a site, are expensive and labor-intensive to install. Drive-point piezometers—simple, cost-effective wells that can be installed by hand—are a common tool for sampling groundwater in shallow, alluvial aquifers, but most groundwater velocity measurement techniques require equipment that is too large for these narrow (usually <2 cm inside diameter) piezometers. In this technical note, we introduce a low-cost sensor and well packer system (<$90 USD) for performing point dilution tests in narrow piezometers. Field data show that the magnitude of groundwater velocity measured with this technique agrees with velocities computed from natural gradient tracer tests. Additionally, with proper calibration, these sensors can be used to continuously monitor in-well specific conductance, either during inter-well tracer tests with saline tracers or for water quality monitoring. Finally, this system is a viable tool for rapid assessment of the magnitude of groundwater velocity in shallow aquifers.

54 ENVIRONMENTAL SCIENCES↗

Single-cell stable isotope probing in microbial ecology

Abstract Environmental and host-associated microbiomes are typically diverse assemblages of organisms performing myriad activities and engaging in a network of interactions that play out in spatially structured contexts. As the sum of these activities and interactions give rise to overall microbiome function, with important consequences for environmental processes and human health, elucidating specific microbial activities within complex communities is a pressing challenge. Single-cell stable isotope probing (SC-SIP) encompasses multiple techniques that typically utilize Raman microspectroscopy or nanoscale secondary ion mass spectrometry (NanoSIMS) to enable spatially resolved tracking of isotope tracers in cells, cellular components, and metabolites. SC-SIP techniques are uniquely suited for illuminating single-cell activities in microbial communities and for testing hypotheses about cellular functions generated for example from meta-omics datasets. Here, we illustrate the insights enabled by SC-SIP techniques by reviewing selected applications in microbiology and offer a perspective on their potential for future research.

Alcolombri, Uria (ORCID:0000000335615091)↗