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At least 19 records

Accurate and efficient measurement of impurity (dilute) diffusion coefficients without isotope tracer experiments

We report most impurity diffusion coefficients were measured in the 1960s and 1970s using tracer experiments with only 14 sets of tracer measurements performed worldwide in the past 15 years. It is thus impractical to rely on tracer experiments to obtain the missing thousands of impurity diffusion coefficients. A recently developed forward-simulation analysis can change the scenario by reliably extracting impurity diffusion coefficients from regular diffusion couple profiles. A comparison of 51 values obtained from the forward-simulation analysis with tracer experiment values in the literature shows an excellent agreement, thus validating the reliability of the forward-simulation analysis in obtaining accurate impurity diffusion coefficients.

36 MATERIALS SCIENCE↗

Standoff Detection of Chemical Plumes Using Swept-ECQCL Remote Detection Technology: Results from EMRTC Complex Terrain Dual Tracer Experiment

As part of the Complex Terrain Dual Tracer Experiments performed in support of the LYNM program, a swept-wavelength external cavity quantum cascade laser (swept-ECQCL) remote detection system was deployed to measure chemical plume propagation with high temporal resolution. The swept-ECQCL remote detection technology was initially developed at PNNL, and is now under further development at Opticslah, LLC under SBIR funding from DOE (DOE SBIR Phase I Project DE-SC0019855, Remote Detection Technologies, Program Manager Chris Ramos). The swept-ECQCL technology provides a single-frequency infrared laser source which is rapidly scanned over a large wavelength range to measure the infrared absorption of gases, liquids, or solids. Analysis of the measured infrared absorption spectrum is used to detect, identify, and quantify the chemical species which are present. While most previous laser-based techniques used small wavelength tuning ranges to measure only a few isolated spectral lines of a few species, the swept-ECQCL provides the large tuning range needed to measure multiple species simultaneously, and to detect broad absorption features from large molecules or condensed phase materials. In addition, the swept-ECQCL systems have high enough spectral resolution and sensitivity to measure narrow lines of small molecules and determine isotope ratios. The remote detection system for gas plumes is based on the swept-ECQCL technology, and consists of a swept-ECQCL source, infrared detector, control electronics, and beam transmitting and alignment optics. The remote detection system directs the infrared output of the swept-ECQCL to a target retro reflector typically located at ~10-10,000 m distance. The swept-ECQCL wavelength is varied continuously over a large wavelength range (>1000 nm) at rates up to 1000 Hz. The swept ECQCL light reflected from the remote target is collected and focused onto an infrared photodetector. By measuring the detector signal continuously as the swept-ECQCL wavelength is varied, a time-series of absorption spectra are measured for the gases along the beam line of-sight. Based on analysis and fitting of the measured absorption spectra, the time-dependent chemical concentrations of species are determined. Multiple species and mixtures can be detected simultaneously, for all species with absorption features above the sensor noise floor. The sensor output is thus a continuous, high-speed record of identified chemicals along with their concentrations and isotope ratios of interest. The high-speed operation enables low-noise operation in conditions of atmospheric turbulence and allows tracking of fluctuating concentrations in transient chemical plumes as needed for reliable remote detection applications. All components operate with minimal cooling requirements and no cryogens are needed. In addition, the output infrared light is invisible with an intensity below the maximum permissible exposure (MPE) threshold of 100 mW/cm2 for these infrared wavelengths and thus eye safe. The measurement concept for plume detection using the swept-ECQCL remote detection system is as follows. The ECQCL beam is directed toward a remote retro-reflector, which reflects the beam back to the ECQCL system where it is focused onto an infrared photodetector. The line-of-sight from the ECQCL system to the retro-reflector defines the measurement path. The detected infrared signal is recorded continuously and detects the absorption of molecular species along the measurement path. Before a plume release, the system measures absorption from atmospheric constituents, which in this LWIR band consist primarily of lines from H 2 O and CO 2 , with additional weaker absorption from N 2 O, NH 3 , and O 3 possibly contributing. The system then measures any changes in absorption due to the tracer compounds when they enter the measurement path. The shape of absorption features is used to distinguish and identify the different tracer compounds, and the strength of the absorption is used to determine the path-integrated concentration – also called the column density.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

An Overview of the EMRTC Complex-Terrain Dual-Tracer Experiment

LANL, in collaboration with LLNL, PNNL, Telops, University of Arizona, USARL, and EMRTC conducted exploratory atmospheric tracer experiments at EMRTC’s Field Laboratory in the nearby Socorro Mountains of New Mexico the first week of November, 2019.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Data collected using small uncrewed aircraft systems during the TRacking Aerosol Convection interactions ExpeRiment (TRACER)

Abstract. The main goal of the TRacking Aerosol Convection interactions ExpeRiment (TRACER) project was to further understand the role that regional circulations and aerosol loading play in the convective cloud life cycle across the greater Houston, Texas, area. To accomplish this goal, the United States Department of Energy and research partners collaborated to deploy atmospheric observing systems across the region. Cloud and precipitation radars, radiosondes, and air quality sensors captured atmospheric and cloud characteristics. A dense lower-atmospheric dataset was developed using ground-based remote sensors, a tethersonde, and uncrewed aerial systems (UASs). TRACER-UAS is a subproject that deployed two UAS platforms to gather high-resolution observations in the lower atmosphere between 1 June and 30 September 2022. The University of Oklahoma CopterSonde and the University of Colorado Boulder RAAVEN (Robust Autonomous Aerial Vehicle – Endurant Nimble) were flown at two coastal locations between the Gulf of Mexico and Houston. The University of Colorado Boulder RAAVEN gathered measurements of atmospheric thermodynamic state, winds and turbulence, and aerosol size distribution. Meanwhile, the University of Oklahoma CopterSonde system operated on a regular basis to resolve the vertical structure of the thermodynamic and kinematic state. Together, a complementary dataset of over 200 flight hours across 61 d was generated, and data from each platform proved to be in strong agreement. In this paper, the platforms and respective data collection and processing are described. The dataset described herein provides information on boundary layer evolution, the sea breeze circulation, conditions prior to and nearby deep convection, and the vertical structure and evolution of aerosols. The quality-controlled TRACER-UAS observations from the CopterSonde and RAAVEN can be found at https://doi.org/10.5439/1969004 (Lappin, 2023) and https://doi.org/10.5439/1985470 (de Boer, 2023), respectively.

54 ENVIRONMENTAL SCIENCES↗

Determination of the oxide scale growth mechanism using 18O-tracer experiments in combination with Transmission Electron Microscopy and nanoscale Secondary Ion Mass Spectrometry

Highlights: • {sup 18}O-tracer experiments to determine oxide scale growth mechanism on a Fe-Cr alloy. • Cr{sub 2}O{sub 3} scale growth primarily by means of metal outwards diffusion in air at 850 °C • nanoSIMS mapping on TEM lamella more accurate than SIMS sputter depth profiling • nanoSIMS mapping on TEM lamella reveal information about local oxide growth. • Strong local variation of oxide scale growth - Abstract: Two-stage {sup 18}O{sub 2}/{sup 16}O{sub 2} exposures can be used to investigate the effect that alloying elements, secondary phases, or surface treatments have on the high temperature oxidation behaviour of certain materials. During subsequent exposures to {sup 16}O{sub 2}- and {sup 18}O{sub 2}-rich atmospheres, {sup 16}O- and {sup 18}O-rich layers are formed. Analysis of the layers using Secondary Ion Mass Spectrometry (SIMS) depth profiling allows for conclusions to be drawn about the oxide scale growth mechanism. The conclusions are, however, not entirely unambiguous due to the limited lateral resolution of the technology. Rough surface topography and the thickness variation of the oxide scale over the analysed volume add to the ambiguity of the findings. In this study, an Fe-20%Cr alloy was exposed to both {sup 18}O- and {sup 16}O-rich environments at 850 °C. Two methods were used to analyse the thermally grown Cr{sub 2}O{sub 3} scale: (1) traditional SIMS depth profiling and (2) preparation of a cross-sectional lamellae for Transmission Electron Microscopy (TEM), which, subsequently, was analysed in a NanoSIMS. The NanoSIMS {sup 16}O and {sup 18}O elemental maps were then superimposed on the TEM image. In comparison with traditional SIMS depth profiling, the nanoSIMS elemental maps reveal detailed information about local oxide growth in different parts of an oxide scale. Moreover, a clear {sup 16}O/{sup 18}O interface can be seen in the nanoSIMS maps, which is not the case in the sputter depth profiles. The findings of this study show that the aforementioned issues associated with sputter depth profiling can be eliminated by mapping a cross-section of an oxide scale using high resolution nanoSIMS.

36 MATERIALS SCIENCE↗

The Joint Ninth Aerosol, Clouds, Precipitation and Climate (ACPC) initiative and TRacking Aerosol Convection interactions ExpeRiment (TRACER) Workshop

The joint ninth Aerosols-Clouds-Precipitation-and-Climate (ACPC; http://www.acpcinitiative.org) initiative and TRacking Aerosol Convection interactions ExpeRiment (TRACER; Jensen et al., 2022) workshop was convened from 16–19 May 2023 at Texas Southern University (TSU), Houston, TX, and online to discuss progress towards understanding the interactions among aerosols, clouds, precipitation, and climate.

54 ENVIRONMENTAL SCIENCES↗

Tracking Aerosol Convective Interactions Experiment (TRACER) Science Plan

Convective clouds play an important role in the Earth’s climate system as a driver of large-scale circulations and a primary mechanism for the transport of heat, moisture, aerosols, and momentum throughout the troposphere. Despite their climatic importance, multi-scale models continue to have persistent biases produced by insufficient representation of convective clouds. This is the result of an incomplete understanding of key processes such as convective initiation, updraft and downdraft dynamics, cloud and precipitation microphysics, and aerosol-convection interactions. The Aerosol-Cloud-Precipitation-Climate Initiative, an international research group dedicated to advancing understanding of aerosol impacts on clouds relevant to climate, has identified the Houston, Texas region as an optimal location for targeted studies of aerosol-convection interactions within frequently developing isolated deep convection. Houston lies within a humid subtropical climate regime, where onshore flow and sea-breeze convection interact with a range of aerosol conditions associated with Houston’s urban and industrial emissions. Pilot studies have suggested that convective clouds in this region are potentially significantly impacted by the varying aerosol conditions. To increase our understanding of convective cloud life cycles and aerosol-convection interactions, the Tracking Aerosol Convection Interactions Experiment (TRACER) aims to collect a comprehensive data set focused on the evolution of convective clouds and the environment (including aerosol, cloud, thermodynamics, and lightning) in which the clouds initiate, grow, and decay. A unique component of TRACER is that a large number of individual, isolated convective cells will be tracked and measured in high spatial and temporal resolution for the purposes of: (i) Characterizing and linking convective cloud kinematic and microphysical life cycles, (ii) Quantifying environmental thermodynamic and kinematic controls on convective life cycle properties, (iii) Isolating and quantifying the impacts of aerosol properties on convective cloud kinematic and microphysical evolution. TRACER includes a one-year deployment of the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility’s first ARM Mobile Facility (AMF1) and second-generation C-Band Scanning ARM Precipitation Radar (CSAPR2) aimed at collecting statistical data sets of cloud, precipitation, atmospheric state, and aerosol under varying aerosol loading and local circulation (sea breeze and urban heat island) conditions. A four-month intensive operational period (IOP) from June through September will include deployment of an ancillary site with aerosol, atmospheric state, and precipitation measurements at a location rarely impacted by Houston’s anthropogenic emissions, which will be commonplace near the AMF1 site. Convective cell tracking by the CSAPR2 will provide high-resolution polarimetric and velocity observations under a range of environmental (including aerosol loading) conditions. High-frequency radiosonde launches will capture quickly evolving thermodynamic and kinematic conditions near convective cells, a requirement for isolating aerosol effects on clouds. TRACER will additionally leverage a lightning mapping array, surface meteorological networks, and air pollution networks, and proposals will be entered to deploy additional mobile radar and radiosonde assets during the IOP. This unique combination of cloud, precipitation, lightning, aerosol, and atmospheric state measurements associated with tracked convective cells will ultimately improve our understanding of the convective cloud life cycle and its interaction with individual environmental factors such that improved, next-generation cumulus, microphysics, turbulence, and aerosol parameterizations can be designed.

Convective clouds, aerosols, cloud life cycle, atm↗

A deliberate tracer experiment in Santa Monica Basin

A tracer technique was developed for measurements of diffusion across oceanic density strata using SF6 and perfluorodecalin (PFD) tracers in the Santa Monica Basin. Fifty days after injection, the tracers were found to have mixed along the isopycnal surface to nearly every part of the basin. The diapycnal spreading of the tracer distributions yielded an apparent eddy diffusivity of 0.33 + or - 0.08 sq cm/s at the ambient density gradient of 4.0 + or - 0.5 x 10 to the -9th g/cm to the 4th.

Ledwell, J. R.↗

Detecting 127 Xe in an atmospheric tracer experiment

The Xcounts algorithm for calculating air concentrations of radioactive xenon isotopes (Eslinger et al., 2023) has been extended to estimate 127 Xe in addition to 131m Xe, 133m Xe, 133 Xe, and 135 Xe. The algorithm was applied to 119 samples collected with a SAUNA Q B system (Ringbom et al., 2023) during a two-month atmospheric tracer release experiment. Finally, the algorithm identified two samples with 127 Xe present from a single 1.5 h release about 3.5 km upwind of the sampler and no false detections of 127 Xe were observed in the other samples.

127Xe calibration↗

Interpretation of Tracer Experiments on Inverted Five-spot Well-patterns within the Western Half of the Farnsworth Unit Oil Field

The Southwest Carbon Partnership (SWP), one of the U.S. Department of Energy (U.S. DOE) seven Regional Carbon Sequestration Partnerships, is currently working to demonstrate the utilization and storage of CO 2 in the Farnsworth Unit (FWU) Enhanced Oil Recovery (EOR) site under the final development phase of this U.S. DOE initiative. A component of the research is to use fluid tracers to understand the multifluid flow patterns that develop between injection and production wells via collected field data and supporting numerical reservoir models. The FWU, located in the Anadarko Basin, Ochiltree County, Texas, and being operated by Chaparral Energy, is a mature EOR water-flood field, which is currently being converted to a CO 2 flow, with inverted 5-spot patterns transitioning from pure water to alternating CO 2 and water floods (i.e., water alternating gas (WAG)) at an approximate rate of one every 6 to 10 months. The SWP tracer program is conducting a suite of tracer injections into the active 5-spot patterns at the FWU. Tracers have been selected to be nonreactive and either principally soluble in CO 2 (gas soluble) or water (aqueous soluble). In addition to characterizing the multifluid flow behaviour within reservoir, the gas and aqueous tracers have roles in detecting any leakage from the reservoir. A total of seven unique perfluorocarbon tracer (PFT) compounds make up the suite of gas soluble tracers and eight unique naphthalene sulfonate tracer (NPT) compounds comprise the aqueous soluble tracers. Lastly, all selected tracers are significantly detectable below the parts per billion concentrations, allowing for high resolution for the inter-well tests at relatively low injection volumes.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

The Santa Monica Basin Tracer Experiment - A study of diapycnal and isopycnal mixing

Cross isopycnal (diapycnal) and lateral mixing and stirring below the sill of Santa Monica Basin were studied by releasing two tracers, sulfur hexafluoride and perfluorodecalin, as close as possible to an isopycnal surface and measuring their subsequent dispersion. The target for the release was a potential temperature surface at about 790 m depth, roughly 100 m above the bottom and 50 m below the sill. Three surveys, performed immediately after, about 7 weeks after, and about 6 months after the release, showed that the time scales for lateral stirring and mixing in the basin were between 2 and 5 months. The diapycnal diffusivity for the whole period was found to be 0.29 + or - 0.06 sq cm/s near the injection surface, where the buoyancy frequency was about 1.1 cph. This estimate may include some mixing in the turbulent boundary layer near the walls of the basin. The best estimate for the diapycnal diffusivity in the basin interior is 0.25 + or - 0.08 sq cm/s.

Ledwell, James R.↗

Tracking Aerosol Convection Interactions Experiment (TRACER) Field Campaign Report

Convective clouds serve a critical role in the Earth’s energy and water cycles through their transport of heat, moisture, momentum, and chemical species through the troposphere driving the global circulation (e.g., Hartmann et al. 1984, Del Genio et al. 2012, Su et al. 2014). On more local scales, convective clouds impact the atmospheric heating profile through diabatic heating effects, removal of water from the atmospheric column through precipitation, and conditioning of the local environment impacting further development of clouds (e.g., Sullivan and Voigt 2021). These critical roles underscore the importance of realistic representation of convective processes across scales of models from large-eddy simulation (LES), to convection-permitting models (CPM; e.g., Kendon et al. 2020, Marinescu et al. 2021), to numerical weather prediction (NWP) models used for operational weather forecasting, to Earth system models used to predict climate sensitivity (Sanderson et al. 2011, Sherwood et al. 2014, Tomassini et al. 2014, Zhao et al. 2016, Cronin et al. 2017). A key component of improving model representation of convective clouds is better quantification and parameterization of updraft microphysics and dynamics, including their interactions with the surrounding environment and storm organization (Bony et al. 2015, Hagos and Houze 2016, Donner et al. 2016, Morrison et al. 2020). Aerosol is an important environmental factor that could affect convective clouds and precipitation since cloud droplet and ice formation processes are initiated by it. Andrae et al. (2004) hypothesized that aerosols associated with increased biomass burning particles acting as cloud condensation nuclei (CCN) result in smaller and more monodisperse cloud droplets leading to suppression of warm rain formation, ultimately leading to more cloud water being lofted above the freezing level based on observations in the Amazon region. The subsequent increase in latent heat release increases the buoyancy of rising convective parcels invigorating the deep convection. This work was followed by a description of the theoretical basis for this “cold-phase invigoration” by Rosenfeld et al. (2008), who argued that it could have a significant effect for deep convective clouds with warm cloud-bases. Several modeling studies (e.g., Khain et al. 2005, 2009, van den Heever et al. 2006, Fan et al. 2007, 2009, 2012, Lee et al. 2008, Storer et al. 2010, Lebo et al. 2012, Storer and van den Heever 2013, Chen et al. 2020, Dagan et al. 2022) have investigated these aerosol-convection interactions and the environmental factors that influence their relative importance and magnitude. More recently, several studies have indicated that “warm-phase invigoration”, the enhancement of convection through condensational heating, also appears to play a role in enhancing both shallow cumuli (Seiki and Nakajima 2014, Saleeby et al 2015) and deeper tropical convection (Lebo and Seinfeld 2011, Khain et al. 2012, Sheffield et al 2015, Fan et al. 2018, Igel and van den Heever 2021), as well as Houston thunderstorms (Fan et al. 2007, 2020). However, still other studies have provided additional evidence of systematic biases in simulated convective outflow ice size distribution properties, which are consistent with a lack of poorly understood secondary ice production within convective updrafts (e.g., Fridlind et al. 2017). To help address these critical gaps in our understanding of cloud processes, aerosol processes and aerosol-cloud interactions, the Tracking Aerosol Convection Interactions Experiment was designed building upon efforts by the Aerosol, Cloud, Precipitation and Climate (ACPC) Initiative (http://acpcintiative.org/), a joint effort of the International Geosphere-Biosphere Programme (IGBP) and the World Climate Research Program (WCRP) that focused on resolving uncertainties in the interactions between aerosol and clouds towards better understanding the role that these interactions play in the climate system. The TRACER campaign was motivated by recommendations from a number of pilot studies undertaken by ACPC (van den Heever et al. 2017, Fridlind et al. 2019, Hu et al. 2019, Fan et al. 2020, Marinescu et al. 2021, Hernandez-Deckers et al. 2022) that pointed towards the southeastern Texas region as a locale where aerosol-convection interactions could be studied owing to the copious occurrence of isolated convection during the summer months accompanied by diverse and significant sources of aerosols from both anthropogenic and natural sources. The TRACER campaign began on 01 October 2021 and extended through 30 September 2022 with an intensive operational period (IOP) during June-September 2022. Three main sites (Table 1) were managed by the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility.

54 ENVIRONMENTAL SCIENCES↗

Deployment of portable, modular gas samplers as part of an atmospheric tracer experiment

Underground nuclear explosions release noble gases into the atmosphere that can be detected to support international monitoring efforts. Atmospheric transport models help predict the movement of these gases over long distances, but struggle to predict the movement in the atmosphere local to the release. A field experiment was designed to monitor the movement of 127 Xe within a 5-km radius. Four gas samplers were deployed as part of this experiment to collect atmospheric samples at various distances from the release point. In conclusion, these samples were then analyzed in a near-field lab using a NaI detector and in an off-site lab using gamma-gamma coincidence and beta-gamma coincidence counting.

Radioxenon↗

Tracking Aerosol Convection Interactions ExpeRiment (TRACER) Science Plan

Convective clouds play an important role in the Earth’s climate system as a driver of large-scale circulations and a primary mechanism for the transport of heat, moisture, aerosols, and momentum throughout the troposphere. Despite their climatic importance, multi-scale models continue to have persistent biases produced by insufficient representation of convective clouds. This is the result of an incomplete understanding of key processes such as convective initiation, updraft and downdraft dynamics, cloud and precipitation microphysics, and aerosol-convection interactions.

54 ENVIRONMENTAL SCIENCES↗

Tracking Aerosol Convective Interactions Experiment (TRACER) Science Plan

Convective clouds play an important role in the Earth's climate system as a driver of large-scale circulations and a primary mechanism for the transport of heat, moisture, aerosols, and momentum throughout the troposphere. Despite their climatic importance, multi-scale models continue to have persistent biases produced by insufficient representation of convective clouds. This is the result of an incomplete understanding of key processes such as convective initiation, updraft and downdraft dynamics, cloud and precipitation microphysics, and aerosol-convection interactions.The Aerosol-Cloud-Precipitation-Climate Initiative, an international research group dedicated to advancing understanding of aerosol impacts on clouds relevant to climate, has identified the Houston, Texas region as an optimal location for targeted studies of aerosol-convection interactions within frequently developing isolated deep convection. Houston lies within a humid subtropical climate regime, where onshore flow and sea-breeze convection interact with a range of aerosol conditions associated with Houston's urban and industrial emissions. Pilot studies have suggested that convective clouds in this region are potentially significantly impacted by the varying aerosol conditions.

Jensen, M.↗

Shallow cloud variability in Houston, Texas, during the ESCAPE and TRACER field experiments

Shallow convection plays an important role in Earth's climate system by regulating the vertical transport of heat, moisture, and momentum in the lower troposphere. Aerosols, large-scale meteorology, and low-level convergence influence the spatiotemporal variability in shallow convection, and the coastal urban area of Houston, Texas, is an ideal laboratory to investigate these complex interactions. Here, geostationary satellite and ground-based radar observations from June to September 2022 during the TRacking Aerosol Convection interactions ExpeRiment (TRACER) and Experiment of Sea Breeze Convection, Aerosols, Precipitation, and Environment (ESCAPE) field campaigns are used to characterize the spatial coverage, vertical extent, and precipitation fraction of shallow convective clouds. The fused operational remote sensing datasets over a 250 km × 250 km domain are evaluated against profiling observations. The domain-wide diurnal shallow cloud fractions are used to identify four distinct modes of shallow convection. In all clusters, the domain-wide cloud fractions are consistently higher than the domain-wide precipitation fractions, and shallow cloud fractions are higher over water than they are over land, while the shallow precipitation fractions show the opposite behavior. In the two modes with minimal deep cloud activity, shallow cloud frequency is highest over ocean in the early morning, and there is a transition to higher shallow cloud frequency over land by the afternoon in one cluster or to high shallow cloud frequencies everywhere by the afternoon in the other. Lastly, we find regions with higher shallow cloud top heights and a large region along the coastline where shallow clouds are more likely to precipitate.

54 ENVIRONMENTAL SCIENCES↗