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DOE OSTI2014

Efficiencies and Optimization of Weak Base Anion Ion-Exchange Resin for Groundwater Hexavalent Chromium Removal at Hanford

The U.S. Department of Energy’s (DOE’s) contractor, CH2M HILL Plateau Remediation Company, has successfully converted a series of groundwater treatment facilities to use a new treatment resin that is delivering more than $3 million in annual cost savings and efficiency in treating groundwater contamination at the DOE Hanford Site in southeastern Washington State. During the production era, the nuclear reactors at the Hanford Site required a continuous supply of high-quality cooling water during operations. Cooling water consumption ranged from about 151,417 to 378,541 L/min (40,000 to 100,000 gal/min) per reactor, depending on specific operating conditions. Water from the Columbia River was filtered and treated chemically prior to use as cooling water, including the addition of sodium dichromate as a corrosion inhibitor. Hexavalent chromium was the primary component of the sodium dichromate and was introduced into the groundwater at the Hanford Site as a result of planned and unplanned discharges from the reactors starting in 1944. Groundwater contamination by hexavalent chromium and other contaminants related to nuclear reactor operations resulted in the need for groundwater remedial actions within the Hanford Site reactor areas. Beginning in 1995, groundwater treatment methods were evaluated, leading to the use of pump-and-treat facilities with ion exchange using Dowex™ 21K, a regenerable, strong-base anion exchange resin. This required regeneration of the resin, which was performed offsite. In 2008, DOE recognized that regulatory agreements would require significant expansion for the groundwater chromium treatment capacity. As a result, CH2M HILL performed testing at the Hanford Site in 2009 and 2010 to demonstrate resin performance in the specific groundwater chemistry at different waste sites. The testing demonstrated that a weak-base anion, single-use resin, specifically ResinTech SIR-700 ®, was effective at removing chromium, had a significantly higher capacity, could be disposed of efficiently onsite, and would eliminate the complexities and programmatic risks from sampling, packaging, transportation, and return of resin for regeneration.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2016

DEVELOPING ATMOSPHERIC RETRIEVAL METHODS FOR DIRECT IMAGING SPECTROSCOPY OF GAS GIANTS IN REFLECTED LIGHT. I. METHANE ABUNDANCES AND BASIC CLOUD PROPERTIES

Upcoming space-based coronagraphic instruments in the next decade will perform reflected light spectroscopy and photometry of cool directly imaged extrasolar giant planets. We are developing a new atmospheric retrieval methodology to help assess the science return and inform the instrument design for such future missions, and ultimately interpret the resulting observations. Our retrieval technique employs a geometric albedo model coupled with both a Markov chain Monte Carlo Ensemble Sampler ( emcee ) and a multimodal nested sampling algorithm ( MultiNest ) to map the posterior distribution. This combination makes the global evidence calculation more robust for any given model and highlights possible discrepancies in the likelihood maps. As a proof of concept, our current atmospheric model contains one or two cloud layers, methane as a major absorber, and a H{sub 2}–He background gas. This 6-to-9 parameter model is appropriate for Jupiter-like planets and can be easily expanded in the future. In addition to deriving the marginal likelihood distribution and confidence intervals for the model parameters, we perform model selection to determine the significance of methane and cloud detection as a function of expected signal-to-noise ratio in the presence of spectral noise correlations. After internal validation, the method is applied to realistic spectra of Jupiter, Saturn, and HD 99492c, a model observing target. We find that the presence or absence of clouds and methane can be determined with high confidence, while parameter uncertainties are model dependent and correlated. Such general methods will also be applicable to the interpretation of direct imaging spectra of cloudy terrestrial planets.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

An algorithm for detecting and quantifying disturbance and recovery in high-frequency time series

Determining when a disturbance has occurred, its severity, and when the system recovered, is important to numerous questions in the aquatic sciences. This problem can be conceptualized as the timing and degree of perturbation from a typical state, and when the system returns to that typical state. We present an algorithm for detecting disturbance and recovery designed for high-frequency time series, e.g., data produced by automated sampling devices in instrumented buoys and flux towers. The algorithm quantifies differences in the empirical cumulative distribution functions of moving windows over reference and evaluation periods, and is sensitive to changes in the mean, variance, and higher statistical moments. Tests on simulated data show it accurately identifies disturbance and recovery. Three case studies illustrate the application of our algorithm in different empirical settings. A case study on dissolved oxygen in a Florida, USA estuary following a hurricane identified the disturbance and recovery 73 d later. A case study on air temperature and net ecosystem exchange in the Florida everglades identified cold snaps coinciding with periods of reduced carbon uptake. A case study on rotifer abundance following zebra mussel invasion in the Hudson River, NY showed rotifer collapse following invasion and recovery over a decade later. Methods such as ours can improve understanding response to disturbance and facilitate comparative and synthetic study of disturbance impacts across ecosystems.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

Ion-Neutron Irradiated BOR60 Sample Preparation and Characterization: Nuclear Science User Facility 2017 Milestone Report

This document outlines the results obtained by Oak Ridge National Laboratory (ORNL) in collaboration with the University of Michigan-led Consolidated Innovative Nuclear Research project, “Feasibility of combined ion-neutron irradiation for accessing high dose levels.” In this reporting period, neutron irradiated were prepared and shipped to the University of Michigan for subsequent ion irradiation. The specimens were returned to ORNL’s Low Activation Materials Development and Analysis facility, prepared via focused ion beam for examination using scanning/transmission electron microscopy (S/TEM), and then examined using S/TEM to measure the as-irradiated microstructure. This report briefly summarizes the S/TEM results obtained at ORNL’s Low Activation Materials Development and Analysis facility.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2012

Synthesis of homogeneous Ca{sub 0.5}Sr{sub 0.5}FeO{sub 2.5+{delta}} compound using a mirror furnace method

Graphical abstract: X-ray diffraction pattern indexing of Ca{sub 0.5}Sr{sub 0.5}FeO{sub 2.5+{delta}} powder sample obtained by mirror furnace method after thermal treatment. Highlights: Black-Right-Pointing-Pointer A homogenous compound Ca{sub 0.5}Sr{sub 0.5}FeO{sub 2.5+{delta}} has been synthesized for the first time by a mirror furnace method. Black-Right-Pointing-Pointer Ca{sub 0.5}Sr{sub 0.5}FeO{sub 2.5+{delta}} powder sample is perfectly homogenous, confirmed by X-ray diffraction, Raman spectroscopy and EDS technique. Black-Right-Pointing-Pointer The thermal treatment of Ca{sub 0.5}Sr{sub 0.5}FeO{sub 2.5+{delta}} powder sample can increase their average grain sizes. -- Abstract: A new synthesis method using melting zone technique via the double mirror furnace around 1600 Degree-Sign C is used to obtain homogenous brownmillerite compounds Ca{sub 1-x}Sr{sub x}FeO{sub 2.5+{delta}} in the range 0.3 {<=} x {<=} 0.7. These compounds play important role in understanding the mystery of the oxygen diffusion in the perovskite-related oxides. We have successfully solved the miscibility gap problem by synthesizing a good quality of homogenous powder samples of Ca{sub 0.5}Sr{sub 0.5}FeO{sub 2.5+{delta}} compound. Our result was confirmed by X-rays diffraction, Raman spectroscopy and energy dispersive spectroscopy analysis. Thermal treatment was also applied until 800 Degree-Sign C under vacuum to confirm again the homogeneity of powder samples, improve its quality and show that no decomposition or return to form Ca- and Sr-enriched microdomains takes place as a result of phase separation.

36 MATERIALS SCIENCE↗

DOE OSTI2022

On the Viability of Quantum Annealers to Solve Fluid Flows

This paper explores the suitability of upcoming novel computing technologies, particularly adiabatic annealing based quantum computers, to solve fluid dynamics problems that form a critical component of several science and engineering applications. For our experiments, we start with a well-studied one-dimensional simple flow problem, and provide a framework to convert such problems in continuum to a form amenable for deployment on such quantum annealers. Since the DWave annealer returns multiple states sampling the energy landscape of the problem, we explore multiple solution selection strategies to approximate the solution of the problem. We analyze the continuum solutions obtained both qualitatively and quantitatively as well as their sensitivities to the particular solution selection scheme.

42 ENGINEERING↗

DOE OSTI2026

Opportunities and Limitations of Nuclear Magnetic Resonance Spectroscopy in Astrobiology

For decades, Nuclear Magnetic Resonance (NMR) spectroscopy has been utilized as a powerful tool in various scientific disciplines, most prominently in chemistry, to determine molecular structures or monitor reactions. While well established in various fields, NMR applications in astrobiology are still unclear. This work aims to explore the potential of NMR in astrobiology, highlighting strengths but also weaknesses. We illustrate capabilities of NMR with two applications: (1) recently developed methods for position-specific carbon isotope analysis of complex organics; and (2) well-established tools for performing quantitative compositional analysis of complex organic mixtures. By utilizing samples relevant to astrobiology, specifically the amino acid valine and analogue mixtures of organics, we showcase that molecules retain a source dependent and distinct intramolecular carbon isotope fingerprint. We demonstrate that compositional sample analysis provides an independent and complementary line of evidence pointing towards the origin of a molecule or mixture. Together, these NMR tools have the potential to support life detection efforts, and aid in distinguishing between biotic and abiotic samples. Finally, we discuss sensitivity, detection limits, the portability of NMR, and propose how integration with mass-spectrometry techniques will be imperative to enable more targeted and comprehensive analyses relevant to astrobiology, including in-situ analysis but also sample return missions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2018

Elemental Composition of Analogs to Mars Return Samples Studied with X-Ray Fluorescence Imaging at NSLS-II

In 2020, NASA will launch out into the first step of what may be an ambitious, multi-mission campaign with the goal to bring back for analysis in laboratories here to Earth a collection of rock, regolith, and atmosphere samples from Mars. It is the main objective of this endeavor to determine whether or not Mars was ever host to ancient microbial life. Finding evidence for extinct (or extant) life on Mars has the potential to fundamentally alter our view of the origin and evolution of life. It would provide proof for Earth being just one amongst others regarding the question of biological activity in the Solar System. Furthermore, returned Martian samples would provide a rich repository of information on the history of planetary accretion and differentiation, geochronology, atmospheric evolution, and the paleo-environmental history of Mars, adding tremendous additional value to such a mission beyond the issue of extraterrestrial life. Here the potential knowledge to be obtained by such a collection of samples will equal or exceed that of the Apollo lunar sample archive, which even today yields new insights on the history of the Solar System, over 40 years after they were returned to Earth.

36 MATERIALS SCIENCE↗

DOE OSTI2013

Participant Assisted Data Collection Methods in the California Healthy Homes Indoor Air Quality Study of 2011-13

From November 2011 to March 2013, air quality was measured over 6-day periods in 324 residences across California using a mail-out strategy. All interactions with study participants, from recruitment, to data collection, to communication of results, were conducted with remote communication methods including conventional mail, electronic mail, telephone and text messaging. Potential participants were reached primarily by sharing study information with community groups and organizations that directed interested individuals to complete an online screening survey. Pollutant concentrations were measured with sampling equipment that was mailed to participants' homes with deployment instructions. Residence and household characteristics and activity data were collected via two phone surveys and an activity log. A comparison of responses to survey questions completed online versus over the phone indicated that a substantial fraction of participants (roughly 20%) required a researcher's assistance to respond to basic questions about appliance characteristics. Using the printed instructions and telephone assistance from researchers, roughly 90% of participants successfully deployed and returned sampling materials accurately and on schedule. The mail-out strategy employed in this study was found to be a cost-effective means for collecting residential air quality data.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Revealing the Moon's Taurus‐Littrow Landslide via Integrated Analysis of Pristine Apollo 17 Soil Core 73001/2

The “light mantle” deposit at the base of South Massif in the Moon's Taurus‐Littrow Valley was a primary science target for the Apollo 17 exploration. The possibility that it was a landslide triggered by ejecta from Tycho Crater is critical for establishing the age of Tycho and constraining recent lunar impact chronology; however, the mechanism of emplacement of the deposit has recently been questioned. The newly opened 73001/73002 double drive tube from Station 3 sampled 70.6 cm deep into the regolith and represents the first stratigraphic section of an extraterrestrial landslide deposit returned to Earth. Here we provide an overview of the stratigraphy of the 73001/73002 core based on top to bottom variations revealed by coordinated laboratory analyses and explore constraints on the emplacement of the light mantle deposit. Briefly, the upper ∼10 cm of 73002 contains a disturbed zone from space weathering and emplacement of ejecta from a nearby crater that excavated and ejected basaltic material. Below 10 cm is a nearly uniform unit of immature regolith. These data support a single event for the emplacement of the deposit at this location, followed by weathering and mixing of materials from nearby crater ejecta in the upper 10 cm. Slight variations in chemistry and clast components may reflect the relative stratigraphy of the South Massif slope, with material toward the bottom of 73001 originating from lower slopes and material from higher up in the core representing regolith from higher up the South Massif slopes.

58 GEOSCIENCES↗

DOE OSTI2018

Impact of UV Pulsed Laser Radiation and of the Electron Flow on Dielectric States of Polymer Composite Nanomaterial Based on LDPE Matrix

The influence of the soft electron flow and irradiating pulsed UV laser on dielectric states of polymer composite nanomaterial based on LDPE matrix is experimentally studied. It was shown that irradiation of the samples LDPE–ZnO by electron beam (10 keV) for 10–15 minutes gives rise the appearance of the horizontal portion of the temperature dependence of capacitance (permittivity) and to memory effect (slow relaxation of dielectric situation within a few days). Irradiation with pulsed UV laser of the LDPE–CdS sample allows you to switch into a conducting state and return it to their original state upon application of a weak electric field. The observed phenomena may find practical applications for the polymer electronic memories and switching devices.

36 MATERIALS SCIENCE↗

DOE OSTI2019

Cloud System Evolution in the Trades (CSET): Following the Evolution of Boundary Layer Cloud Systems with the NSF–NCAR GV

The Cloud System Evolution in the Trades (CSET) study was designed to describe and explain the evolution of the boundary layer aerosol, cloud, and thermodynamic structures along trajectories within the North Pacific trade winds. The study centered on seven round trips of the National Science Foundation–National Center for Atmospheric Research (NSF–NCAR) Gulfstream V (GV) between Sacramento, California, and Kona, Hawaii, between 7 July and 9 August 2015. The CSET observing strategy was to sample aerosol, cloud, and boundary layer properties upwind from the transition zone over the North Pacific and to resample these areas two days later. Global Forecast System forecast trajectories were used to plan the outbound flight to Hawaii with updated forecast trajectories setting the return flight plan two days later. Two key elements of the CSET observing system were the newly developed High-Performance Instrumented Airborne Platform for Environmental Research (HIAPER) Cloud Radar (HCR) and the high-spectral-resolution lidar (HSRL). Together they provided unprecedented characterizations of aerosol, cloud, and precipitation structures that were combined with in situ measurements of aerosol, cloud, precipitation, and turbulence properties. The cloud systems sampled included solid stratocumulus infused with smoke from Canadian wildfires, mesoscale cloud–precipitation complexes, and patches of shallow cumuli in very clean environments. Ultraclean layers observed frequently near the top of the boundary layer were often associated with shallow, optically thin, layered veil clouds. In conclusion, the extensive aerosol, cloud, drizzle, and boundary layer sampling made over open areas of the northeast Pacific along 2-day trajectories during CSET will be an invaluable resource for modeling studies of boundary layer cloud system evolution and its governing physical processes.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

MARLOWE: An Untargeted Proteomics, Statistical Approach to Taxonomic Classification for Forensics

General proteomics research for fundamental science typically addresses laboratory- or patient-derived samples of known origin and composition. However, in a few research areas, such as environmental proteomics, clinical identification of infectious organisms, archeology, art/cultural history, and forensics, attributing the origin of a protein-containing sample to the organisms that produced it is a central focus. A small number of groups have approached this problem and developed software tools for taxonomic characterization and/or identification using bottom-up proteomics. Most such tools identify peptides via database search, and many rely on organism-specific peptides as markers. Our group recently introduced MARLOWE, a software tool for taxonomic characterization of unknown samples based on de novo peptide identification and signal-erosion-resistant strong peptides, which are shared peptides distributed in a taxonomy-dependent manner. In the current work, we further characterize the utility of MARLOWE using publicly available proteomics data from forensically-relevant samples. MARLOWE characterizes samples based on their protein profile, and returns ranked organism lists of potential contributors and taxonomic scores based on shared strong peptides between organisms. Overall, the correct characterization rate ranges between 44 and 100%, depending on the sample type and data acquisition parameters (with lower numbers associated with lower-quality data sets). MARLOWE demonstrates successful characterization of true contributors and close relatives, and provides sufficient specificity to distinguish certain microbial species. MARLOWE demonstrates its ability to provide insight into potential taxonomic sources for a wide range of sample types without prior assumptions about sample contents. As a result, this approach can find utility in forensic science and also broadly in bioanalytical applications that utilize proteomics approaches for taxonomic characterization.

Bacteria↗

DOE OSTI2020

OrganiCam: First Camera for Noncontact Biodetection in Space

Los Alamos National Laboratory designed a compact laser-induced fluorescence imaging camera with Raman spectrometer to identify organic molecules and biosignatures in environments such as Martian caves, icy-moons, and asteroid surfaces. OrganiCam is the primary instrument on the Laser-Induced Fluorescence Exploration of Caves for Organics and Volatiles using an Elevated Platform (LIFE COVE) NASA mission concept. OrganiCam could also determine if instruments being sent into space for NASA are sterile and analyze samples returned to Earth. OrganiCam’s robust design for extreme environments, portability, simple operation, and low power requirement build on LANL’s 50+ years designing robotic instruments for space applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2012

MPACT LSDS Progress Report: LANL and LANL-Funded Activities in Support of Spent Fuel Measurements Using a Lead Slowing Down Spectrometer in FY 2012

During FY 2012, Lead Slowing Down Spectrometer (LSDS) measurement campaigns took place at the Los Alamos Neutron Science Center, and the Rensselaer Polytechnic Institute. At Los Alamos, we measured the response of a thorium fission chamber to a 25 gram plutonium sample, and evaluated the performance of a 4 He-filled proportional counter. At RPI, the effort lead by Professor Danon, performed an assay of fuel pins, and used a fission chamber with plutonium to evaluate the impact of room return.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Triple oxygen and hydrogen stable isotope composition of water in Murchison carbonaceous chondrite accessed by thermogravimetry-enabled laser spectroscopy

For this work, we have developed the capability to measure 17 O/ 16 O in H 2 O and OH - of hydrous minerals by a technique using thermogravimetric analysis coupled with isotope ratio infrared spectroscopy (TGA-IRIS) on a suite of liquid water standards, terrestrial mineral standards, multi-mineral synthetic mixtures of terrestrial samples, and Murchison carbonaceous chondrite. This 17 O/ 16 O analytical capability is combined with the previously developed TGA-IRIS capability of 18 O/ 16 O, which enables us to calculate Δ `17 O values. Additionally, we have made 2 H/ 1 H measurements by TGA-IRIS on the suite of materials. Analyses of 328 standard water samples sealed into silver tubes (0.25 μL, 174 VSMOW and 154 GISP) analyzed over the course of three years yielded δ 18 O values by TGA-IRIS with precision of ±0.30 ‰, δ 17 O of ±0.24 ‰, Δ `17 O of ±0.126 ‰, and δ 2 H ± 7.5 ‰ (± 1 Std. Dev.). TGA-IRIS analyses of a suite of hydrous minerals (oxy-hydroxide, mica, serpentines, sulfide, phyllosillicates) yields similar precision. TGA-IRIS analyses of the CM2 carbonaceous chondrite Murchison resulted in δ 18 O, δ 17 O, Δ `17 O, and δ 2 H values of the H 2 O and/or OH - from its hydrous minerals. Δ `17 O values of Murchison H 2 O range from 1.034 ‰ at 350 °C, to -0.368 ‰ at 650 °C, to -1.75 ‰ at 850 °C. TGA-IRIS can generate Δ `17 O values of H 2 O and/or OH - in hydrous materials that are well within the precision needed for the analysis of meteoritic samples, as well as samples returned from asteroids, such as Ryugu and Bennu.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2015

Rethinking the Default Construction of Multimodel Climate Ensembles

Here, we discuss the current code of practice in the climate sciences to routinely create climate model ensembles as ensembles of opportunity from the newest phase of the Coupled Model Intercomparison Project (CMIP). We give a two-step argument to rethink this process. First, the differences between generations of ensembles corresponding to different CMIP phases in key climate quantities are not large enough to warrant an automatic separation into generational ensembles for CMIP3 and CMIP5. Second, we suggest that climate model ensembles cannot continue to be mere ensembles of opportunity but should always be based on a transparent scientific decision process. If ensembles can be constrained by observation, then they should be constructed as target ensembles that are specifically tailored to a physical question. If model ensembles cannot be constrained by observation, then they should be constructed as cross-generational ensembles, including all available model data to enhance structural model diversity and to better sample the underlying uncertainties. To facilitate this, CMIP should guide the necessarily ongoing process of updating experimental protocols for the evaluation and documentation of coupled models. Finally, with an emphasis on easy access to model data and facilitating the filtering of climate model data across all CMIP generations and experiments, our community could return to the underlying idea of using model data ensembles to improve uncertainty quantification, evaluation, and cross-institutional exchange.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Effect of a Fine-Scale Layered Structure of the Atmosphere on Infrasound Signals from Fragmenting Meteoroids

We investigate the influence of a fine-scale (FS) layered structure in the atmosphere on the propagation of infrasound signals generated by fragmenting meteoroids. Using a pseudo-differential parabolic equation (PPE) approach, we model broadband acoustic signals from point sources at altitudes of 35–100 km. The presence of FS fluctuations in the stratosphere (37–45 km) and the lower thermosphere (100–120 km) modifies ray trajectories, causing multiple arrivals and prolonged signal durations at ground stations. In particular, meteoroids fragmenting at 80–100 km can produce two distinct thermospheric arrivals beyond 150 km range, while meteoroids descending to 50 km or below yield weak, long-lived arrivals within the acoustic shadow zone via antiguiding propagation and diffraction. Comparison with observed infrasound data confirms that FS-layered inhomogeneities can account for multi-arrival “N-waves,” broadening potential interpretations of meteoroid signals. The results also apply to other atmospheric-entry objects, such as sample return capsules, emphasizing how FS structure impacts shock wave propagation. In conclusion, our findings advance understanding of wavefield evolution in a layered atmosphere and have broad relevance for global infrasound monitoring of diverse phenomena (e.g., re-entry capsules, rocket launches, and large-scale explosions).

Aeroacoustics↗