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All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Bio-distribution and deposition of wildfire smoke chemicals into olfactory bulb and brain of rats after intranasal instillation

Epidemiological and experimental studies suggest wildfire smoke is a potential contributor to neurological dysfunction and associated with neuroinflammation. Using doses comparable to those encountered during intense wildfire events (200-300 μg/m 3 ), we explore the absorption, distribution, metabolism, and elimination (ADME) and pharmacokinetics of representative members of major chemical classes (acid, phenol, PAH, aldehyde) in inhaled wood smoke condensates. Male Sprague Dawley rats were intranasally instilled with smoldering eucalyptus woodsmoke extract (WSE) reconstituted in saline spiked with 14 C-labeled palmitic acid (PA), benzo[a]pyrene (B[a]P), catechol (CAT) or benzaldehyde (BZ). Serum was collected from 5 min to 2 weeks after exposure and tissues were collected at 0.5, 2, 4, 24 h and 2 weeks after exposure. Urine was collected over the 24 h exposure. Tissues were collected, rinsed in PBS and analyzed by accelerator mass spectrometry (AMS) for 14C-labeled chemicals. PA and B[a]P entered circulation slowly, reached maximum concentration (C max ) near 15 ng/mL at 2 h, and had circulating concentrations near 1/3 C max 24 h after exposure. CAT and BZ rapidly entered circulation and were mostly cleared at 2 h. Excess 14 C from all four chemicals was detected in olfactory bulb and brain over the first 24 h but only PA (or its metabolites) was retained in olfactory bulb, brain and kidney at 2 weeks post exposure. All excess 14 C was cleared from the lung at 2 weeks. Metabolite analysis of urine (CAT, BZ and B(a)P) dosed samples did not detect any parent compound. CAT and BZ were rapidly cleared. The slower uptake and clearance of PA or B[a]P or their reactive metabolites when dosed with WSE in brain and olfactory bulb potentially provide greater opportunity for inflammatory response. This study suggests that wildfire smoke chemicals can enter the brain directly from the nasal cavity to the olfactory bulb and via systemic circulation.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗
DOE OSTI2015

Iron mineral structure, reactivity, and isotopic composition in a South Pacific Gyre ferromanganese nodule over 4 Ma

Deep-sea ferromanganese nodules accumulate trace elements from seawater and underlying sediment porewaters during the growth of concentric mineral layers over millions of years. These trace elements have the potential to record past ocean geochemical conditions. The goal of this study was to determine whether Fe mineral alteration occurs and how the speciation of trace elements responds to alteration over ~3.7Ma of marine ferromanganese nodule (MFN) formation, a timeline constrained by estimates from 9 Be/ 10 Be concentrations in the nodule material. We determined Fe-bearing phases and Fe isotope composition in a South Pacific Gyre (SPG) nodule. Specifically, the distribution patterns and speciation of trace element uptake by these Fe phases were investigated. The time interval covered by the growth of our sample of the nodule was derived from 9 Be/ 10 Be accelerator mass spectrometry (AMS). The composition and distribution of major and trace elements were mapped at various spatial scales, using micro-X-ray fluorescence (μXRF), electron microprobe analysis (EMPA), and inductively coupled plasma mass spectrometry (ICP-MS). Fe phases were characterized by micro-extended X-ray absorption fine structure (μEXAFS) spectroscopy and micro-X-ray diffraction (μXRD). Speciation of Ti and V, associated with Fe, was measured using micro-X-ray absorption near edge structure (μXANES) spectroscopy. Iron isotope composition (δ 56/54 Fe) in subsamples of 1-3mm increments along the radius of the nodule was determined with multiple-collector ICP-MS (MC-ICP-MS). The SPG nodule formed through primarily hydrogeneous inputs at a rate of 4.0±0.4mm/Ma. The nodule exhibited a high diversity of Fe mineral phases: feroxyhite (δ-FeOOH), goethite (α-FeOOH), lepidocrocite (γ-FeOOH), and poorly ordered ferrihydrite-like phases. These findings provide evidence that Fe oxyhydroxides within the nodule undergo alteration to more stable phases over millions of years. Trace Ti and V were spatially correlated with Fe and found to be adsorbed to Fe-bearing minerals. Ti/Fe and V/Fe ratios, and Ti and V speciation, did not vary along the nodule radius. The δ 56/54 Fe values, when averaged over sample increments representing 0.25-0.75Ma, were homogeneous within uncertainty along the nodule radius, at -0.12±0.07‰ (2sd, n=10). Our results indicate that the Fe isotope composition of the nodule remained constant during nodule growth and that mineral alteration did not affect the primary Fe isotope composition of the nodule. Furthermore, the average δ 56/54 Fe value of -0.12‰ we find is consistent with Fe sourced from continental eolian particles (dust). Despite mineral alteration, the trace element partitioning of Ti and V, and Fe isotope composition, do not appear to change within the sensitivity of our measurements. These findings suggest that Fe oxyhydroxides within hydrogenetic ferromanganese nodules are out of geochemical contact with seawater once they are covered by subsequent concentric mineral layers. Even though Fe-bearing minerals are altered, trace element ratios, speciation and Fe isotope composition are preserved within the nodule.

58 GEOSCIENCES↗
DOE OSTI2021

Phagosomal chloride dynamics in the alveolar macrophage

Acidification in intracellular organelles is tightly linked to the influx of Cl – counteracting proton translocation by the electrogenic V-ATPase. We quantified the dynamics of Cl – transfer accompanying cargo incorporation into single phagosomes in alveolar macrophages (AMs). Phagosomal Cl – concentration and acidification magnitude were followed in real time with maximal acidification achieved at levels of approximately 200 mM. Live cell confocal microscopy verified that phagosomal Cl – influx utilized predominantly the Cl – channel CFTR. Relative levels of elemental chlorine (Cl) in hard X-ray fluorescence microprobe (XFM) analysis within single phagosomes validated the increase in Cl – content. XFM revealed the complex interplay between elemental K content inside the phagosome and changes in Cl – during phagosomal particle uptake. Cl – -dependent changes in phagosomal membrane potential were obtained using second harmonic generation (SHG) microscopy. These studies provide a mechanistic insight for screening studies in drug development targeting pulmonary inflammatory disease.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2019

Investigations of vertical wind variations at a mountain top in the Himalaya using Doppler Lidar observations and model simulations

Hight-resolved observations of vertical winds remain nearly non-existing over the Himalayas, despite of an­ticipated crucial role of vertical motions in transporting pollution across the Himalayan hms. The present study analyze the vertical wind observations from surface to 1 km above ground level over Manora Peak (29.4° N; 79.5° E; 1958 m ams!) in the Himalaya performed using a Doppler Lidar during the Ganges Valley Aerosol Experiment (GVAX). Vertical wind exhibited a pronounced diurnal variability at Manora Peak comprising of upward motions during the daytime (05-10 UT) and downward motions during nighttime typical of a mountain­valley system. Mean vertical wind speeds are observed to be varying from -0.8 to +0.8 ms- 1 during the study period with a variance of 0.1-1.5 m2s·2, which is attributed to the thermally driven turbulence. Mean vertical winds are observed to be stronger in the Doppler Lidar profiles above Manora Peak (-0_8 to 0.8 ms- 1) as compared to near surface measurements at this station using an ultrasonic anemometer ( -0.4 to 0.4 ms - 1 ), and low altitude stations in India. Daytime vertical wind speeds are observed to be higher during pre-monsoon (0.81 ms- 1), as compared to post-monsoon (0.24 ms- 1) and winter (0.33 ms- 1)_ Average Black Carbon (BC) concentrations are significantly higher during strong upward vertical winds, which indicates efficient transport of polluted air mass from low-altitude regions to the Himalaya. Weather Research and Forecasting (WRF) model reproduces the observed diurnal pattern in the vertical wind at the observation site however the model un­derestimates the variability.

Shukla, K K.↗
DOE OSTI2017

Recent advances in the detection of specific natural organic compounds as carriers for radionuclides in soil and water environments, with examples of radioiodine and plutonium

Among the key environmental factors influencing the fate and transport of radionuclides in the environment is natural organic matter (NOM). While this has been known for decades, there still remains great uncertainty in predicting NOM-radionuclide interactions because of lack of understanding of radionuclide interactions with the specific organic moieties within NOM. Furthermore, radionuclide-NOM studies conducted using modelled organic compounds or elevated radionuclide concentrations provide compromised information related to true environmental conditions. Thus, sensitive techniques are required not only for the detection of radionuclides, and their different species, at ambient and/or far-field concentrations, but also for potential trace organic compounds that are chemically binding these radionuclides. GC-MS and AMS techniques developed in our lab are reviewed in this paper that aim to assess how two radionuclides, iodine and plutonium, form strong bonds with NOM by entirely different mechanisms; iodine tends to bind to aromatic functionalities, whereas plutonium binds to N-containing hydroxamate siderophores at ambient concentrations. While low-level measurements are a prerequisite for assessing iodine and plutonium migration at nuclear waste sites and as environmental tracers, it is necessary to determine their in-situ speciation, which ultimately controls their mobility and transport in natural environments. Finally and more importantly, advanced molecular-level instrumentation (e.g., nuclear magnetic resonance (NMR) and Fourier-transform ion cyclotron resonance coupled with electrospray ionization (ESI-FTICRMS) were applied to resolve either directly or indirectly the molecular environments in which the radionuclides are associated with the NOM.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Wanted! Nuclear Data for Dark Matter Astrophysics

Astronomical observations from small galaxies to the largest scales in the universe can be consistently explained by the simple idea of dark matter. The nature of dark matter is however still unknown. Empirically it cannot be any of the known particles, and many theories postulate it as a new elementary particle. Searches for dark matter particles are under way: production at high-energy accelerators, direct detection through dark matter-nucleus scattering, indirect detection through cosmic rays, gamma rays, or effects on stars. Particle dark matter searches rely on observing an excess of events above background, and a lot of controversies have arisen over the origin of observed excesses. With the new high-quality cosmic ray measurements from the AMS-02 experiment, the major uncertainty in modeling cosmic ray fluxes is in the nuclear physics cross sections for spallation and fragmentation of cosmic rays off interstellar hydrogen and helium. The understanding of direct detection backgrounds is limited by poor knowledge of cosmic ray activation in detector materials, with order of magnitude differences between simulation codes. A scarcity of data on nucleon spin densities blurs the connection between dark matter theory and experiments. What is needed, ideally, are more and better measurements of spallation cross sections relevant to cosmic rays and cosmogenic activation, and data on the nucleon spin densities in nuclei.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2018

Fast-neutron multiplicity counter for active measurements of uranium oxide certified material

We developed a fast-neutron multiplicity counter (FNMC) based on stilbene and EJ-309 organic 11 scintillators. The system can detect and discriminate correlated photon and neutron multiplets emitted by fission 12 reactions. We used the system to estimate the fissile mass of uranium oxide samples in active interrogation mode at the 13 Zero Power Physics Reactor of Idaho National Laboratory (INL). Two sets of certified reference material (CRM) 14 samples were characterized. The U-235 enrichment of the first set is constant at 93.2 wt%, and the UO 2 mass ranges 15 between 0.5 and 4 kg. The second set includes samples of increasing enrichment (from 20 wt% to 97 wt%) and constant 16 UO 2 mass of 230 g. We used two AmLi sources to induce fission reactions in the samples. Despite the intense gamma17 ray background of the UO 2 and interrogating sources, the system could measure induced fission neutrons emerging from 18 the interrogated samples without additional shielding surrounding the sample and only relying on pulse shape 19 discrimination to classify neutron and gamma-ray pulses. Here, the overall neutron count rate and time-correlated counts are 20 well correlated with the sample fissile mass. We also proved that CRM samples can be used to build a calibration curve 21 to assay the U-235 mass of unknown samples of different mass, geometry and enrichment, with an average bias error of 22 8%, for U-235 mass higher than 390 g.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

Genetic algorithm optimization of tin–copper graded shielding for improved plutonium safeguards measurements

Plutonium nuclear material safeguards is essential to ensure that states do not divert plutonium to clandestine nuclear weapons programs. Traditional safeguards methods rely on correlated neutron measurements. Detection systems based on organic scintillators, which are sensitive to fast neutrons and photons, are gaining support for use in safeguards applications due to increased capabilities and shorter measurement times compared to the current state-of-the-art. A drawback of organic scintillators in plutonium measurements is data throughput limitations; 241 Am builds up in plutonium samples and emits 60-keV gamma rays with a high specific activity. In this work, a genetic algorithm is used to design graded shielding made of tin and copper to attenuate the 60-keV gamma rays. The shield is designed to limit the attenuation of the higher-energy, fission photons, because fission photons can be used as a signature. The genetic algorithm optimization takes days to run, while a complete search space exploration would take years. The genetic algorithm was run for different levels of 60-keV gamma-ray attenuation, and the thickness of the required shielding layers was determined at each level. Tin–copper shielding was placed in front of an array of organic scintillation detectors for a measurement of approximately 4.5 kg of alpha-phase, weapons-grade plutonium, an AmLi source, and a 252 Cf source. We show that the shield successfully attenuated low-energy, non-fission gamma rays, which significantly improved the organic scintillator performance.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2018

Naphthalene DNA adduct formation and tolerance in the lung

Naphthalene (NA) is a respiratory toxicant and possible human carcinogen. NA is a ubiquitous combustion product and significant component of jet fuel. The National Toxicology Program found that NA forms tumors in two species, in rats (nose) and mice (lung). However, it has been argued that NA does not pose a cancer risk to humans because NA is bioactivated by cytochrome P450 monooxygenase enzymes that have very high efficiency in the lung tissue of rodents but low efficiency in the lung tissue of humans. It is thought that NA carcinogenesis in rodents is related to repeated cycles of lung epithelial injury and repair, an indirect mechanism. Repeated in vivo exposure to NA leads to development of tolerance, with the emergence of cells more resistant to NA insult. We tested the hypothesis that tolerance involves reduced susceptibility to the formation of NA-DNA adducts. NA-DNA adduct formation in tolerant mice was examined in individual, metabolically-active mouse airways exposed ex vivo to 250 μM 14 C-NA. Ex vivo dosing was used since it had been done previously and the act of creating a radioactive aerosol of a potential carcinogen posed too many safety and regulatory obstacles. Following extensive rinsing to remove unbound 14 C-NA, DNA was extracted and 14 C-NA-DNA adducts were quantified by accelerator mass spectrometry (AMS). The tolerant mice appeared to have slightly lower NA-DNA adduct levels than non-tolerant controls, but intra-group variations were large and the difference was statistically insignificant. It appears the tolerance may be more related to other mechanisms, such as NA-protein interactions in the airway, than DNA-adduct formation.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2019

Towards successful cleaning of chert samples for improved 10Be and 26Al measurements

In situ-produced cosmogenic 10 Be and 26 Al measurements are widely applied in geomorphological studies and in archaeology and paleoanthropology as a chronologic tool applicable to the past 5 Ma. While most of these measurements are made from concentrates of quartz, a ubiquitous and resistant mineral, it is of great interest to extend this method to other silicates and particularly to the amorphous silicates whose purification may not be as straightforward. This paper presents a cleaning procedure that has been applied on ten samples of various siliceous rocks (chert, granite and quartzolite). The aim is to monitor the 10 Be, 27 Al and 26 Al concentration evolution as a function of cleaning steps. While this protocol appears suitable for 10 Be, when measuring 26 Al careful attention should be paid to 27 Al, whose concentration should be measured regularly to ensure that a constant value is achieved and most important, allowing measuring 26 Al/ 27 Al by AMS.

36 MATERIALS SCIENCE↗
DOE OSTI2016

A novel method for production of spherical Ti-6Al-4V powder for additive manufacturing

We report a novel method was developed to produce spherical Ti-6Al-4V powder for advanced near-net-shape manufacturing processes including additive manufacturing and powder injection molding. The new process synergistically integrates a few common low-cost processing techniques including granulation, sintering, and de-oxygenation to produce spherical Ti alloy powders without relying on costly melting and atomizing techniques. This new granulation-sintering-deoxygenation (GSD) process can use low-cost source powders such as scrap Ti as the raw material. The spherical Ti-6Al-4V powder produced using this process has controlled particle size distribution and low oxygen content (< 0.15%), which meet the Aerospace Material Specification (AMS-4998) for spherical Ti-6Al-4V powder.

42 ENGINEERING↗
DOE OSTI2022

Clean quartz matters for cosmogenic nuclide analyses: An exploration of the importance of sample purity using the CRONUS-N reference material

We report reference materials are key for assessing inter-laboratory variability and measurement quality, and for placing analytical uncertainty bounds on sample analyses. Here, we investigate four years of data resulting from repeated processing of the CRONUS-N reference material for cosmogenic 10 Be and 26 Al analyses. At University of Vermont, we prepared a CRONUS-N aliquot with most of our sample batches from 2013 to 2017; these reference material samples were then distributed to four different accelerator mass spectrometry facilities, yielding 73 10 Be analyses and 58 26 Al analyses. We determine CRONUS-N 10 Be concentrations of (2.26 ± 0.14) x 10 5 atoms g -1 (n = 73, mean, 1 SD) and 26 Al concentrations of (1.00 ± 0.08) x 10 6 atoms g -1 (n = 58, mean, 1 SD). We find a reproducibility of 6.3% for 10 Be and 7.7% for 26 Al (relative standard deviations). We also document highly variable 27 Al and Mg concentrations and a 10 Be dispersion twice as large as the mean AMS analytic uncertainty. Analyses of the CRONUS-N material with and without density separation demonstrate that non-quartz minerals are present in the material and have a large impact on measured concentrations of 27 Al, 10 Be, and impurities; these non-quartz minerals represent only a very small portion of the total mass (0.6–0.8%) but have a disproportionally large effect on the resulting data. Our results highlight the importance of completely removing all non-quartz mineral phases from samples prior to Be/Al extraction for the determination of in situ cosmogenic 10 Be and 26 Al concentrations.

58 GEOSCIENCES↗
DOE OSTI2023

Benzo[$\mathcal{a}$]pyrene toxicokinetics in humans following dietary supplementation with 3,3'-diindolylmethane (DIM) or Brussels sprouts

Utilizing the atto-zeptomole sensitivity of UPLC-accelerator mass spectrometry (UPLC-AMS), we previously demonstrated significant first-pass metabolism following escalating (25–250 ng) oral micro-dosing in humans of [ 14 C]-benzo[a]pyrene ([ 14 C]-BaP). The present study examines the potential for supplementation with Brussels sprouts (BS) or 3,3' -diindolylmethane (DIM) to alter plasma levels of [ 14 C]-BaP and metabolites over a 48-h period following micro-dosing with 50 ng (5.4 nCi) [ 14 C]-BaP. Volunteers were dosed with [ 14 C]-BaP following fourteen days on a cruciferous vegetable restricted diet, or the same diet supplemented for seven days with 50 g of BS or 300 mg of BR-DIM ® prior to dosing. BS or DIM reduced total [ 14 C] recovered from plasma by 56–67% relative to nonintervention. Dietary supplementation with DIM markedly increased T max and reduced C max for [ 14 C]-BaP indicative of slower absorption. Further, both dietary treatments significantly reduced C max values of four downstream BaP metabolites, consistent with delaying BaP absorption. Dietary treatments also appeared to reduce the T 1/2 and the plasma AUC( 0,$\infty$ ) for Unknown Metabolite C, indicating some effect in accelerating clearance of this metabolite. Toxicokinetic constants for other metabolites followed the pattern for [ 14 C]-BaP (metabolite profiles remained relatively consistent) and non-compartmental analysis did not indicate other significant alterations. Significant amounts of metabolites in plasma were at the bay region of [ 14 C]-BaP irrespective of treatment. Although the number of subjects and large interindividual variation are limitations of this study, it represents the first human trial showing dietary intervention altering toxicokinetics of a defined dose of a known human carcinogen.

3,3'-diindolylmethane↗
DOE OSTI2019

Naphthalene genotoxicity: DNA adducts in primate and mouse airway explants

Naphthalene (NA) is a ubiquitous environmental pollutant and possible human carcinogen that forms tumors in rodents with tissue/regional and species selectivity. This study seeks here to determine whether NA is able to directly adduct DNA in an ex vivo culture system. Metabolically active lung tissue was isolated and incubated in explant culture with carbon-14 labeled NA (0, 25, 250 μM) or 1,2-naphthoquinone (NQ), followed by AMS analyses of metabolite binding to DNA. Despite relatively low metabolic bioactivation in the primate airway, dose-dependent NA-DNA adduct formation was detected. More airway adducts were detected in female mice (4.7-fold) and primates (2.1-fold) than in males of the same species. Few adducts were detected in rat airway or nasal epithelium. NQ, which is a metabolic product of NA, proved to be even more potent, with levels of adduct formation 70–80-fold higher than seen when tissues were incubated with the parent compound NA. This is the first study to demonstrate NA-DNA adduct formation at a site of carcinogenesis, the mouse lung. Adducts were also detected in non-human primate lung and with a NQ metabolite of NA. Taken together, this suggests that NA may contribute to in vivo carcinogenesis through a genotoxic mechanism.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2017

Folsom Mammoth Hunters? The Terminal Pleistocene Assemblage From Owl Cave (10BV30), Wasden Site, Idaho

The 1960s and 1970s excavations at Owl Cave (10BV30) recovered mammoth bone and Folsom-like points from the same strata, suggesting evidence for a post-Clovis mammoth kill. However, a synthesis of the excavation data was never published, and the locality has since been purged from the roster of sites with human/extinct megafauna associations. In this paper, we present dates on bone from the oldest stratum, review provenience data, conduct a bone-surface modification study, and present the results of a protein-residue analysis. Our study fails to make the case for mammoth hunting by Folsom peoples. Although two of the point fragments tested positive for horse or elephant protein, recent AMS dates indicate that all of the mammoth remains predate Folsom, and horse remains are absent from the Owl Cave collection. Further, no unambiguously cultural surface modifications were identified on any of the mammoth remains. Given the available data, the Owl Cave deposits are most parsimoniously read as containing a Folsom-age occupation in a buried context, the first of its kind in the desert West, but one nonetheless part of a palimpsest of terminal Pleistocene materials.

99 GENERAL AND MISCELLANEOUS↗
DOE OSTI2021

Tunable Atomic Layer Deposition into Ultra-High-Aspect-Ratio (>60000:1) Aerogel Monoliths Enabled by Transport Modeling

Atomic layer deposition (ALD) modification of ultra-high-aspect-ratio structures (>10,000:1) is a powerful platform with applications in catalysis, filtration, and energy conversion. However, the deposition of conformal and tunable ALD coatings at these aspect ratios remains challenging, resulting in empirical tradeoffs between precursor utilization and reaction time. Here, we demonstrate tunable control of the ALD infiltration depth into an aerogel monolith (AM) and develop a reaction-diffusion model to accurately describe the coating process. Specifically, we investigate the ALD exposure time and precursor dose needed to conformally coat a silica AM with pore sizes of ~20 nm, a monolith thickness of ~2.5 mm, and aspect ratios exceeding 60,000:1. We demonstrate complete infiltration into the AM, which is quantified by elemental mapping. A reaction-diffusion model is developed, which accounts for multiple doses and precursor depletion in the ALD chamber during an exposure step. The experimentally validated model enables the prediction and tuning of infiltration depth into a tortuous, high-aspect-ratio structure such as an AM, allowing for the synthesis of rationally designed material architectures. Additionally, the model allows for co-optimization of the total deposition time and percentage of unreacted precursor, which are important for the manufacturability and sustainability of ALD processing. Lastly, we demonstrate that ultra-thin ALD Al 2 O 3 coatings can be used to stabilize silica AMs against structural degradation under high-temperature annealing conditions (700-800 °C), by limiting changes in surface area and monolith volume. As a result, this improved high-temperature stability has implications for numerous aerogel applications, including catalysis and thermal insulation.

14 SOLAR ENERGY↗