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At least 271 records · Page 15
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Ligand Desorption and Fragmentation in Oleate-Capped CdSe Nanocrystals under High-Intensity Photoexcitation

Semiconductor nanocrystals (NCs) offer prospective use as active optical elements in photovoltaics, light-emitting diodes, lasers, and photocatalysts due to their tunable optical absorption and emission properties, high stability, and scalable solution processing, as well as compatibility with additive manufacturing routes. Over the course of experiments, during device fabrication, or while in use commercially, these materials are often subjected to intense or prolonged electronic excitation and high carrier densities. The influence of such conditions on ligand integrity and binding remains underexplored. Here, in this study, we expose CdSe NCs to laser excitation and monitor changes in oleate that is covalently attached to the NC surface using nuclear magnetic resonance as a function of time and laser intensity. Higher photon doses cause increased rates of ligand loss from the particles, with upward of 50% total ligand desorption measured for the longest, most intense excitation. Surprisingly, for a range of excitation intensities, fragmentation of the oleate is detected and occurs concomitantly with formation of aldehydes, terminal alkenes, H 2 , and water. After illumination, NC size, shape, and bandgap remain constant although low-energy absorption features (Urbach tails) develop in some samples, indicating formation of substantial trap states. The observed reaction chemistry, which here occurs with low photon to chemical conversion efficiency, suggests that ligand reactivity may require examination for improved NC dispersion stability but can also be manipulated to yield desired photocatalytically accessed chemical species.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Grain boundary facilitated dissolution of nanocrystalline NpO 2 (s) from legacy waste processing

Dissolution of actinide dioxides, including neptunium dioxide (NpO 2 (s)), is paramount for the prediction of the environmental fate of nuclear materials. Quantifying dissolution rates, as well as understanding qualitative dissolution mechanisms, informs performance assessment for geologic disposal of spent nuclear fuel and management of legacy radioactive waste. The aim of this research was to measure the dissolution rate of nanocrystalline NpO 2 (s), produced through legacy nuclear waste processing, under oxidizing conditions, as well as to characterize surface alteration to the material. The solid phase was characterized using electron microscopy techniques (SEM/STEM) and X-ray photoelectron spectroscopy (XPS), indicating preferential dissolution of Np-hydroxide contained in the grain boundaries of NpO 2 (s) and fragmentation of grains from the matrix. The oxidative dissolution was monitored over 40 weeks, yielding a two-step kinetic dissolution model involving hydration of NpO 2 (s) and subsequent oxidation and dissolution of the hydroxide phase. Here, the proposed dissolution models for nanocrystalline NpO 2 (s) suggest that microstructural features such as grain boundaries are key factors affecting dissolution, including release of colloidal particles, and ultimately, environmental fate and transport of nuclear materials.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Correcting the PFNS for more consistent fission modeling

For FY20, we had a deliverable to write a report detailing efforts to simultaneously evaluate both the prompt neutron multiplicity, $\overline{ν}$, and the prompt neutron fission neutron spectrum, PFNS, using CGMF. CGMF is the LANL-developed fission fragment decay code that consistently evaporates prompt neutrons and γ rays using the Hauser-Feshbach statistical theory of compound reactions. The decay begins by constructing the initial conditions of the fission fragments, then decaying each one from the excited state by neutrons and γ rays, conserving energy, momentum, spin, and parity in each step of the emission. The initial conditions of the fragments, along with the multiplicity, energy, and direction of each emitted neutron or γ ray, are recorded, allowing for the full reconstruction of the fission event. These event histories allow us to reconstruct average quantities, as well as correlations between observables, that can be compared with experimental or evaluated data. In that initial report, although there was already a favorable comparison between $\overline{ν}$ from CGMF, experiment, and the current ENDF/B-VIII.0 evaluation, we showed that there was still significant work to be done to improve the PFNS from CGMF. Historically, the PFNS is calculated too soft by Hauser-Feshbach fission models, and CGMF is no exception. The incorrect shape presents a significant challenge in fission modeling, including for our understanding of the fission process and for our ability to consistently calculate and predict a variety of prompt fission observables (such as fission fragment initial conditions, neutron and γ-ray multiplicities and energies, and the correlations between all observables). In our companion report, we detail our success in using CGMF to evaluate $\overline{ν}$. Although not included in the optimization explicitly, we also keep the initial conditions of the fission fragments physical, along with reproducing reasonably well the neutron multiplicity distribution. As we would expect from the sensitivities calculations from, the average neutron energies change very little from the $\overline{ν}$ optimization along with the PFNS (as will be shown in Sec. 2.6). The conclusion was that the global and statistical models would have to be investigated instead of just the fission fragment initial conditions (as is sufficient for $\overline{ν}$). This report details those efforts.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

2023 American Society for Mass Spectrometry (ASMS) 71st Annual Conference on Mass Spectrometry and Allied Topics

Title (20 words): The investigation of the mechanism for the water splitting by holmium oxide nitrate complex in gas-phase Introduction (120 words): The studies for hydrogen from water splitting is important for clean energy economy as molecular hydrogen is a potential energy carrier. Therefore, understanding the fundamental chemistry of water splitting is essential. The water splitting activated by [Ho(NO3)4]- was previously studied. The suggested mechanism was to first eliminate •NO2 from [Ho(NO3)4]- to make [HoO(NO3)3]-. Then, water was added to form [HoO(NO3)3(H2O)]-, followed by eliminating the •OH to form [HoOH(NO3)3]-. However, we proposed a new mechanism with the formation of [Ho(NO3)3]- prior to the water addition. Once water is added to this intermediate to make [Ho(NO3)3(H2O)]-, the •H is eliminated to form [HoOH(NO3)3]-. Here we have used a labeled experiments with 18-O nitrates. The results to support the new mechanism are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Alpha-decay induced shortening of fission tracks simulated by in situ ion irradiation

The diffusion of defects (e.g., vacancies and interstitials) and elements used for dating (e.g., He and Pb) in a mineral structure is a thermal process: This is the primary assumption used to determine the age and thermal history of minerals. For instance, thermal history reconstruction, through the number and length distribution of tracks produced by spontaneous fission of 238 U, is obtained by assuming a thermal event to be the only energy source for shortening of fission tracks. Here, we report a new, non-thermal energy source that induces additional shortening of fission tracks by the irradiation of alpha-recoils from the alpha-decay of 238 U and 232 Th. We simulate alpha-decay induced track-shortening by combining ion accelerator irradiations with transmission electron microscopy. This allows for the first observation of track-shrinkage during in situ ion irradiation. We show that rather than alpha-particles, alpha-recoils induce a significant shortening of fission tracks by nuclear-collisions. The shortening of track-length can be quantified as a function of alpha-decay event dose. However, apatite is less sensitive than zircon to this non-thermal process. Furthermore, the findings exemplify the interactions among different types of self-irradiation from alpha-particles, alpha-recoils and fission-fragment nuclei in single mineral grains and have important implications for the use of zircon and apatite for radiometric dating and thermochronology.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

An orphan gene BOOSTER enhances photosynthetic efficiency and plant productivity

Organelle-to-nucleus DNA transfer is an ongoing process playing an important role in the evolution of eukaryotic life. Here, genome-wide association studies (GWAS) of non-photochemical quenching parameters in 743 Populus trichocarpa accessions identified a nuclear-encoded genomic region associated with variation in photosynthesis under fluctuating light. The identified gene, BOOSTER (BSTR), comprises three exons, two with apparent endophytic origin and the third containing a large fragment of plastid-encoded Rubisco large subunit. Higher expression of BSTR facilitated anterograde signaling between nucleus and plastid, which corresponded to enhanced expression of Rubisco, increased photosynthesis, and up to 35% greater plant height and 88% biomass in poplar accessions under field conditions. Overexpression of BSTR in Populus tremula × P. alba achieved up to a 200% in plant height. Similarly, Arabidopsis plants heterologously expressing BSTR gained up to 200% in biomass and up to 50% increase in seed.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2025

Protoplast fusion as a strategy to increase ploidy in Rhodotorula toruloides for strain development

Rhodotorula toruloides is a red oleaginous yeast with growing commercial interest because of its hardiness and exceptional lipid production capacity. Because it is a basidiomycete yeast with a complex life cycle, many of the classical breeding methods used with ascomycetes are unavailable for strain improvement. However, we have been able to construct polyploid yeast by fusing protoplasts of parents with the same mating type. Fusing of Y-6985 (A2) and Y-48190 (A2), which had been transformed with complementary antibiotic markers, led to the recovery of two diploids and one triploid. The stability of the fusion yeasts was tested by plating them on non-selective medium after several growth cycles under antibiotics and then testing five colonies per strain for nuclear DNA contents using flow cytometry and standard cell cycle analysis: the triploid and one diploid were stable. Fusants inherited their mitochondria from a single parent, which was demonstrated using restriction fragment length polymorphism (RFLP) of mitochondrial DNA. The phenotypic properties of the parents and fusants were compared in glucose fed-batch bioreactor studies and cellulosic sugar batch cultures. The final lipid titers for the fed-batch cultures were 24.9–39.7 g/L with Y-6985 and the diploid and triploid performing the best and worst, respectively. The fusants demonstrated intermediate hardiness for growth on hydrolysate prepared with dilute-acid pretreated switchgrass and were outperformed by Y-48190. Unlike one of the haploid parents, the fusants grew in 70% v/v concentrated hydrolysate. Furthermore, they did not grow as fast as the other haploid. In this study, a modernized protoplast fusion method is resurrected a useful tool for strain development in this yeast, which is complementary with other available methods.

Lignocellulose↗
DOE OSTI2024

Relativistic effects in Green's function Monte Carlo calculations of neutrino-nucleus scattering

Here, microscopic calculations of neutrino-nucleus scattering cross sections are critical for the success of the neutrino-oscillation program. In addition to retaining nuclear correlations in the initial and final state of the reaction, they are based on consistent nuclear interactions and transition current operators, thereby enabling robust uncertainty quantification. In this work, we address a significant limitation of these microscopic methods, which arises from their nonrelativistic nature. By performing the calculations in a reference frame that minimizes nucleon momenta and utilizing the so-called two-fragment model, we extend the applicability of Green's function Monte Carlo calculations of neutrino-nucleus scattering to higher momenta than currently possible. To validate this approach, we compare our theoretical predictions against inclusive data measured by the MiniBooNE, T2K, and MINER ν A experiments.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Precise measurement of nuclear interaction cross sections towards neutron-skin determination with R 3 B

The R 3 B (Reactions with Relativistic Radioactive Beams) experiment as a major instrument of the NUSTAR collaboration for the research facility FAIR in Darmstadt is designed for kinematically complete studies of reactions with high-energy radioactive beams. Part of the broad physics program of R 3 B is to constrain the asymmetry term in the nuclear equation-of-state and hence improve the description of highly asymmetric nuclear matter (e.g., in neutron stars). For a precise determination of the neutron-skin thickness – an observable which is directly correlated with the symmetry energy in theoretical calculations – by measuring absolute fragmentation cross sections, it is essential to quantify the uncertainty and challenge the reaction model under stable conditions. During the successful FAIR Phase-0 campaign of R 3 B, we precisely measured the energy dependence of total interaction cross sections in 12 C + 12 C collisions, for a direct comparison with calculations based on the eikonal reaction theory.

Ponnath, L. (ORCID:0000000286742624)↗
DOE OSTI2021

Cumulative short-lived photofission product yields for nuclear forensic application

Experiments have long been carried out with linear accelerator (linac) produced bremsstrahlung X-rays to study high-energy photon-induced fission, known as “photofission”. One benefit of photofission, when compared with neutron-induced fission, is the ability to investigate fundamental physics of fission at excitation energies lower than what is possible with neutrons [1]. Absorption of an incident neutron results in a compound nucleus with an excitation energy at least equal to the neutron binding energy; thus, the lowest energy region of the fission barrier cannot be studied. Fission product yield distributions are dependent on the incident particle energy and the target nucleus mass. They are generally represented by a double-humped curve, with low and high mass “peaks” and an intermediate mass “valley”. As incident particle energy increases, the excitation energy of the nucleus increases, thereby increasing the overall yield of isotopes in the valley with respect to the two maxima or peaks of the fission product curve [3]. Photofission is most probable for incident photons around 14 MeV due to the giant dipole resonance. Induced photofission around this energy results in a fission product yield distribution that resembles 14 MeV DT neutron fission more than thermal or fast (500 keV) neutron fission. In post-detonation nuclear forensics, the peak-to-valley ratio of the fission product yield curve could be used for characterizing device type by providing an indication of the neutron energy spectrum that had induced fission (e.g., 500 keV vs. 14 MeV). The goal of this work is to improve nuclear data for isotopes of interest in nuclear forensics and special nuclear material (SNM) detection, specifically the fission product yield data via photofission experiments for the isotopes of 238U and 232Th. Photofission has been proposed as a less costly and more flexible production method for the valley isotopes that are representative of DT neutron fission product yield distributions, which would benefit nuclear forensics exercises in testing for analysis techniques. Natural uranium and thorium targets were irradiated with bremsstrahlung photons (nominal endpoint energies of 8, 14, and 20 MeV), generated via impingement of high-energy electrons on a tungsten electron-to-photon radiator. Gamma-ray spectroscopy was used to observe and identify the decay of the resulting fission products. The photofission yields of 102 fission products were measured for the set of the 238U and 232Th targets at the three bremsstrahlung X-ray endpoint energies 8, 14, and 20 MeV. These fragments included masses ranging from A=84 to A=144, with half-lives as short as 1.07 seconds.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2023

ECCE unpolarized TMD measurements

For this work, we performed feasibility studies for various measurements that are related to unpolarized TMD distribution and fragmentation functions for the ECCE detector proposal. The processes studied include semi-inclusive Deep inelastic scattering (SIDIS) where single hadrons (pions and kaons) were detected in addition to the scattered DIS lepton. The single hadron cross sections and multiplicities were extracted as a function of the DIS variables x and Q 2 , as well as the semi-inclusive variables z, which corresponds to the momentum fraction the detected hadron carries relative to the struck parton and P T , which corresponds to the transverse momentum of the detected hadron relative to the virtual photon. The expected statistical precision of such measurements is extrapolated to accumulated luminosities of 10 fb –1 and potential systematic uncertainties are approximated given the deviations between true and reconstructed yields. The expected uncertainties are then used to obtain the expected impact on the related TMD distribution and fragmentation functions. We find that the ECCE detector proposal fulfills the physics requirements on these channels as detailed in the EIC Yellow Report.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Stepwise deprotonation of truxene: structures, metal complexation, and charge-dependent optical properties

As a planar subunit of C 60 -fullerene, truxene (C 27 H 18 ) represents a highly symmetrical rigid hydrocarbon with strong blue emission. Herein, we used truxene as a model to investigate the chemical reactivity of a fullerene fragment with alkali metals. Monoanion, dianion, and trianion products with different alkali metal counterions were crystallized and fully characterized, revealing the core curvature dependence on charge and alkali metal coordination. Moreover, a proton nuclear magnetic resonance study coupled with computational analysis demonstrated that deprotonation of the aliphatic CH 2 segments introduces aromaticity in the five-membered rings. Importantly, the UV-vis absorption and photoluminescence of truxenyl anions with different charges reveal intriguing charge-dependent optical properties, implying variation of the electronic structure based on the deprotonation process. An increase in aromaticity and π-conjugation yielded a red shift in the absorption and photoluminescent spectra; in particular, large Stokes shifts were observed in the truxenyl monoanion and dianion with high emission quantum yield and time of decay. Overall, stepwise deprotonation of truxene provides the first crystallographically characterized examples of truxenyl anions with three different charges and charge-dependent optical properties, pointing to their potential applications in carbon-based functional materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Correlations Between Fission Fragment and Neutron Anisotropies in Neutron-Induced Fission

Several sources of angular anisotropy for fission fragments and prompt neutrons have been studied in neutron-induced fission reactions. These include kinematic recoils of the target from the incident neutron beam and the fragments from the emission of the prompt neutrons, preferential directions of the emission of the fission fragments with respect to the beam axis due to the population of particular transition states at the fission barrier, and forward-peaked angular distributions of pre-equilibrium neutrons which are emitted before the formation of a compound nucleus. In addition, there are several potential sources of angular anisotropies that are more difficult to disentangle: the angular distributions of prompt neutrons from fully accelerated fragments or from scission neutrons, and the emission of neutrons from fission fragments that are not fully accelerated. Here, we study the effects of the first group of anisotropy sources, particularly exploring the correlations between the fission-fragment anisotropy and the resulting neutron anisotropy. While kinematic effects were already accounted for in our Hauser-Feshbach Monte Carlo code cgmf, anisotropic angular distributions for the fission fragments and pre-equilibrium neutrons resulting from neutron-induced fission on 233,234,235,238 U, 239,241 Pu, and 237 Np have been introduced for the first time. The effects of these sources of anisotropy are examined over a range of incident neutron energies, from thermal to 20 MeV, and compared with experimental data from the Chi-Nu liquid scintillator array. The anisotropy of the fission fragments is reflected in the anisotropy of the prompt neutrons, especially as the outgoing energy of the prompt neutrons increases, allowing for an extraction of the fission-fragment anisotropy to be made from a measurement of the neutrons.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Antiferromagnetic Ordering in Quasi-One-Dimensional FeBi 4 S 7

Here, we report a detailed study of the synthesis, composition, magnetic structure, and transport properties of a quasi-one-dimensional antiferromagnet FeBi 4 S 7 that contains chains of edge-sharing FeS 6 octahedra. High-resolution powder X-ray diffraction (PXRD) analysis, aided by variation of synthetic conditions, suggests that the true formula of the material is Fe 1.2 Bi 3.8 S 7 , due to the minor substitution of Fe into Bi sites. This finding is in agreement with crystal structure refinement from neutron powder diffraction data as well as with the small band gap of 0.23 eV determined from electrical transport measurements. Analysis of the neutron diffraction pattern collected below the antiferromagnetic ordering temperature of 64 K revealed ferromagnetic coupling between the Fe moments in the chains of FeS 6 octahedra. The overall ordering, however, is antiferromagnetic due to the antiparallel arrangement of moments on neighboring chains. The collinear spin arrangement is described by a k-vector (1, 0, 1/2), which indicates doubling of the unit cell in the c direction and the loss of the C-centering translation as compared to the nuclear cell. The ferromagnetic nature of the sulfide-bridged chains of Fe 2+ ions in FeBi 4 S 7 , in contrast to the antiferromagnetic coupling between Fe moments in compounds with similar structural fragments, can be justified by the analysis of metric parameters that characterize the Fe–S bonding in these materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

ECCE sensitivity studies for single hadron transverse single spin asymmetry measurements

Here, we performed feasibility studies for various single transverse spin measurements that are related to the Sivers effect, transversity and the tensor charge, and the Collins fragmentation function. The processes studied include semi-inclusive deep inelastic scattering (SIDIS) where single hadrons (pions and kaons) were detected in addition to the scattered DIS lepton. The data were obtained in pythia6 and geant4 simulated e+p collisions at 18 GeV on 275 GeV, 18 on 100, 10 on 100, and 5 on 41 that use the ECCE detector configuration. Typical DIS kinematics were selected, most notably Q 2 >1 GeV 2 , and cover the x range from 10 -4 to 1. The single spin asymmetries were extracted as a function of x and Q 2 , as well as the semi-inclusive variables z, which corresponds to the momentum fraction the detected hadron carries relative to the struck parton, and P T , which corresponds to the transverse momentum of the detected hadron relative to the virtual photon. They are obtained in azimuthal moments in combinations of the azimuthal angles of the hadron transverse momentum and transverse spin of the nucleon relative to the lepton scattering plane. In order to extract asymmetries, the initially unpolarized MonteCarlo was re-weighted in the true kinematic variables, hadron types and parton flavors based on global fits of fixed target SIDIS experiments and e + e – annihilation data. The expected statistical precision of such measurements is extrapolated to 10 fb –1 and potential systematic uncertainties are approximated given the deviations between true and reconstructed yields. Similar neutron information is obtained by comparing the ECCE e+p pseudo-data with the same from the EIC Yellow Report and scaling the corresponding Yellow Report e+ 3 He pseudo-data uncertainties accordingly. The impact on the knowledge of the Sivers functions, transversity and tensor charges, and the Collins function has then been evaluated in the same phenomenological extractions as in the Yellow Report. Finally, the impact is found to be comparable to that obtained with the parametrized Yellow Report detector and shows that the ECCE detector configuration can fulfill the physics goals on these quantities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Permethylation as a strategy for high–molecular–weight polysaccharide structure analysis by nuclear magnetic resonance—Case study of Xylella fastidiosa extracellular polysaccharide

Current practices for structural analysis of extremely large-molecular-weight polysaccharides via solution-state nuclear magnetic resonance (NMR) spectroscopy incorporate partial depolymerization protocols that enable polysaccharide solubilization in suitable solvents. Non-specific depolymerization techniques utilized for glycosidic bond cleavage, such as chemical degradation or ultrasonication, potentially generate structural fragments that can complicate complete and accurate characterization of polysaccharide structures. Utilization of appropriate enzymes for polysaccharide degradation, on the other hand, requires prior structural knowledge and optimal enzyme activity conditions that are not available to an analyst working with novel or unknown compounds. Herein, we describe an application of a permethylation strategy that allows the complete dissolution of intact polysaccharides for NMR structural characterization. This approach is utilized for NMR analysis of Xylella fastidiosa extracellular polysaccharide (EPS), which is essential for the virulence of the plant pathogen that affects multiple commercial crops and is responsible for multibillion dollar losses each year.

13C↗
DOE OSTI2020

Polyoxometalate-based complexes as ligands for the study of actinide chemistry

The complexation of actinide cations by polyoxometalates (POMs) has been extensively studied over the past 50 years. In this perspective article, we present the rich structural diversity of actinide-POM complexes and their contribution to the extension of our knowledges of actinide chemistry, especially regarding aspect of their redox chemistry, as well as application for the capture and separation of these cations in the context of nuclear fuel remediation. Furthermore, these heterometallic assemblies have also proven highly valuable as model for heterogeneous systems based on actinides supported by metal oxide surfaces. In particular, activation of the An–O bond of actinyl fragments upon complexation with lacunary POMs has been reported, creating opportunities for future developments regarding the reactivity of these heterometallic assemblies.

Auvray, Thomas↗
DOE OSTI2020

Total kinetic energy and mass yields from the fast neutron-induced fission of $^{239}\hbox {Pu}$

The total kinetic energy (TKE) release in fission is an important observable, constituting over 80% of the energy released in fission (E f ≈ 200MeV). While the TKE release in the 239 Pu(n,f) reaction was previously measured up to 50 MeV incident neutron energy (E n ), there were features in TKE release at the highest values of E n that were puzzling. There was a marked flattening of TKE release from E n = 30 to 50 MeV, in disagreement with the clearly decreasing TKE observed from E n = 0.5 to 30 MeV. To verify and clarify this trend, TKE measurements at higher values of E n were made. We present absolute measurements of TKE release in 239 Pu(n,f) from E n = 2.4 to 100 MeV. Here, we used silicon PIN detectors to measure the fragment energies and deduce mass-yield curves using the 2E-method. We also discuss fission asymmetry and the relationships between approx. fission fragment mass and distortion.

239Pu↗