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DOE OSTI2023

Facile Room-Temperature Electrodeposition of Rare Earth Metals in a Fluorine-Free Task-Specific Electrolyte

Electrochemical deposition of rare earth metals at room temperature has attracted increasing interest due to its advantage in energy efficiency over traditional hydrometallurgical and pyrometallurgical processes. Recent progress has been made with fluorinated electrolyte systems; however, the formation of an electrode-passivating fluoride layer by electrolyte decomposition is often overlooked. Such a passivation layer causes significant and rapid decay of the deposition current and significantly hinders practical application. To address this issue, we demonstrate a fluorine (F)-free task-specific electrolyte utilizing the borohydride anion for the efficient electrodeposition of rare earth metals. By eliminating the passivation effect, the deposition process exhibits a stable current and accumulates a thick neodymium deposit on the electrode. Raman spectroscopy of the electrolyte reveals a synergetic effect between rare earth borohydride and lithium borohydride which promotes the dissociation of both borohydride salts, resulting in significantly increased ionic conductivity and electrochemical performance. Cyclic voltammetry and in-depth X-ray photoelectron spectroscopy of the deposits suggest that the electrodeposition of rare earth metals could undergo a Li-mediated reduction process. Finally, quantitative analysis of the deposits reveals that the overall concentration of the rare earth elements reaches 75% which contains 40–48% metallic phase.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Theory of nuclear fission

Atomic nuclei are quantum many-body systems of protons and neutrons held together by strong nuclear forces. Under the proper conditions, nuclei can break into two (sometimes three) fragments which will subsequently decay by emitting particles. This phenomenon is called nuclear fission. Since different fission events may produce different fragmentations, the end-products of all fissions that occurred in a small chemical sample of matter comprise hundreds of different isotopes, including α particles, together with a large number of emitted neutrons, photons, electrons and antineutrinos. The extraordinary complexity of this process, which happens at length scales of the order of a femtometer, mostly takes less than a femtosecond but is not entirely over until all the lingering β decays have completed – which can take years – is a fascinating window into the physics of atomic nuclei. While fission may be more naturally known in the context of its technological applications, it also plays a crucial role in the synthesis of heavy elements in astrophysical environments. In both cases, simulations are needed for the many systems or energies inaccessible to experiments in the laboratory. In this context, the level of accuracy and precision required poses formidable challenges to nuclear theory. Overall, the goal of this article is to provide a comprehensive overview of the theoretical methods employed in the description of nuclear fission.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2019

Formation and stability of long basal-prismatic facets in Mg

Long BP facets bounding {101¯2} 1¯011 twins in Mg ( ≥ 4nm) have been observed experimentally. However, the formation of these long BP facets has not been studied and their contribution/role to the twin growth remains unclear. We observed a long straight BP facet (27 nm) using high-resolution transmission electron microscopy (HRTEM) and investigated its formation, stability, and mobility by atomistic simulations. Experimentally, a serrated twin interface containing short CTBs and short BP facets near a (101¯2) twin tip is observed to transform under the effects of the electron beam into a long straight semi-coherent BP facet that contains disclination dipoles. Molecular dynamics (MD) simulations of the relaxation of a 3D twin domain reveals another process whereby a long partially-relaxed BP interface forms and contains an I 2 stacking fault. A comparison between the energy of these configurations as obtained by atomistic simulations suggests that these transformations occur in two steps: (1) serrated interfaces composed of coherent BP segments with lengths less than 2 nm combine and form a long and straight coherent BP facets and (2) these long coherent BP facets quickly transform into relaxed ones with misfit defects. Importantly, it is found that long BP facets are relatively immobile, and upon reloading, decay into more mobile serrated interfaces prior to migrating. Here, the work presented suggests that the atomistic configurations of BP facets during twin growth processes differ significantly from relaxed BP interfaces that would be observed by TEM.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Amplitude analysis and branching-fraction measurement of ${D}_s^{+}\to {K}_S^0{\pi}^{+}{\pi}^0$

By using 6.32 fb -1 of data collected with the BESIII detector at center-of-mass energies between 4.178 and 4.226 GeV, we perform an amplitude analysis of the decay $D^+_s$→$K^0_Sπ^+π^0$ and determine the relative fractions and phase differences of different intermediate processes, which include $K^0_Sρ$(770) + ,$K^0_Sρ$(1450) + , $K^*$(892)$^0π^+$, $K^*$(892)$^+π^0$, and $K^*$(1410)$^0π^+$. With the detection efficiency based on the amplitude analysis results, the absolute branching fraction is measured to be $\mathcal{B}$($D^+_s$→$K^0_Sπ^+π^0$)=(5.43±0.30 stat ±0.15 syst )×10 -3 .

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2018

High-fidelity quantum gates on quantum-dot-confined electron spins in low-Q optical microcavities

We propose some high-fidelity quantum circuits for quantum computing on electron spins of quantum dots (QD) embedded in low-Q optical microcavities, including the two-qubit controlled-NOT gate and the multiple-target-qubit controlled-NOT gate. The fidelities of both quantum gates can, in principle, be robust to imperfections involved in a practical input–output process of a single photon by converting the infidelity into a heralded error. Furthermore, the influence of two different decay channels is detailed. By decreasing the quality factor of the present microcavity, we can largely increase the efficiencies of these quantum gates while their high fidelities remain unaffected. This proposal also has another advantage regarding its experimental feasibility, in that both quantum gates can work faithfully even when the QD-cavity systems are non-identical, which is of particular importance in current semiconductor QD technology.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Tuning the Quantum Dot (QD)/Mediator Interface for Optimal Efficiency of QD-Sensitized Near-Infrared-to-Visible Photon Upconversion Systems

Lead sulfide (PbS) quantum dots (QDs) have shown promising performance as a sensitizer in infrared-to-visible photon upconversion systems. To investigate the key design rules, we compare three PbS-sensitized upconversion systems using three mediator molecules with the same tetracene triplet acceptor at different distances from the QD. Using transient absorption spectroscopy, we directly measure the triplet energy-transfer rates and efficiencies from the QD to the mediator and from the mediator to the emitter. With increasing distance between the mediator and PbS QD, the efficiency of the first triplet energy transfer from the QD to the mediator decreases because of a decrease in the rate of this triplet energy-transfer step, while the efficiency of the second triplet energy transfer from the mediator to the emitter increases because of a reduction in the QD-induced mediator triplet state decay. The latter effect is a result of the slow rate constant of the second triplet energy-transfer process, which is 3 orders of magnitude slower than the diffusion-limited value. The combined results lead to a net decrease of the steady-state upconversion quantum yield with distance, which could be predicted by our kinetic model. Our result shows that the QD/mediator interface affects both the first and second triplet energy transfer processes in the photon upconversion system, and the QD/mediator distance has an opposite effect on the efficiencies of the first and second triplet energy transfer. Lastly, these findings provide important insight for the further rational improvement of the overall efficiency of QD-based upconversion systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Astrophysical neutrino production diagnostics with the Glashow resonance

We study the Glashow resonance ν-bar {sub e} + e {sup −} → W {sup −} → hadrons at 6.3 PeV as diagnostic of the production processes of ultra-high energy neutrinos. The focus lies on describing the physics of neutrino production from pion decay as accurate as possible by including the kinematics of weak decays and Monte Carlo simulations of pp and pγ interactions. We discuss optically thick (to photohadronic interactions) sources, sources of cosmic ray ''nuclei'' and muon damped sources. Even in the proposed upgrade IceCube-Gen2, a discrimination of scenarios such as pp versus pγ is extremely challenging under realistic assumptions. Nonetheless, the Glashow resonance can serve as a smoking gun signature of neutrino production from photohadronic (Aγ) interactions of heavier nuclei, as the expected Glashow event rate exceeds that of pp interactions. We finally quantify the exposures for which the non-observation of Glashow events exerts pressure on certain scenarios.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2019

Binding energy and lifetime of excitons in metallic nanotubes

The difficulty of describing excitons in semiconducting single-wall nanotubes analytically lies with the fact that excitons can neither be considered strictly one- nor two-dimensional objects. However, the situation changes in the case of metallic nanotubes where, by virtue of screening from gapless metallic subbands, the radius of the exciton becomes much larger than the radius of the nanotube R ex >> R. Taking advantage of this, we develop the theory of excitons in metallic nanotubes, determining that their binding energy is about 0.08v/R, in agreement with the existing experimental data. Additionally, because of the presence of the gapless subbands, there are processes where bound excitons are scattered into unbound electron-hole pairs belonging to the gapless subbands. Such processes lead to a finite exciton lifetime and the broadening of its spectral function. Here, we calculate the corresponding decay rate of the excitons.

excitons↗

DOE OSTI2013

Charmonium production in proton-proton collisions and in collisions of lead nuclei at CERN and comparison with Brookhaven data

A review of experimental data on charmoniumproduction that were obtained in fixed-target experiments at the SPS synchrotron and in proton-proton collisions and in collisions of lead nuclei in beams of the Large Hadron Collider (LHC) at CERN (Switzerland) is presented. A comparison with data obtained at the Brookhaven National Laboratory (USA) from experiments at the Relativistic Heavy Ion Collider (RHIC) is performed. Measurement of the suppression of J/{psi}-meson production as a possible signal of the production of quark-gluon plasmawas proposed back in 1986 by T. Matsui and H. Satz. An anomalous suppression of J/{psi}-meson production was discovered by the NA50 Collaboration at SPS (CERN) in central collisions of lead nuclei at the c.m. collision energy of 158 GeV per nucleon. Data obtained at the c.m. energy of 200 GeV per nucleon in the PHENIX experiment at RHIC indicate that, depending on multiplicity, the suppression of J/{psi}-meson production at this energy approximately corresponds to the suppression of J/{psi}-meson production in collisions of lead nuclei at the SPS accelerator. Theoretical models that take into account the regeneration of J/{psi} mesons describe better RHIC experimental data. The measurement of charmonium production in proton-proton collisions and in collisions of lead nuclei in LHC beams revealed the importance of taking into account the regeneration process. At the LHC energies, it is also necessary to take into account the contribution of B-meson decays. Future measurements of charmonium production at the LHC to a higher statistical precision and over an extended energy region would be of importance for obtaining deeper insight into the mechanism of charmonium production and for studying the properties of matter at high energy density and temperature.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2012

Search for New Physics in the Exclusive $\gamma_{Delayed}$ + Missing Transverse Energy Channel in $p\bar{p}$ collisions at $\sqrt{s}$ = 1.96 TeV

This dissertation presents the results of a search in the exclusive photon plus missing transverse energy ( γ + E T ) finnal state in proton antiproton collisions at a center of mass energy of 1.96 TeV using the Collider Detector at Fermilab experiment. The strategy used here is to search for delayed photons coming from gauge mediated supersymmetric events with the exclusive production of X ~0 1 → γG ~ . In these models the ~ 01 is the lightest neutralino and has nanosecond lifetime before decaying to a photon ( γ) and gravitino ( ~ G) which exits the detector unrecorded. In order to search for this process we select collisions that have a single photon plus missing transverse energy and little other activity in the detector and examine the arrival time of the photon. This arrival time is then compared against expectations from a data driven background of the standard model sources. In the data collected from the Fermilab Tevatron collider from December 2004 to June 2010, representing 6.3 fb -1 of data, we observe 322 events in the photon arrival timing region from 2 nanoseconds to 7 nanoseconds with a data driven background prediction of 257 ± 35. An excess of 65 events is observed, equivalent to a standard deviation (N σ ) of 1.65 from the null hypothesis.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2026

Assessment of Molybdate Based Corrosion Inhibitor for use at the Savannah River Tank Farm Cooling Water System

The Savannah River Site (SRS) has relied on 51 underground storage tanks, many dating back to the 1950s, to store radioactive liquid waste generated from nuclear processing and radionuclide production. These tanks use carbon steel cooling coils, cooled by soft, acidic water, to dissipate the decayed heat produced by radioactive waste. For decades, following historical industry practices, chromate has been added to the cooling water (~450 ppm at pH 9-11) to effectively inhibit corrosion, ensuring cooling coil longevity. Inspections of failed coils reveal that chromate-treated surfaces are generally well-preserved.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS1971

Chemical physics of molecules and continuous channel electron multipliers

The A approaches X, B approaches X and B approaches A bands of CO(+) have been excited using monochromatic photons and the band intensities measured. Using such data the variations of the electronic transition moments for these above emission bands as well as for the absorption bands have been determined. Further, the specific cross sections for the absorption processes have been determined by measuring the total emission intensity in the band system through which the upper state decays. The band intensity measurements and the derived results are presented.

Judge, D. L.↗

NASA NTRS1974

The lunar atmosphere

In contrast to the earth's atmosphere, the atmosphere of the moon is exceedingly tenuous and appears to consist mainly of noble gases. The solar wind impinges on the lunar surface, supplying detectable amounts of helium, neon and Ar-36. Influxes of solar wind protons and carbon and nitrogen ions are significant, but atmospheric gases containing these elements have not been positively identified. Radiogenic Ar-40 and Rn-222 produced within the moon have been detected. The present rate of effusion of argon from the moon accounts for about 0.4% of the total production of Ar-40 due to decay of K-40 if the average abundance of potassium in the moon is 1000 ppm. Lack of weathering processes in the regolith suggests that most of the atmospheric Ar-40 originates deep in the lunar interior, perhaps in a partially molten core. If so, other gases may be vented along with the argon.

Hodges, R. R., Jr.↗

NASA NTRS1987

Determination of lifetime and surface recombination velocity of p-n junction solar cells and diodes by observing transients

The unified view of transient methods for the determination of recombination lifetime tau and back surface recombination velocity S presented here for silicon solar cells and diodes attempts to define limitations of existing methods and to evolve improvements. The presence of sizable junction capacitance for silicon devices under forward voltage invalidates the use of conventional open-circuit voltage decay (OCVD) and reverse recovery. This led Green (1983) to his method of compensated open-circuit voltage decay, in which the addition of an external resistor shunting the solar cell partially corrects for the presence of the junction capacitance. Setting this resistance to zero produces an electrical short-circuit current-decay method, which has the advantage of enabling determination of both tau and S. In an alternate approach, one may insert the functional dependence of the junction capacitance on forward voltage. This new method, denoted by the acronym OCVDCAP, enables the determination of tau with apparently greater accuracy than that obtained by previous methods utilizing voltage transients. But OCVDCAP has in common with the previous methods that it determines tau only and has practical utility only for determining tau of long-base devices. This means that it is useful only for thick base regions. In principle, however, it has an advantage over short-circuit current decay: it requires only pressure contacts, not ohmic contacts, and therefore may be used to determine tau after key processing steps in manufacturing.

Lindholm, Fredrik A.↗

NASA NTRS1990

Spallation processes and nuclear interaction products of cosmic rays

Most cosmic-ray nuclei heavier than helium have suffered nuclear collisions in the interstellar gas, with transformation of nuclear composition. The isotopic and elemental composition at the sources has to be inferred from the observed composition near the Earth. The source composition permits tests of current ideas on sites of origin, nucleosynthesis in stars, evolution of stars, the mixing and composition of the interstellar medium and injection processes prior to acceleration. The effects of nuclear spallation, production of radioactive nuclides and the time dependence of their decay provide valuable information on the acceleration and propagation of cosmic rays, their nuclear transformations, and their confinement time in the Galaxy. The formation of spallation products that only decay by electron capture and are relatively long-lived permits an investigation of the nature and density fluctuations (like clouds) of the interstellar medium. Since nuclear collisions yield positrons, antiprotons, gamma rays and neutrinos, we shall discuss these topics briefly.

Non-NASA Center↗

NASA NTRS2014

Determining the Source of Water Vapor in a Cerium Oxide Electrochemical Oxygen Separator to Achieve Aviator Grade Oxygen

More than a metric ton of water is transported to the International Space Station (ISS) each year to provide breathing oxygen for the astronauts. Water is a safe and compact form of stored oxygen. The water is electrolyzed on ISS and ambient pressure oxygen is delivered to the cabin. A much smaller amount of oxygen is used each year in spacesuits to conduct Extra Vehicular Activities (EVAs). Space suits need high pressure (>1000 psia) high purity oxygen (must meet Aviator Breathing Oxygen "ABO" specifications, >99.5% O2). The water / water electrolysis system cannot directly provide high pressure, high purity oxygen, so oxygen for EVAs is transported to ISS in high pressure gas tanks. The tanks are relatively large and heavy, and the majority of the system launch weight is for the tanks and not the oxygen. Extracting high purity oxygen from cabin air and mechanically compressing the oxygen might enable on-board production of EVA grade oxygen using the existing water / water electrolysis system. This capability might also benefit human spaceflight missions, where oxygen for EVAs could be stored in the form of water, and converted into high pressure oxygen on-demand. Cerium oxide solid electrolyte-based ion transport membranes have been shown to separate oxygen from air, and a supported monolithic wafer form of the CeO2 electrolyte membrane has been shown to deliver oxygen at pressures greater than 300 psia. These supported monolithic wafers can withstand high pressure differentials even though the membrane is very thin, because the ion transport membrane is supported on both sides (Fig 1). The monolithic supported wafers have six distinct layers, each with matched coefficients of thermal expansion. The wafers are assembled into a cell stack which allows easy air flow across the wafers, uniform current distribution, and uniform current density (Fig 2). The oxygen separation is reported to be "infinitely selective" to oxygen [1] with reported purity of 99.99% [2]. Combined with a mechanical compressor, a Solid Electrolyte Oxygen Separator (SEOS) should be capable of producing ABO grade oxygen at pressures >2400 psia, on the space station. Feasibility tests using a SEOS integrated with a mechanical compressor identified an unexpected contaminant in the oxygen: water vapour was found in the oxygen product, sometimes at concentrations higher than 40 ppm (the ABO limit for water vapour is 7 ppm). If solid electrolyte membranes are really "infinitely selective" to oxygen as they are reported to be, where did the water come from? If water is getting into the oxygen, what other contaminants might get into the oxygen? Microscopic analyses of wafers, welds, and oxygen delivery tubes were performed in an attempt to find the source of the water vapour contamination. Hot and cold pressure decay tests were performed. Measurements of water vapour as a function of O2 delivery rate, O2 delivery pressure, and process air humidity levels were the most instructive in finding the source of water contamination (Fig 3). Water contamination was directly affected by oxygen delivery rate (doubling the oxygen production rate cut the water level in half). Water was affected by process air humidity levels and delivery pressure in a way that indicates the water was diffusing into the oxygen delivery system.

Graf, John↗

DOE OSTI2024

A Measurement of the Eta Meson Radiative Decay Width via the Primakoff Effect

The ? meson is an interesting tool to study fundamental symmetries in Quantum Chromodynamics (QCD). In particular, its radiative decay width, ? p? Ñ ??q, is an important quantity that can be predicted in the framework of Chiral Perturbation Theory. A precision measurement of this quantity would provide critical inputs to understanding the mixing of the ? and ?1 mesons and extracting constants with wide-ranging applications in low-energy QCD. This decay width has been measured in the past using two different experimental techniques. The more popular technique utilized e`e´ collisions to produce ? mesons through electromagnetic interactions. Today, the Particle Data Group (PDG) averages the results of five such experiments to obtain their currently-accepted value of the decay width as: 0.515?0.018 keV. However the first measurement of this quantity was obtained from a fixed-target experiment that measured the cross section for photoproduction of ? mesons on a nuclear target via the Primakoff effect. Their result of 0.324?0.046 keV shows strong tension with the average of the collider measurements, motivating a new, high precision measurement using the Primakoff method. For this purpose, the PrimEx-eta experiment was conducted in Hall D of the Thomas Jefferson National Accelerator Facility (Jefferson Lab or JLab). The data is currently being analyzed to measure the differential cross section for the photoproduction of ? mesons on a liquid, 4He target. Preliminary results obtained from the analysis of the first phase of the PrimEx-eta experiment show reasonable agreement with the currently-accepted PDG value of the radiative decay width. However, as will be discussed, there are many challenges to this precision measurement which must be studied before any results can be finalized and compared with previous measurements. In parallel to the ? decay width measurement, the PrimEx-eta experiment measured the total cross section for the fundamental, Quantum Electrodynamics (QED) process of Compton scattering from the atomic electrons inside the target. The results obtained from this measurement are in strong agreement with the next-to-leading order QED calculations, and the total combined uncertainties are below 3% for incident photon energies between 7-10 GeV. In addition to providing the first precision measurement of the total Compton scattering cross section within this beam energy range, this measurement verifies the capability of the PrimEx-eta experimental setup to perform absolute cross section measurements at forward angles, and serves as a reference process for the calibration of systematic uncertainties.

Smith, Andrew↗

DOE OSTI2018

Unlocking preservation bias in the amber insect fossil record through experimental decay

Fossils entombed in amber are a unique resource for reconstructing forest ecosystems, and resolving relationships of modern taxa. Such fossils are famous for their perfect, life-like appearance. However, preservation quality is vast with many sites showing only cuticular preservation, or no fossils. The taphonomic processes that control this range are largely unknown; as such, we know little about potential bias in this important record. Here we employ actualistic experiments, using, fruit flies and modern tree resin to determine whether resin type, gut microbiota, and dehydration prior to entombment affects decay. We used solid phase microextraction gas chromatography-mass spectrometry (SPME GC-MS) to confirm distinct tree resin chemistry; gut microbiota of flies was modified using antibiotics and categorized though sequencing. Decay was assessed using phase contrast synchrotron tomography. Resin type demonstrates a significant control on decay rate. The composition of the gut microbiota was also influential, with minor changes in composition affecting decay rate. Dehydration prior to entombment, contrary to expectations, enhanced decay. Our analyses show that there is potential significant bias in the amber fossil record, especially between sites with different resin types where ecological completeness and preservational fidelity are likely affected.

59 BASIC BIOLOGICAL SCIENCES↗

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