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Moisture-Induced Alumina Scale Spallation: The Hydrogen Factor

For some time the oxidation community has been concerned with interfacial spallation of protective alumina scales, not just upon immediate cool down, but as a time-delayed phenomenon. Moisture-induced delayed spallation (MIDS) and desktop spallation (DTS) of thermal barrier coatings (TBCs) refer to this process. It is most apparent for relatively adherent alumina scales that have survived initial cool down in a dry environment, have built up considerable thickness and strain energy, and have been somewhat damaged, such as by cyclic oxidation cracking. Indeed, a "sensitive zone" can be described that maximizes the observed effect as a function of all the relevant factors. Moisture has been postulated to serve as a source of interfacial hydrogen embrittlement. Hydrogen is derived from reaction with aluminum in the alloy at an exposed interface. The purpose of this monograph is to trace the close analogy of this phenomenon to other hydrogen-induced effects, such as embrittlement of aluminides and blistering of alloys and anodic alumina films. A formalized, top-down, logic-tree structure is presented as a guide to this discussion. A theoretical basis for interfacial weakening by hydrogen is first cited, as are demonstrations of hydrogen detection as a reaction product or interfacial species. Further support is provided by critical experiments that recreate the moisture effect, but by isolating hydrogen from other potential causative factors. These experiments include tests in H 2-containing atmospheres or cathodic hydrogen charging. Accordingly, they strongly indicate that interfacial hydrogen, derived from moisture, is the key chemical species accounting for delayed alumina scale spallation.

Smialek, James L.↗

Project X: Accelerator Reference Design

Project X is a high-intensity proton facility being developed to support a world-leading program of Intensity Frontier physics over the next two decades at Fermilab. Project X is an integral part of the U.S. Intensity Frontier Roadmap as described in the P5 report of May 2008 [1] and within the Fermilab Strategic Plan of November 2011 [2]. This document represents Part I of the “Project X Book” describing the Project X accelerator facility and the broad range of physics research opportunities enabled by Project X. Parts II and III provide in-depth descriptions of the physics research program, both within and beyond particle physics [3]. The primary elements of the U.S. program to be supported by Project X include: Neutrino Experiments: Experimental studies of neutrino oscillations and neutrino interaction physics with ultra-intense neutrino beams provided by a high-power proton source with energies up to 120 GeV, utilizing near detectors at the Fermilab site and massive detectors at distant underground laboratories. Goal: At least 2 MW of proton beam power at any energy between 60 to 120 GeV; several hundred kW of proton beam power on target at 8 GeV. Kaon, Muon, Nucleon, and Neutron Precision Experiments: World-leading experiments studying ultra-rare kaon decays, searching for muon-to-electron conversion and nuclear electron dipole moments (EDMs), and exploring neutron properties at very high precision. Goal: MW-class proton beams supporting multiple experiments at 1 and 3 GeV, with flexible capability for providing distinct beam formats to concurrent users while allowing simultaneous operations with the neutrino program. Material Science and Nuclear Energy Applications: High-intensity accelerator, spallation, target and transmutation technology demonstrations will provide critical input into the design of future energy systems, including next generation fission reactors, nuclear waste transmutation systems and future thorium fuel-cycle power systems. Possible applications of muon spin rotation techniques provide sensitive probes of the magnetic structure of materials. Goal: Provide MW-class proton beams at 1 GeV, coupled with novel targets required to support a broad range of materials science and energy applications. Platform for Evolution to Future Frontier Facilities: A high-intensity proton source will strengthen and modernize the Fermilab injector complex, providing a robust platform upon which to build future frontier facilities. The Neutrino Factory and Muon Collider are examples that would provide world-leading capabilities at the Intensity and Energy Frontiers for many decades to come. Goal: Provide a straightforward upgrade path for a 4 MW, low-duty-factor source of protons at energies between 5 and 15 GeV. These four elements are expected to form the basis of the Mission Need statement required for the Department of Energy (DOE) Critical Decision 0 (CD-0), and represent the fundamental design criteria for Project X. The following chapters present the Reference Design for the Project X accelerator facility. The Reference Design is based on a continuous wave (CW) superconducting (SC) linac providing up to 1 and 3 MW of beam power at 1 and 3 GeV respectively. A pulsed linac provides acceleration of roughly 4% of the beam delivered from the CW linac to the 8 GeV injection energy of the existing Recycler/Main Injector complex. Upgrades to the Recycler and Main Injector support a factor of three increase, beyond current capabilities, in proton beam power at 60 to 120 GeV. The Reference Design represents a facility that will be unique in the world with unmatched capabilities for the delivery of very high beam power, with flexible beam formats, to multiple users at multiple energies. The utilization of linacs within the Project X facility enables capabilities beyond what is achievable with circular accelerators. It is anticipated that the final configuration and operating parameters of the complex will be further refined through the R&D program in advance of CD-2.

Holmes, Stephen D.↗

Laser surface modification of medical grade alloys for reduced heating in a magnetic resonance imaging environment

Nanoscale surface modification of medical grade metallic alloys was conducted using a neodymium-doped yttrium aluminum garnet laser-based dopant diffusion technique. The objective of this approach was to minimize the induction heating by reducing the absorbed radio frequency field. Such an approach is advantageous in that the dopant is diffused into the alloy and is not susceptible to detachment or spallation as would an externally applied coating, and is expected to not deteriorate the mechanical and electrical properties of the base alloy or device. Experiments were conducted using a controlled environment laser system with the ability to control laser properties (i.e., laser power, spot size, and irradiation time) and dopant characteristics (i.e., temperature, concentration, and pressure). The reflective and transmissive properties of both the doped and untreated samples were measured in a radio frequency (63.86 MHz) magnetic field using a system comprising a high power signal generator, a localized magnetic field source and sensor, and a signal analyzer. The results indicate an increase in the reflectivity of the laser-treated samples compared to untreated samples. The effect of reflectivity on the heating of the alloys is investigated through a mathematical model incorporating Maxwell’s equations and heat conduction.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Benchmarking of the MCNPX predictions of the neutron time-emission spectra at LANSCE - 25332

We currently operate Mark-III generation of the spallation neutron target-moderator-reflector-shield (TMRS) assembly at the Manuel Lujan Jr. Neutron Scattering Center of the Los Alamos Neutron Science Center (LANSCE). Mark-III is scheduled for replacement with the next-generation TMRS Mark-IV in 2020. Mark-IV enhances the neutronic performance in the eV-MeV energy range by increasing intensity and improving energy resolution. The increased eV-MeV neutron flux, together with the elevated gamma-ray background, has implications for the radiation shielding of the neutron flight paths and scientific instruments. To update the shielding design, we need to maintain a thoroughly benchmarked MCNPX model of the entire TMRS assembly. In this article we use our detailed MCNPX model of Mark-III to calculate the neutron time-emission spectra. With these spectra we generate the resolution function for SAMMY calculations of capture cross section in {sup 197}Au in the resonance region between 70 eV and 1 keV. We compare the calculated data with the experimental data measured with the DANCE instrument using the neutron time-of-flight technique. We show that our current model predicts measurements accurately and thus provides a solid base for developing the radiation shielding design of the new TMRS assembly. (authors)

07 ISOTOPE AND RADIATION SOURCES↗

Explosion Source Models and the Scattering Origin of Regional Phases from SPE Phase 1 Coda Spectral Ratios

The Source Physics Experiment(SPE)explosions provide comprehensive ground truth information,and nearby recordings that are rarely available in typical monitoring scenarios. Here, we look for relationships with local and regional distance data to understand source and propagation effects in an effort to improve monitoring at a distance. We examine source spectral ratios, which can be measured to high precision by taking advantage of many SPE and independently operated stations, as well as the redundancy available from coda waves. Classical source models (Mueller and Murphy, 1971, MM71; Denny and Johnson, 1991, DJ91)predict the source ratios poorly; however, a hybrid model(MM71 with DJ91 cavity radii)performs better, and by varying cavity and elastic radii we obtain models that fit to within measurement precision. Based on this, the best prediction model for the SPE suite is the hybrid model with cavity radius decreased by 95%, and elastic radius decreased by 75%. This works best for mid-range scaled depths of burial (SPE-1, 2, 3, and 5). We do not guarantee transportability to other geologies,depth and scaled depth ranges. Finally, we observe a distinct spectral modulation at 6-9Hzthat is not predicted by classical models, and is most likely the result of interference of short period surface waves(Rg)with those produced by spallation of near surface layers.The same modulationis observed for compressional (P) and shear(S) waves at distance, indicating the origin of these waves as scattered Rg.The scattering process must be accounted for quantitatively when using distant signals to monitor treaty compliance over broad regions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Method of using deuterium-cluster foils for an intense pulsed neutron source

A method is provided for producing neutrons, comprising: providing a converter foil comprising deuterium clusters; focusing a laser on the foil with power and energy sufficient to cause deuteron ions to separate from the foil; and striking a surface of a target with the deuteron ions from the converter foil with energy sufficient to cause neutron production by a reaction selected from the group consisting of D-D fusion, D-T fusion, D-metal nuclear spallation, and p-metal. A further method is provided for assembling a plurality of target assemblies for a target injector to be used in the previously mentioned manner. A further method is provided for producing neutrons, comprising: splitting a laser beam into a first beam and a second beam; striking a first surface of a target with the first beam, and an opposite second surface of the target with the second beam with energy sufficient to cause neutron production.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

The EURISOL Multi-MW Target Unit: Neutronics, Dose Rate, Shielding and Activation Calculations

The EURISOL (The EURopean Isotope Separation On-Line Radioactive Ion Beam) project aims at designing a facility for producing high intensity radioactive ion beams, with unprecedented (two to three orders of magnitude higher) intensities, compared to the majority of the worldwide existing RIB facilities. For this purpose, a proton beam of energy 1 GeV and intensity up to 4 mA impinges on a liquid mercury target (the converter). The high neutron fluxes (in excess of 10{sup 15} n cm{sup -2} s{sup -1}) produced by spallation nuclear reactions in the converter induce fission on {sup 235}U targets surrounding the liquid mercury converter. In order to attain the intended high intensity radioactive ion beams, the appropriate configuration (geometry and materials) of the target unit components (converter, fission targets, moderators, reflectors) must be determined, to attain the highest possible fission rates in the uranium targets (in excess of 10{sup 15} fissions per second). The extremely high neutron and photon fluxes resulting from the operation of the target unit impose, for radiological protection and safety purposes, a careful assessment of the dose rates in the surrounding areas. Activation of the structural components must be studied. Thick shielding barriers must be designed. In this work, the so-called MAFF inspired target configuration, allowing a versatile operation, maintenance, remote control and storage of the fission targets is considered. The results obtained using the state-of-the-art Monte Carlo codes MCNPX and FLUKA are presented. The neutronics, dose rate, shielding and activation calculations, needed for radiological protection and safety assessment purposes are discussed.

43 PARTICLE ACCELERATORS↗

Prompt Neutron Multiplicity Measurements with Portable Detectors

Mobile detection of kilogram quantities of special nuclear materials (SNM) during maritime transportation is a challenging problem for the U.S. Department of Homeland Security. Counting neutrons emitted by the SNM and partitioning them from background neutrons of multiple origins is the most effective passive means of detecting the SNM. Unfortunately, neutron detection, counting, and partitioning in a maritime environment is complex due to the presence of spallation neutrons (commonly known as “ship effect”) and to the complicated nature of the neutron scattering in that environment. This work studied the possibilities of building a prototype neutron detector using boron- 10 (10B) as the converter in a novel form factor called “straws” that would address the above problem by examining multiplicity distributions of neutrons originating from a fissioning source. Currently, commercially manufactured fission meters (FM) are available that separate cosmic neutrons from non-cosmic neutrons and quantitatively determine the strength of a fissioning source; however, these FMs use 3He, which is becoming increasingly difficult to procure; also the size and weight of a commercial FM is not conducive to manual neutron detection operations in a maritime environment. The current project may provide a near-term solution to the crisis that has arisen from the global scarcity of 3He by offering a viable alternative to the FM. The prototype detector provides a large-area, efficient, lightweight, more granular neutron responsive detection surface (to facilitate imaging) to ease the application of the new FMs. A novel prototype fission meter is being designed at National Security Technologies, LLC, using a thin uniform coating of 10B as neutron converter (only 1 micron thick) inside a large array of thin (4 mm diameter) copper tubes. The copper tubes are only 2-mil thick, and each holds the stretched anode wire under tension and high voltage. The tubes are filled with proportional counter gas (a mixture of 90% Ar and 10% CO2). The tubes operate in proportional counter mode and attract mobile charged particles (alpha-particles) created in the nuclear interaction 10B(n, a)7Li. Several MCNPX calculations covering the substantial design parameter space of neutron multiplicity detectors have been performed and are presented. Our detector’s thermal neutron detection efficiency is compared to two Ortec commercial products, the Fission Meter and Detective-EX. Pulse height spectra originating from the charged particles created in the nuclear reaction 10B(n, a) 7Li* + 2.310 MeV (94%) – excited state (1) and 10B(n, a) 7Li + 2.792 MeV (6%) – ground state (2) are examined, and the response to incident gamma rays are demonstrated.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Validation of Monte Carlo simulation of neutron production in a spallation experiment

A renewed interest in experimental research on Accelerator-Driven Systems (ADS) has been initiated by the global attempt to produce energy from thorium as a safe(r), clean(er) and (more) proliferation-resistant alternative to the uranium-fuelled thermal nuclear reactors. The ADS research has been actively pursued at the Joint Institute for Nuclear Research (JINR), Dubna, since decades. Most recently, the emission of fast neutrons was experimentally investigated at the massive (m = 512 kg) natural uranium spallation target QUINTA. The target has been irradiated with the relativistic deuteron beams of energy from 0.5 AGeV up to 4 AGeV at the JINR Nuclotron accelerator in numerous experiments since 2011. Neutron production inside the target was studied through the gamma-ray spectrometry measurement of natural uranium activation detectors. Experimental reaction rates for (n,γ), (n,f) and (n,2n) reactions in uranium have provided valuable information about the neutron distribution over a wide range of energies up to some GeV. The experimental data were compared to the predictions of Monte Carlo simulations using the MCNPX 2.7.0 code. In conclusion, the results are presented and potential sources of partial disagreement are discussed later in this work.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Ultra-High Energy Cosmic Radiation: Current Issues and Future Prospects

We briefly review the current experimental and theoretical status of cosmic radiation above {approx}10{sup 17} eV, including secondary neutrinos and gamma-rays. We focus on questions related to chemical composition and sky distributions of these particles as well as on the location and nature of their sources.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Production of Actinium-225 via High Energy Proton Induced Spallation of Thorium-232

The science of cancer research is currently expanding its use of alpha particle emitting radioisotopes. Coupled with the discovery and proliferation of molecular species that seek out and attach to tumors, new therapy and diagnostics are being developed to enhance the treatment of cancer and other diseases. This latest technology is commonly referred to as Alpha Immunotherapy (AIT). Actinium-225/Bismuth-213 is a parent/daughter alpha-emitting radioisotope pair that is highly sought after because of the potential for treating numerous diseases and its ability to be chemically compatible with many known and widely used carrier molecules (such as monoclonal antibodies and proteins/peptides). Unfortunately, the worldwide supply of actinium-225 is limited to about 1,000mCi annually and most of that is currently spoken for, thus limiting the ability of this radioisotope pair to enter into research and subsequently clinical trials. The route proposed herein utilizes high energy protons to produce actinium-225 via spallation of a thorium-232 target. As part of previous R and D efforts carried out at Argonne National Laboratory recently in support of the proposed US FRIB facility, it was shown that a very effective production mechanism for actinium-225 is spallation of thorium-232 by high energy proton beams. The base-line simulation for the production rate of actinium-225 by this reaction mechanism is 8E12 atoms per second at 200 MeV proton beam energy with 50 g/cm2 thorium target and 100 kW beam power. An irradiation of one actinium-225 half-life (10 days) produces {approx}100 Ci of actinium-225. For a given beam current the reaction cross section increases slightly with energy to about 400 MeV and then decreases slightly for beam energies in the several GeV regime. The object of this effort is to refine the simulations at proton beam energies of 400 MeV and above up to about 8 GeV. Once completed, the simulations will be experimentally verified using 400 MeV and 8 GeV protons available at Fermi National Accelerator Laboratory. Targets will be processed at Argonne National Laboratory to separate and purify the actinium-225 that will subsequently be transferred to NorthStar laboratory facilities for product quality testing and comparison to the product quality of ORNL produced actinium-225, which is currently the industry standard. The test irradiations at FNAL will produce 1-20 mCi per day which is more than sufficient for quantitative evaluation of the proposed production process. The beneficial outcome of this effort will be a new production route for actinium-225 that does not use or require any uranium-233 materials owned by DOE or use any radium-226 as an irradiation target but can supply the medical community's needs for actinium-225 now and in the future.

07 ISOTOPE AND RADIATION SOURCES↗

Cosmogenic neutron-capture-produced nuclides in stony meteorites

The complete neutron-flux results and production rates for Cl-36, Ni-59, and Co-60 in stony meteorites of various radii and composition are presented. The relative neutron source strengths and neutron production-versus-depth profiles were determined by using calculated H-3 production rates. The absolute source strengths were normalized to that determined for the moon by Woolum et al. (1975). The energy spectrum of the source neutrons and the neutron transport calculations, which employed the ANISN computer code, were similar to those used for the moon by Lingenfelter et al. (1972). The production rates of the three radionuclides were determined as a function of depth in various spherical meteoroids from the calculated equilibrium neutron-flux distributions and from energy-dependent neutron-capture cross sections. Rates for producing these radionuclides by spallation reactions were also calculated.

Spergel, M. S.↗

New result for the neutron β -asymmetry parameter A 0 from UCNA

Background: The neutron β-decay asymmetry parameter A 0 defines the angular correlation between the spin of the neutron and the momentum of the emitted electron. Values for A 0 permit an extraction of the ratio of the weak axial-vector to vector coupling constants, λ≡g A /g V , which under assumption of the conserved vector current hypothesis (g V =1) determines g A . Precise values for g A are important as a benchmark for lattice QCD calculations and as a test of the standard model. Purpose: The UCNA experiment, carried out at the Ultracold Neutron (UCN) source at the Los Alamos Neutron Science Center, was the first measurement of any neutron β-decay angular correlation performed with UCN. This article reports the most precise result for A 0 obtained to date from the UCNA experiment, as a result of higher statistics and reduced key systematic uncertainties, including from the neutron polarization and the characterization of the electron detector response. Methods: UCN produced via the downscattering of moderated spallation neutrons in a solid deuterium crystal were polarized via transport through a 7 T polarizing magnet and a spin flipper, which permitted selection of either spin state. The UCN were then contained within a 3-m long cylindrical decay volume, situated along the central axis of a superconducting 1 T solenoidal spectrometer. With the neutron spins then oriented parallel or anti-parallel to the solenoidal field, an asymmetry in the numbers of emitted decay electrons detected in two electron detector packages located on both ends of the spectrometer permitted an extraction of A 0 . Results: The UCNA experiment reports a new 0.67% precision result for A 0 of A 0 = -0.12054(44) stat (68) syst , which yields λ=g A /g V = -1.2783(22). Combination with the previous UCNA result and accounting for correlated systematic uncertainties produces A 0 = -0.12015(34) stat (63) syst and λ=g A /g V = -1.2772(20).Conclusions: This new result for A 0 and g A /g V from the UCNA experiment has provided confirmation of the shift in values for g A /g V that has emerged in the published results from more recent experiments, which are in striking disagreement with the results from older experiments. Individual systematic corrections to the asymmetries in older experiments (published prior to 2002) were >10%, whereas those in the more recent ones (published after 2002) have been of the scale of <2%. Finally, the impact of these older results on the global average will be minimized should future measurements of A 0 reach the 0.1% level of precision with central values near the most recent results.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Moisture-Induced Alumina Scale Spallation: The Hydrogen Factor

For some time our community has been concerned with interfacial spallation of protective alumina scales, not just upon immediate cooldown, but as a time-delayed phenomenon. Moisture-induced delayed spallation (MIDS) and desktop spallation (DTS) of TBC's refer to this process. It is most apparent for relatively adherent alumina scales that have survived cool down in a dry environment, built up considerable thickness and strain energy, and have been somewhat damaged, such as by cyclic oxidation cracking. Indeed, a "sweet zone" can be defined that maximizes the observed effect as a function of all the relevant factors. Moisture has been postulated to serve as a source of interfacial hydrogen embrittlement derived from reaction with aluminum in the alloy at an exposed interface. The purpose of this monograph is to trace the close analogy of this phenomenon to other hydrogen effects, such as embrittlement of aluminides and blistering of alloys and anodic alumina films. A formalized, top-down, logic tree structure is presented as a guide to this discussion. A theoretical basis for interfacial weakening by hydrogen is first cited, as are demonstrations of hydrogen as a reaction product or detected interfacial species. Further support is provided by critical experiments that produce the same moisture effect, but by isolating hydrogen from other potential causative factors. These experiments include tests in H2-containing atmospheres or cathodic hydrogen charging.

Smialek, James L.↗

Code Release for “Unlocking Extreme Space Weather through Advanced Modeling of Legacy Vela Spacecraft” ER

The software being developed for this project has two mains aims. First, a Bayesian Model Calibration (BMC) procedure is being developed to calibrate a spallation model that simulates protons hitting a spacecraft orbiting earth to real data. The procedure will be developed for general data (there is no data release requested as part of this code release). Second, an inverse physics modeling task is being undertaken to map the number of resulting neutrons observed from this process to the expected number of protons that hit the model. This second task is of statistical interest; to publish on it, the code will need to be open source.

Murph, Alexander↗

THE B/C AND SUB-IRON/IRON COSMIC RAY RATIOS—FURTHER EVIDENCE IN FAVOR OF THE SPIRAL-ARM DIFFUSION MODEL

The boron to carbon (B/C) and sub-Fe/Fe ratios provide an important clue on cosmic ray (CR) propagation within the Galaxy. These ratios estimate the grammage that the CRs traverse as they propagate from their sources to Earth. Attempts to explain these ratios within the standard CR propagation models require ad hoc modifications and even with those these models necessitate inconsistent grammages to explain both ratios. As an alternative, physically motivated model, we have proposed that CRs originate preferably within the galactic spiral arms. CR propagation from dynamic spiral arms has important imprints on various secondary to primary ratios, such as the B/C ratio and the positron fraction. We use our spiral-arm diffusion model with the spallation network extended up to nickel to calculate the sub-Fe/Fe ratio. We show that without any additional parameters the spiral-arm model consistently explains both ratios with the same grammage, providing further evidence in favor of this model.

79 ASTRONOMY AND ASTROPHYSICS↗

Proton upsets in LSI memories in space

Two types of large scale integrated dynamic random access memory devices were tested and found to be subject to soft errors when exposed to protons incident at energies between 18 and 130 MeV. These errors are shown to differ significantly from those induced in the same devices by alphas from an Am-241 source. There is considerable variation among devices in their sensitivity to proton-induced soft errors, even among devices of the same type. For protons incident at 130 MeV, the soft error cross sections measured in these experiments varied from 10 to the -8th to 10 to the -6th sq cm/proton. For individual devices, however, the soft error cross section consistently increased with beam energy from 18-130 MeV. Analysis indicates that the soft errors induced by energetic protons result from spallation interactions between the incident protons and the nuclei of the atoms comprising the device. Because energetic protons are the most numerous of both the galactic and solar cosmic rays and form the inner radiation belt, proton-induced soft errors have potentially serious implications for many electronic systems flown in space.

Mcnulty, P. J.↗