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At least 685 records · Page 38

Modeling Ionizing Radiation for Spaceflight Dynamic Radioisotope Power Systems

This paper presents methods, simulations, and analyses for spaceflight ionizing radiation exposures to three dynamic radioisotope power systems(DRPSs). The specific systems being investigated are part of an open solicitation by the National Aeronautics and Space Administration (NASA) and the US Department of Energy (DOE)to develop DRPS convertor technologies. The analyses include ionizing radiation sources from PuO2andgalactic cosmic rays (GCRs) over notional 20-year mission architectures with optional 10-year exposures from Jovian radiation environments. Total integrated doses to various components are calculated and compared to known material degradation thresholds in the open literature. Based on the findings, certain material trades are recommended for Jovian and non-Jovian mission architectures based solely on ionizing radiation. However, consideration is given to known and unknown synergistic degradation effects(i.e., radiation in combination with heat, pressure, or outgassing)that may be relevant to these systems and are not captured in these analyses.

Models↗

Muon Tracking Studies in a Skew Parametric Resonance Ionization Cooling Channel

Skew Parametric-resonance Ionization Cooling (SPIC) is an extension of the Parametric-resonance Ionization Cooling (PIC) framework that has previously been explored as the final 6D cooling stage of a high-luminosity muon collider. The addition of skew quadrupoles to the PIC magnetic focusing channel induces coupled dynamic behavior of the beam that is radially periodic. The periodicity of the radial motion allows for the avoidance of unwanted resonances in the horizontal and vertical transverse planes, while still providing periodic locations at which ionization cooling components can be implemented. A first practical implementation of the magnetic field components required in the SPIC channel is modeled in MADX. Dynamic features of the coupled correlated optics with and without induced parametric resonance are presented and discussed.

43 PARTICLE ACCELERATORS↗

Skew-Quad Parametric-Resonance Ionization Cooling: Theory and Modeling

Muon beam ionization cooling is a key component for the next generation of high-luminosity muon colliders. To reach adequately high luminosity without excessively large muon intensities, it was proposed previously to combine ionization cooling with techniques using a parametric resonance (PIC). Practical implementation of PIC proposal is a subject of this report. We show that an addition of skew quadrupoles to a planar PIC channel gives enough flexibility in the design to avoid unwanted resonances, while meeting the requirements of radially-periodic beam focusing at ionization-cooling plates, large dynamic aperture and an oscillating dispersion needed for aberration corrections. Theoretical arguments are corroborated with models and a detailed numerical analysis, providing step-by-step guidance for the design of Skew-quad PIC (SPIC) beamline.

43 PARTICLE ACCELERATORS↗

The Ionization Constants of DCO{sub 3}{sup -} and DPO{sub 4}{sup 2-} under Candu Reactor Primary Coolant Conditions by Raman Spectroscopy

The ionization constants of bicarbonate and hydrogen phosphate have been measured in light and heavy water up to 325 deg. C using Raman spectroscopy. Ionization constants in heavy water at temperatures above 100 deg. C have been measured for very few acids and bases. Together with other results, this work will be used to develop and verify models of the deuterium isotope effect on oxide solubilities in Candu reactor primary coolant. A custom-built titanium/sapphire flow cell was paired with a Horiba Jobin Yvon HR800 LabRAM system to collect Raman spectra of aqueous solutions under Candu primary coolant temperatures. The temperature-controlled cell is made of materials that are relatively inert under the extreme experimental conditions required for hydrothermal studies. Raman spectra were collected with detector polarizations parallel and perpendicular to the laser polarization. These were subtracted and corrected to obtain the reduced isotropic spectrum, which contains only symmetric vibrations, has a flat baseline, and has peak areas proportional to species concentration. Vibrational modes involving deuterium are shifted to lower wavenumbers in heavy water due to the increased mass of deuterium over hydrogen. The speciation between the two solvents is also measurably different. The relative concentration of the acidic species in solution increases with temperature, making its peaks easier to fit at high temperatures. The Raman band positions shift to lower wavenumbers with increasing temperature because the hydrogen bonding in bulk water begins to break down, which strengthens hydrogen bonding to the ions. The basic equilibrium constants were determined from the concentration of each species in solution combined with an activity coefficient model. A simplified form of the 'density' model was then fitted to the data. These fit results were combined with literature values of pK{sub w} in light and heavy water to determine the pK{sub a} values at saturation vapor pressure. The experimental results show excellent agreement with known literature values in light water where they exist at lower temperatures. These equilibrium constants are the first to be reported for both chemical systems in heavy water above 25 deg. C. This work extends the equilibrium constants in H{sub 2}O: - For HCO{sub 3}{sup -} from 250 deg. C to 325 deg. C; - For HPO{sub 4}{sup 2-} from 50 deg. C to 300 deg. C. These are the first ever ionization constants in D{sub 2}O for DPO{sub 4}{sup 2-} and the first values above 25 deg. C for DCO{sub 3}{sup -}. These results will be used to develop predictive models for the deuterium isotope effect on activated corrosion product transport under Candu nuclear reactor primary coolant conditions.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

On‐Demand Ambient Ionization of Picoliter Samples Using Charge Pulses

Abstract Relay electrospray ionization (rESI) from a capillary containing a sample solution (or from an array of such capillaries) is triggered by charge deposition onto the capillary. Suitable sources of primary ions, besides electrosprays, are plasma ion and piezoelectric discharge plasma sources. With no requirement for physical contact, high‐throughput sample screening is enabled by rapidly addressing individual secondary (sample) capillaries. Sub‐pL sample volumes can be loaded and sprayed. Polar analytes, including neurotransmitters, phosphopeptides, oligonucleotides, illicit drugs, and pharmaceutical compounds are successfully ionized by rESI with concentration sensitivities (0.1 ppb for acetylcholine) which are similar to nanoESI but absolute sensitivities are orders of magnitude better. Nonpolar analytes (steroids, alkynes) are ionized by rESI using an open‐tube secondary capillary and injecting electrolytically generated metal cations from the primary electrospray.

Li, Anyin↗

On‐Demand Ambient Ionization of Picoliter Samples Using Charge Pulses

Abstract Relay electrospray ionization (rESI) from a capillary containing a sample solution (or from an array of such capillaries) is triggered by charge deposition onto the capillary. Suitable sources of primary ions, besides electrosprays, are plasma ion and piezoelectric discharge plasma sources. With no requirement for physical contact, high‐throughput sample screening is enabled by rapidly addressing individual secondary (sample) capillaries. Sub‐pL sample volumes can be loaded and sprayed. Polar analytes, including neurotransmitters, phosphopeptides, oligonucleotides, illicit drugs, and pharmaceutical compounds are successfully ionized by rESI with concentration sensitivities (0.1 ppb for acetylcholine) which are similar to nanoESI but absolute sensitivities are orders of magnitude better. Nonpolar analytes (steroids, alkynes) are ionized by rESI using an open‐tube secondary capillary and injecting electrolytically generated metal cations from the primary electrospray.

Li, Anyin↗

Analysis of Residual Explosives by Swab Touch Spray Ionization Mass Spectrometry

Swab touch spray ionization mass spectrometry, an ambient ionization technique, has been applied to the analysis of six explosives from various surfaces including glass, metal, Teflon, plastic, human hands and three types of gloves (nitrile, vinyl and latex). A swab, attached to a metallic handle, was used to sample explosive residues and acted as the ion source. The explosives, 1,3,5-trinitro-1,3,5-triazinane (RDX), 1,3,5,7-tetranitro-1,3,5,7-tetrazocane (HMX), and 2,2-bis[(nitrooxy)methyl]propane-1,3-diyl dinitrate (PETN) had an absolute limit of detection of 10 ng from all the surfaces except for PETN from the nitrile gloves (limit of detection 100 ng). Sodium perchlorate, 2-methyl-1,3,5-trinitrobenzene (TNT) and tetra-butylammonium perchlorate had limits of detection of 100 pg, 10 pg, and 1 pg, respectively from all surfaces. This study demonstrates the feasibility of swab touch spray ionization mass spectrometry for detection of a wide array of explosives from a variety of forensically applicable surfaces with disposable, commercial, tamperproof and individually-wrapped conductive swabs without complicated/lengthy sample preparations or extractions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ionizing vs collisional radiation damage in materials: Separated, competing, and synergistic effects in Ti 3 SiC 2

Comparison between intense radiation environments present in nuclear reactors and charged particle beams is necessary for evaluating next generation fission and fusion reactor materials. Yet, these two irradiation environments encompass different proportions of ionizing and collisional phenomena, so exploring the different energy loss pathways is needed for appropriate analysis. Using the candidate M n+1 AX n phase, Ti 3 SiC 2 , as a test case, this work separates the effects of electronic and nuclear energy loss during ion irradiation, through a combination of 4 MeV Au, 17 MeV Pt, and 14 MeV Cl ion irradiations to examine the effects independently and systematically recombine them. Nuclear energy loss (elastic collisions) is found to be primarily responsible for the formation of a face-centered-cubic phase with anti-site defects, while intense electronic energy loss (ionization) exacerbates the effect and increases lattice strain. Moreover, these dissipation pathways are found to be competing or synergistic depending on their ionization and collisional ratio.

36 MATERIALS SCIENCE↗

Design and Prototyping of an Ionization Profile Monitor for the SNS Accumulator Ring

An ionization profile monitor (IPM) has been designed for the Spallation Neutron Source (SNS) accumulator ring. Utilizing ionized electrons produced by beam-gas ionization, the SNS IPM uses a 120 kV bias potential to overcome beam space charge and accelerate electrons towards a movable particle detector. A 300 G magnetic field is used to confine the transverse electron motion, resulting in profile errors at the estimated 7% level. With a system bandwidth of 17.5 MHz. The SNS IPM is capable of measuring turn-by-turn beam profiles for a fully accumulated beam. This paper presents a description of the system and design.

Bartkoski, Dirk A↗

Time-resolved ionization measurements with intense ultrashort XUV and X-ray free-electron laser pulses

Abstract Modern free-electron lasers (FEL) operating in XUV (extreme ultraviolet) or X-ray range allow an access to novel research areas. One instance is the ultrafast ionization of a solid by an intense femtosecond FEL pulse in XUV which consequently leads to a change of the complex index of refraction on an ultrashort timescale. The photoionization and subsequent impact ionization resulting in electronic and atomic dynamics are modeled with our hybrid code XTANT(X-ray thermal and non-thermal transitions) and a Monte Carlo code XCASCADE(X-ray-induced electron cascades). The simulations predict the temporal kinetics of FEL-induced electron cascades and thus yield temporally and spatially resolved information on the induced changes of the optical properties. In a series of experiments at FERMI and LCLS, single shot measurements with spatio-temporal encoding of the ionization process have been performed by a correlation of the FEL pump pulse with an optical femtosecond probe pulse. An excellent agreement between the experiment and the simulation has been found. Furthermore, we demonstrate that such kind of experiments forms the basis for pulse duration and arrival time jitter monitoring as currently under development for XUV-FELs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

New Resonance Ionization Mass Spectrometry Scheme for Improved Uranium Analysis

Resonance ionization mass spectrometry (RIMS) combines tunable laser spectroscopy with mass spectrometry to provide here a high-efficiency means of analyzing solid materials. We previously showed a very high useful yield of 24% for analysis of uranium using three lasers to excite and ionize atoms sputtered from metallic uranium and uranium dioxide. A new resonance ionization scheme using only two lasers achieves a higher useful yield of 38% by accessing both the ground electronic state and a low-lying electronic state of atomic uranium that is significantly populated by sputtering. The major loss channel in analyzing uranium dioxide is the formation of UOx molecules during sputtering. Prebombardment of the surface with 3 keV noble gas ions prior to analysis reduces the surface and results in a sputtered flux with a greatly enhanced proportion of atomic U. This method of surface reduction results in uranium useful yields as high as 6.6% for uranium dioxide analysis, compared to 2% from previous work.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Effect of Ionizing Radiation on the Redox Chemistry of Penta- and Hexavalent Americium

The recent development of facile methods to oxidize trivalent americium to its higher valence states holds promise for the discovery of new chemistries and critical insight into the behavior of the 5f electrons. However, progress in understanding high valent americium chemistry has been hampered by americium’s inherent ionizing radiation field, and its concomitant effects on americium redox chemistry. Any attempt to understand high valent americium reduction and/or disproportionation must account for the effects of these radiolytic processes. Fortunately, the effects of ionizing radiation on water and aqueous nitric acid solutions are well known. Values for the yields of the major radiolytically produced reactive species that could conceivably react with americium, and their rate coefficients, are available for use in radiation chemical modeling. Therefore, we present a complete, quantitative, mechanistic description of the radiation-induced redox chemistry of the americyl oxidation states in aerated, aqueous nitric acid, as a function of radiation quality (type and energy) and solution composition using multi-scale modeling calculations supported by experiment. The reduction of Am(VI) to Am(V) was found to be most sensitive to the effects of ionizing radiation, undergoing rapid reductions with the steady-state products of aqueous HNO 3 radiolysis, i.e., HNO 2 , H 2 O 2 , and HO 2 •, which dictated its practical lifetime under acidic conditions. In contrast Am(V) is only susceptible to radiolytic oxidation, mainly through its reactions with NO 3 •, and is notably radiation resistant with respect to direct one-electron reduction to produce Am(IV). Our multiscale modeling calculations predict that the lifetime of Am(V) is dictated by its rate of disproportionation, 2AmO 2 + + 4 Haq + → AmO 2 2+ + Am 4+ + 2H 2 O, with a fourth-order dependence on [H aq + ] in agreement with previous experimental findings, giving an optimized rate coefficient of $k$ = 2.27 × 10 -6 M -5 s -1 . This disproportionation initially produces Am(IV) and Am(VI) species, but the lack of any spectroscopic evidence in our study for Am(IV) suggests that solvent reduction of this cation occurs rapidly. The ultimate product of all the Am(VI)/Am(V) irradiations is Am(III), which shows great stability in an irradiation field.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Exploring Approaches for Accelerated Mass Spectrometric Detection of Fluorochemicals from Aqueous Solutions Using Indirect, Adsorbent-Facilitated Desorption Ionization

There is a growing need for rapid, low-cost analytical tools to screen water supplies for persistent contaminants. Due to their ubiquitous presence in the environment and their detrimental effects on human health, there is a public interest in widespread testing for perfluoroalkyl substances (PFAS). However, the most common methods for PFAS analysis can be time-intensive, requiring a preconcentration step followed by liquid chromatography–mass spectrometry (LC–MS), and are cost-prohibitive for most members of the public. To address these challenges, this study explores a novel method for rapid analysis of aqueous analytes by concentrating analytes on solid adsorbents and detecting them using mass spectrometric analysis via desorption ionization directly from the adsorbent surface. We demonstrate this general approach of indirect solution analysis (ISA) with desorption electrospray ionization (ISA-DESI) and laser desorption ionization (ISA-LDI). Various adsorbent materials were screened, including commercial mesoporous carbons, alumina, and metal–organic frameworks (MOFs). Using ISA-DESI, we consistently detect concentrations as low as 5–100 parts per trillion (ppt) for perfluorooctanoic acid (PFOA) and 10–100 ppt for perfluoroundecanoic acid (PFUnDA). This approach enables rapid detection in under 5 min, making it suitable for applications requiring trace detection with fast response times. We further demonstrate the use of ISA-DESI on a range of environmentally relevant contaminants. Advantages of this indirect solution analysis approach include simplified sample preparation, accelerated analysis, and low cost with readily available materials, making it a promising tool to accelerate mass spectrometric PFAS detection for identifying contaminated sites, performing laboratory studies, and monitoring industrial waste streams.

Bays, Nathan Robert [Sandia National Laboratories ↗

Actinide Elemental Ratios of Spent Nuclear Fuel Samples by Resonance Ionization Mass Spectrometry

While resonance ionization mass spectrometry (RIMS) has demonstrated utility in measuring isotopic compositions of elements in complex matrices without the need for chemical separation to remove isobaric interferences, it has had limited application in measuring elemental compositions. The ability to determine elemental compositions via an in situ method like RIMS would be an exceptional asset in spent nuclear fuel analysis, where they are important in assessing reactor histories and whose chemical separation presents a radiological hazard. However, quantitative elemental analysis by RIMS requires special considerations because each element is ionized by its own set of lasers tuned to element specific resonant ionization wavelengths. We present the first comprehensive study of measuring elemental ratios by RIMS in spent nuclear fuel. All actinides produced by neutron capture are enhanced significantly radially from the center to the edge of a fuel pellet. This edge effect is not readily accessible by conventional bulk measurements.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Femtosecond-resolved observation of the fragmentation of buckminsterfullerene following X-ray multiphoton ionization

X-ray free-electron lasers have, over the past decade, opened up the possibility of understanding the ultrafast response of matter to intense X-ray pulses. In earlier research on atoms and small molecules, new aspects of this response were uncovered, such as rapid sequences of inner-shell photoionization and Auger ionization. Here, we studied a larger molecule, buckminsterfullerene (C 60 ), exposed to 640 eV X-rays, and examined the role of chemical effects, such as chemical bonds and charge transfer, on the fragmentation following multiple ionization of the molecule. To provide time resolution, we performed femtosecond-resolved X-ray pump/X-ray probe measurements, which were accompanied by advanced simulations. The simulations and experiment reveal that despite substantial ionization induced by the ultrashort (20 fs) X-ray pump pulse, the fragmentation of C 60 is considerably delayed. This work uncovers the persistence of the molecular structure of C 60 , which hinders fragmentation over a timescale of hundreds of femtoseconds. Furthermore, we demonstrate that a substantial fraction of the ejected fragments are neutral carbon atoms. In conclusion, these findings provide insights into X-ray free-electron laser-induced radiation damage in large molecules, including biomolecules.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Transverse emittance reduction in muon beams by ionization cooling

Accelerated muon beams have been considered for the next-generation studies of high-energy lepton–antilepton collisions and neutrino oscillations. However, high-brightness muon beams have not yet been produced. The main challenge for muon acceleration and storage stems from the large phase-space volume occupied by the beam, derived from the production mechanism of muons through the decay of pions. The phase-space volume of the muon beam can be decreased through ionization cooling. Here we show that ionization cooling leads to a reduction in the transverse emittance of muon beams that traverse lithium hydride or liquid hydrogen absorbers in the Muon Ionization Cooling Experiment. Our results represent a substantial advance towards the realization of muon-based facilities that could operate at the energy and intensity frontiers.

43 PARTICLE ACCELERATORS↗

Impact of ionizing radiation on superconducting qubit coherence

The practical viability of any qubit technology stands on long coherence times and high-fidelity operations with the superconducting qubit modality being an auspicious example, However, superconducting qubit coherence is impacted by broken Cooper pairs referred to as quasiparticles, with a density that is empirically observed to be orders of magnitude greater than the value predicted for thermal equilibrium by the Bardeen-Cooper-Schrieffer (BCS) theory of superconductivity. Previous work has shown that infrared photons significantly increase the quasiparticle density, yet even in the best isolated systems, it still remains higher than expected, suggesting that another generation mechanism exists. In this Letter, we provide evidence that ionizing radiation from environmental radioactive materials and cosmic rays contributes to this observed difference, leading to an elevated quasiparticle density that would ultimately limit superconducting qubits of the type measured here to coherence times in the millisecond regime. Additionally, we further demonstrate that introducing radiation shielding reduces the flux of ionizing radiation and positively correlates with increased coherence time. Albeit a small effect for today’s qubits, reducing or otherwise mitigating the impact of ionizing radiation will be critical for realizing fault-tolerant superconducting quantum computers.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Counting the electrons in a multiphoton ionization by elastic scattering of microwaves

Multiphoton ionization (MPI) is a fundamental first step in high-energy laser-matter interaction and is important for understanding the mechanism of plasma formation. With the discovery of MPI more than 50 years ago, there were numerous attempts to determine the basic physical constants of this process in direct experiments, namely photoionization rates and cross-sections of the MPI; however, no reliable data was available until now, and the spread in the literature values often reaches 2–3 orders of magnitude. This is due to the inability to conduct absolute measurements of plasma electron numbers generated by MPI, which leads to uncertainties and, sometimes, contradictions between MPI cross-section values utilized by different researchers across the field. Here, we report the first direct measurement of absolute plasma electron numbers generated at MPI of air, and subsequently we precisely determine the ionization rate and cross-section of eight-photon ionization of oxygen molecule by 800 nm photons σ 8 = (3.3 ± 0.3)×10 -130 W -8 m 16 s -1 . The method, based on the absolute measurement of the electron number created by MPI using elastic scattering of microwaves off the plasma volume in Rayleigh regime, establishes a general approach to directly measure and tabulate basic constants of the MPI process for various gases and photon energies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗