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At least 163 records · Page 9

A Possible Radiation-Induced Transition from Monazite-(Ce) to Xenotime-(Y)

This study examines two pegmatitic monazite samples (2a and 4b, these numbers are related to a previous study) to determine their crystal chemistry and effects of internal radiation damage using synchrotron high-resolution powder X-ray diffraction and electron-probe micro-analysis. Both the huttonite and cheralite substitutions are discussed. Rietveld structure refinement of sample 2a shows three different phases [2a = monazite-(Ce), 2b = monazite-(Ce), and 2c = xenotime-(Y)] with distinct structural parameters. The changes among the unit-cell parameters between the two monazite-(Ce) phases is more pronounced in the a followed by the b and c unit-cell parameters. Sample 4a is a single-phase monazite-(Sm) that contains 0.164 apfu Th. Phase 2c with space group I41/amd arises from redistribution of La, Ce, Pr, Nd, Sm, Gd, Dy, Si, and Y atoms from those in monazite (space group P21/n). A possible cause for the phase transition from monazite-(Ce) to xenotime-(Y) is α-radiation events over a long geological time. However, other chemical processes cannot be ruled out as a cause for the transition.

structural variations↗

Increasing the Stability of Deep Blue Phosphor‐Sensitized OLEDs Using the Polariton‐Enhanced Purcell Effect

Abstract The stability of efficient, deep blue organic light‐emitting diodes (OLEDs) remains a major challenge in the field of organic electronics. Poor device stability originates from the high probability for destructive non‐radiative triplet exciton annihilation events. Phosphor‐sensitized fluorescence (PSF) is proposed to achieve an efficient, deep blue color by energy transfer from phosphors to fluorophores. Recently, the polariton‐enhanced Purcell (PEP) effect is introduced to decrease the triplet radiative lifetime and density, resulting in an increase in blue phosphorescent OLED lifetime. Here, the PEP effect is introduced to enhance the stability of the PSF‐OLEDs. It is shown that the PEP effect increases all radiative decay rates of the phosphors and fluorophores, leading to a reduction in the triplet annihilation events. Using a Pt‐complex phosphor sensitizer and a so‐called multi‐resonance fluorescent emitter in a PEP cavity, a 3.1‐fold lifetime increase is observed at a current density ofJ= 10 mA cm −2 , reduced EQE roll‐off and deep blue color with Commission Internationale de l'Eclairage coordinates of (0.13, 0.09). The PEP effect maximally extends PSF‐OLED lifetimes in devices with the highest triplet‐to‐singlet energy transfer rates. Moreover, this work suggests that the benefits of PEPs apply to all triplet‐based OLEDs.

Chemistry↗

Photoinitiated Reactions of Molecules and Radicals in Molecular Beams

The UV photochemistry of organic molecules is a fundamental process that governs reactions in the atmosphere, synthetic chemistry, processing of organic aerosols, and biological damage in living tissues. In many organic molecules, the ensuing evolution involves pathways that are in competition, giving rise to different products, isomerization, coupling to other electronic states, and secondary reactive collisions. Because photodissociation is usually fast (picoseconds to microseconds), these processes are far from equilibrium and are controlled by kinetic competition and dynamical forces. The work accomplished was focused primarily on the photochemistry of alpha-keto carboxylic acids, a group of acids produced from natural sources, which are implicated in aerosol formation and biological processes. In the atmosphere, they are destroyed mainly by solar radiation. Studying their photochemistry has been surprisingly difficult because of the complexity of their excited electronic states, and the effect of collisions and secondary reactions. The second project investigated the lifetime of excited electronic states of pyrazine and picoline and had both experimental and theoretical aspects. The work focused on a model molecule, pyruvic acid (PA), because it was hypothesized that it should be a good source of the unstable carbene, methylhydroxycarbene (MHC). PA has an internal hydrogen bond that controls the evolution of its decomposition. The decomposition was studied following excitation to two of its lowest excited states reached by laser irradiation at 351 and 193 nm. The photodissociation dynamics in the absence and presence of collisions was monitored and compared. Understanding the UV photochemistry requires the use of complementary experimental approaches. Two methods were enlisted, which together generated a comprehensive and detailed set of results: (i) The time-sliced velocity map imaging (SVMI) instrument at USC was exploited to determine kinetic energy release of fragments, fast dissociation timescales, and internal state distributions of fragments for which Resonance Enhanced Multiphoton Ionization (REMPI) schemes exist; and (ii) The multiplexed photoionization mass spectrometer (MPIMS) setup developed at the Sandia Combustion Research Facility was used for product discovery, achieved by exploiting tunable narrowband VUV radiation at the Advanced Light Source (ALS), and to follow in real time their subsequent unimolecular and bimolecular reactions. The experimental conditions ranged from collisionless molecular beams to study nascent products to flow reactors of variable pressures to study subsequent bimolecular reactions of the products. The goals stated above were successfully accomplished. By exciting PA to its lowest excited state, MHC was identified as the only primary product and its isomerization to vinylalcohol and acetaldehyde was directly observed in real time. Moreover, we reported the first bimolecular reaction of MHC, which was with acetaldehyde, and identified its reaction product. This paves the way for the study of other reactions of this important carbene intermediate. When excitation was carried out at 193 nm, which imparted much higher energy to PA, many more products were directly observed in real time, some deriving from three-body dissociation. Quantitative branching ratios and secondary reactions of radical products were also determined and analyzed. The studies of pyrazine and picoline focused on the second excited state of these molecules and showed (via ionization studies) that their excited states were very short lived (<100 fs) because of efficient couplings to lower electronic states via vibronic coupling. Theoretical work on modeling the absorption spectrum and decay mechanisms of the excited states are in progress in collaboration with theoreticians.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Large-momentum effective theory

Since the parton model was introduced by Feynman more than 50 years ago, much has been learned about the partonic structure of the proton through a large body of high-energy experimental data and dedicated global fits. However, limited progress has been made in calculating partonic observables such as the parton distribution function (PDFs) from the fundamental theory of strong interactions, quantum chromodynamics (QCD). Recently some advocated for a formalism, large-momentum effective theory (LaMET), through which one can extract parton physics from the properties of the proton traveling at a moderate boost factor such as γ ~ 2 – 5 . The key observation behind this approach is that Lorentz symmetry allows the standard formalism of partons in terms of light-front operators to be replaced by an equivalent one with large-momentum states and time-independent operators of a universality class. With LaMET, the PDFs, generalized PDFs or generalized parton distributions, transverse-momentum-dependent PDFs, and light-front wave functions can all be extracted in principle from lattice simulations of QCD (or other nonperturbative methods) through standard effective field theory matching and running. Future lattice QCD calculations with exascale computational facilities could help one to understand the experimental data related to the hadronic structure, including those from the upcoming electron-ion colliders dedicated to exploring the partonic landscape of the proton. In this work, the progress made in the past few years in the development of the LaMET formalism and its applications is reviewed, with an emphasis on a demonstration of its effectiveness from initial lattice QCD simulations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Medium-induced photon bremsstrahlung in neutrino-nucleus, antineutrino-nucleus, and electron-nucleus scattering from multiple QED interactions

Interactions of charged leptons with nuclei and the naive tree-level kinematics of these processes are affected by radiation of photons induced by the QED nuclear medium. We evaluate cross section modifications at leading orders of the number of correlated interactions inside the nucleus, known as the opacity expansion. We derive results for soft and collinear types of the bremsstrahlung at the first three orders in opacity and generalize them to higher orders. We present the leading in opacity energy spectra of soft and collinear photons and radiative energy loss inside the nucleus for experiments with lepton kinematics in the GeV energy range. At leading power of the Glauber soft-collinear effective field theory, the soft radiation is further resummed to all orders both in opacity and in the electromagnetic coupling constant. We find that the soft and collinear medium-induced radiation is vacuumlike, and additional corrections are power suppressed. Despite the negligible modification to the induced photon spectra, the nuclear medium-induced radiation sizably affects the broadening of charged leptons in the direction orthogonal to their propagation. Published by the American Physical Society 2024

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Radiative Heat Transfer and 2D Transition Metal Dichalcogenide Materials

Here we study the radiative heat transfer power in the family of transition metal dichalcogenide monolayers in their H- and T-symmetries. For this purpose, the electronic and optical properties computed from first-principles are used in effective models to understand the emerging scaling laws for metals and semiconductors as well as specific material signatures as control knobs for radiative heat transfer. Our combined approach of analytical modeling with properties from ab initio simulations can be used for other materials families to build a materials database for radiative heat transfer.

36 MATERIALS SCIENCE↗

Effects of Proton Irradiation on the Performance of Skipper CCDs

Skipper CCDs are a mature detector technology that has been suggested for future space telescope instruments requiring sub-electron readout noise in the near-ultraviolet to the near-infrared. While modern skipper CCDs inherit from the radiation-tolerant p-channel detectors developed by LBNL, the effects of high doses of ionizing radiation on skipper CCDs (such as those expected in space) remains largely unmeasured. We report preliminary results on the performance of p-channel skipper CCDs following irradiation with 217-MeV protons at the Northwestern Medicine Proton Center. The total nonionizing energy loss (NIEL) experienced by the detectors exceeds 6 years at the Sun-Earth Lagrange Point 2 (L2). We demonstrate that the skipper amplifier continues to function as expected following this irradiation. Owing to the low readout noise of these detectors, controlled irradiation tests can be used to sensitively characterize the charge transfer inefficiency, dark current, and the density and time constants of charge traps as a function of proton fluence. We conclude with a brief outlook toward future tests of these detectors at other proton and gamma-ray facilities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Analytical Approximations for Beamstrahlung at Very High Energy Electron-Positron Colliders

Among the many effects that occur in beam-beam electron-positron collisions at TeV energies, emission of hard synchrotron radiation, or beamstrahlung, has special importance. Beamstrahlung determines the energy spectrum of the most energetic electrons, positrons, and photons and supplies the initial condition for the calculation of all other QED processes. In this paper, we show that the description of beamstrahlung simplifies in the limit of large quantum parameter $Υ$, which is realized in 10 TeV collider designs. The beamstrahlung spectra for electrons and photons are given in terms of universal functions. We supply approximations to these functions that will be useful for more general studies of the beam-beam interaction at very high energies.

Accelerator Physics (physics.acc-ph)↗

Sample Preparation and Experimental Design for In Situ Multi-Beam Transmission Electron Microscopy Irradiation Experiments

We discuss the need to understand materials exposed to overlapping extreme environments such as high temperature, radiation, or mechanical stress. When these stressors are combined there may be synergistic effects that enable unique microstructural evolution mechanisms to activate. Understanding of these mechanisms is necessary for the input and refinement of predictive models and critical for engineering of next generation materials. The basic physics and underlying mechanisms require advanced tools to be investigated. The in situ ion irradiation transmission electron microscope (I 3 TEM) is designed to explore these principles. To quantitatively probe the complex dynamic interactions in materials, careful preparation of samples and consideration of experimental design is required. Particular handling or preparation of samples can easily introduce damage or features that obfuscate the measurements. There is no one correct way to prepare a sample; however, many mistakes can be made. The most common errors and things to consider are highlighted within. The I 3 TEM has many adjustable variables and a large potential experimental space, therefore it is best to design experiments with a specific scientific question or questions in mind. Experiments have been performed on large number of sample geometries, material classes, and with many irradiation conditions. The following are a subset of examples that demonstrate unique in situ capabilities utilizing the I 3 TEM. Au nanoparticles prepared by drop casting have been used to investigate the effects of single ion strikes. Au thin films have been used in studies on the effects of multibeam irradiation on microstructure evolution. Zr films have been exposed to irradiation and mechanical tension to examine creep. Ag nanopillars were subjected to simultaneous high temperature, mechanical compression, and ion irradiation to study irradiation induced creep as well. These results impact fields including: structural materials, nuclear energy, energy storage, catalysis, and microelectronics in space environments.

47 OTHER INSTRUMENTATION↗

Flash electropolishing for TEM: Reducing FIB‐induced defects in tungsten with protocols for new materials

Focused ion beam (FIB) milling has become the dominant approach for site-specific transmission electron microscopy (TEM) specimen preparation; however, FIB damage remains a critical limitation for reliable microstructural characterisation, particularly in radiation effects studies. Tungsten is especially susceptible to FIB damage due to its high nuclear stopping power, which promotes the formation and strong diffraction contrast of FIB-induced ‘black spot’ defects that are indistinguishable from very fine irradiation-induced loops/defects resulting from low to intermediate temperature neutron irradiation. In this work, flash electropolishing is systematically evaluated as a post-FIB treatment for minimising preparation-induced artefacts for TEM analysis of tungsten-based alloys. Using a range of non-, ion-, and neutron-irradiated tungsten materials, the effectiveness of flash electropolishing has been assessed through direct comparison with conventional FIB and plasma-FIB preparation including low-energy Ga, Ar, Xe ion cleaning. The results demonstrate that flash electropolishing effectively removes FIB-damaged layers and ‘black spot’ defects, thereby enabling reliable observation of irradiation-induced dislocation structures. Key processing parameters governing flash electropolishing quality – including lamella thickness, applied voltage, polishing duration, electrolyte chemistry, and cathode geometry – have been systematically evaluated, and clear criteria were established for determining when flash electropolishing is required to ensure reliable microstructural analysis. This work also provides practical guidance for implementing flash electropolishing as an artefact-controlled specimen-preparation approach for TEM characterisation of FIB-produced specimens. The systematic protocol can be extended to other, non-tungsten materials.

TEM sample preparation↗

Radiation-Induced Plutonium Redox Chemistry

Plutonium plays a key role in global actinide research and nuclear fuel cycle technologies, and yet, our fundamental understanding of its inherent radiation-induced chemical behavior is limited. These radiation-induced processes cannot simply be switched off, as they are as fundamentally inherent to plutonium as the impact of relativistic effects on its f-electrons. In less chemically complex actinide systems, such as aqueous solutions of neptunium and americium, , radiolysis products play a significant role in the redox cycling of their oxidation states. However, plutonium's multiple, coexisting, and chemically active oxidation states, which comprise of bare ions and dioxo cations, provide additional redox pathways that complicate radiation-induced processes. Oxidation state control is critical for the manipulation of plutonium, especially in used nuclear fuel reprocessing technologies, where oxidation specific states are successfully extracted, and others rejected. Consequently, mechanistically understanding the behavior of plutonium’s multiple oxidation states in the presence of intense ionizing radiation fields is essential for predicting the behavior of this element under multiple conditions that support the development and innovation of nuclear fuel cycle technologies. Here, we present recent advances in our understanding of plutonium radiation chemistry, including the first-ever multiscale model for predicting gamma radiation-induced plutonium redox chemistry, and new chemical kinetics for the reaction of plutonium and its complexes of tributyl phosphate (TBP), N,N-di-(2-ethylhexyl)butyramide (DEHBA), and N,N-di-(2-ethylhexyl)isobutyramide (DEHiBA) with transients radiolysis products, a measured using electron pulse radiolysis.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Metal oxide impregnated conformal coatings for ionizing radiation shielding

Conformal coatings provide environmental protection for sensitive military electronics. Preliminary MCNP™ modeling of metal oxide impregnated acrylic conformal coatings indicates an effective shield for gammas below 10 keV and a reduction in neutron displacement damage to Si-based electronics across the Watt spectrum. This work provides data which can allow an optimal overall shielding worth per total weight to eventually be evaluated.

Hayes, Robert Bruce↗

Electron beam irradiated foil expansion simulated by a coupled HYDRA/MCNP6 application

Simulating the hydrodynamic evolution of a temporally pulsed electron beam with multiple metal foils requires coupling the nearly monoenergetic, relativistic electron beam to the foil target. This deposition may be effectively calculated by Monte Carlo transport. Once this energy is deposited on a computational mesh representing the foil target, highly developed radiation-hydrodynamic codes, such as HYDRA, can describe the subsequent evolution. Currently, HYDRA does not have an internal Monte Carlo electron transport capability. To partially rectify this deficiency, a PYTHON-based scheme to link MCNP6 to HYDRA has been developed for quadrilateral meshes. Results from a seven-foil tantalum target configuration are presented to demonstrate this capability.

42 ENGINEERING↗

Time-dependent collisional radiative modeling of tungsten in the magnetic sheath for erosion diagnosis

Abstract Tungsten is the material of choice for the divertors in ITER, SPARC and future fusion reactors. Accurate diagnosis of tungsten erosion and migration is important for first wall life time, slag production and core performance. The addition of a magnetic presheath requires time-dependent collisional radiative effects to be included for accurate neutral tungsten collisional radiative modeling. Gross erosion measurements could be modified by a factor of 10 due to the inclusion of time-dependent effects for ITER relevant divertor conditions. A simple sputtering model and sheath density model are developed to investigate time-dependent collisional radiative effects. Neutral tungsten spectral lines populated from different metastable levels depend on model parameters leading to potential spectroscopic diagnostics of plasma parameters. Electron temperatures inferred from spectroscopic line ratios are in agreement with Langmuir probe measurements in the Compact Toroidal Hybrid.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

14 MeV DT Neutron Test Facility at the Sandia Ion Beam Laboratory

A recently completed LDRD project has provided a new facility at Sandia for testing effects of energetic neutrons on electronic components. 14 MeV neutrons are produced with a deuterium ion beam onto a thin-film tritide target. The goal of the project was to increase the neutron fluence to levels needed for radiation effects testing and qualification. This goal was achieved through two technical advances. First, a new multi-layer target concept was developed to reduce the rate of tritium loss from the target by isotope exchange, thereby reducing tritium usage and increasing target lifetime. The second advance was the construction of a new test chamber designed to maximize neutron flux at test locations. Together, these increased the available neutron fluence by several orders of magnitude. This new capability is being used in tests for Sandia nuclear weapon programs, evaluation of commercial parts such as highly-scaled CMOS SRAM lCs, and tests of new devices under development at Sandia such as lll-V HBTs, gallium nitride high-voltage diodes, and for fundamental studies of physical mechanisms of device failure.

36 MATERIALS SCIENCE↗