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At least 73 records · Page 4

Fundamental gaps with approximate density functionals: The derivative discontinuity revealed from ensemble considerations

The fundamental gap is a central quantity in the electronic structure of matter. Unfortunately, the fundamental gap is not generally equal to the Kohn-Sham gap of density functional theory (DFT), even in principle. The two gaps differ precisely by the derivative discontinuity, namely, an abrupt change in slope of the exchange-correlation energy as a function of electron number, expected across an integer-electron point. Popular approximate functionals are thought to be devoid of a derivative discontinuity, strongly compromising their performance for prediction of spectroscopic properties. Here we show that, in fact, all exchange-correlation functionals possess a derivative discontinuity, which arises naturally from the application of ensemble considerations within DFT, without any empiricism. This derivative discontinuity can be expressed in closed form using only quantities obtained in the course of a standard DFT calculation of the neutral system. For small, finite systems, addition of this derivative discontinuity indeed results in a greatly improved prediction for the fundamental gap, even when based on the most simple approximate exchange-correlation density functional – the local density approximation (LDA). For solids, the same scheme is exact in principle, but when applied to LDA it results in a vanishing derivative discontinuity correction. This failure is shown to be directly related to the failure of LDA in predicting fundamental gaps from total energy differences in extended systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Fundamental limits in heat-assisted magnetic recording and methods to overcome it with exchange spring structures

The switching probability of magnetic elements for heat-assisted recording with pulsed laser heating was investigated. It was found that FePt elements with a diameter of 5 nm and a height of 10 nm show, at a field of 0.5 T, thermally written-in errors of 12%, which is significantly too large for bit-patterned magnetic recording. Thermally written-in errors can be decreased if larger-head fields are applied. However, larger fields lead to an increase in the fundamental thermal jitter. This leads to a dilemma between thermally written-in errors and fundamental thermal jitter. This dilemma can be partly relaxed by increasing the thickness of the FePt film up to 30 nm. For realistic head fields, it is found that the fundamental thermal jitter is in the same order of magnitude of the fundamental thermal jitter in conventional recording, which is about 0.5–0.8 nm. Composite structures consisting of high Curie top layer and FePt as a hard magnetic storage layer can reduce the thermally written-in errors to be smaller than 10{sup −4} if the damping constant is increased in the soft layer. Large damping may be realized by doping with rare earth elements. Similar to single FePt grains in composite structure, an increase of switching probability is sacrificed by an increase of thermal jitter. Structures utilizing first-order phase transitions breaking the thermal jitter and writability dilemma are discussed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Three-dimensional simulation of thermal harmonic lasing free electron laser with detuning of the fundamental

Detuning of the fundamental is a way to enhance harmonic generation. By this method, the wiggler is composed of two segments in such a way that the fundamental resonance of the second segment to coincide with the third harmonic of the first segment of the wiggler to generate extreme ultraviolet radiation and x-ray emission. A set of coupled, nonlinear, and first-order differential equations in three dimensions describing the evolution of the electron trajectories and the radiation field with warm beam is solved numerically by CYRUS 3D code in the steady-state for two models (1) seeded free electron laser (FEL) and (2) shot noise on the electron beam (self-amplified spontaneous emission FEL). Thermal effects in the form of longitudinal velocity spread are considered. Three-dimensional simulation describes self-consistently the longitudinal spatial dependence of radiation waists, curvatures, and amplitudes together with the evaluation of the electron beam. The evolutions of the transverse modes are investigated for the fundamental resonance and the third harmonic. Also, the effective modes of the third harmonic are studied. In this paper, we found that detuning of the fundamental with shot noise gives more optimistic result than the seeded FEL.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Voltage waveform tailoring for high aspect ratio plasma etching of SiO 2 using Ar/CF 4 /O 2 mixtures: Consequences of low fundamental frequency biases

The use of non-sinusoidal waveforms in low pressure capacitively coupled plasmas intended for microelectronics fabrication has the goal of customizing ion and electron energy and angular distributions to the wafer. One such non-sinusoidal waveform uses the sum of consecutive harmonics of a fundamental sinusoidal frequency, f 0 , having a variable phase offset between the fundamental and even harmonics. In this paper, we discuss results from a computational investigation of the relation between ion energy and DC self-bias when varying the fundamental frequency f 0 for capacitively coupled plasmas sustained in Ar/CF 4 /O 2 and how those trends translate to a high aspect ratio etching of trenches in SiO 2 . The fundamental frequency, f 0 , was varied from 1 to 10 MHz and the relative phase from 0° to 180°. Two distinct regimes were identified. Average ion energy onto the wafer is strongly correlated with the DC self-bias at high f 0 , with there being a maximum at φ = 0° and minimum at φ = 180°. In the low frequency regime, this correlation is weak. Average ion energy onto the wafer is instead dominated by dynamic transients in the applied voltage waveforms, with a maximum at φ = 180° and minimum at φ = 0°. The trends in ion energy translate to etch properties. In both, the high and low frequency regimes, higher ion energies translate to higher etch rates and generally preferable final features, though behaving differently with phase angle.

36 MATERIALS SCIENCE↗

The KLEVER survey: nitrogen abundances at z ~ 2 and probing the existence of a fundamental nitrogen relation

Here we present a comparison of the nitrogen-to-oxygen ratio (N/O) in 37 high-redshift galaxies at z ~ 2 taken from the KMOS Lensed Emission Lines and VElocity Review (KLEVER) Survey with a comparison sample of local galaxies, taken from the Sloan Digital Sky Survey (SDSS). The KLEVER sample shows only a mild enrichment in N/O of +0.1 dex when compared to local galaxies at a given gas-phase metallicity (O/H), but shows a depletion in N/O of –0.35 dex when compared at a fixed stellar mass (M * ). We find a strong anticorrelation in local galaxies between N/O and SFR in the M * –N/O plane, similar to the anticorrelation between O/H and SFR found in the mass–metallicity relation (MZR). We use this anticorrelation to construct a fundamental nitrogen relation (FNR), analogous to the fundamental metallicity relation (FMR). We find that KLEVER galaxies are consistent with both the FMR and the FNR. This suggests that the depletion of N/O in high-z galaxies when considered at a fixed M * is driven by the redshift evolution of the mass–metallicity relation in combination with a near redshift-invariant N/O–O/H relation. Furthermore, the existence of an fundamental nitrogen relation suggests that the mechanisms governing the fundamental metallicity relation must be probed by not only O/H, but also N/O, suggesting pure-pristine gas inflows are not the primary driver of the FMR, and other properties such as variations in galaxy age and star formation efficiency must be important.

79 ASTRONOMY AND ASTROPHYSICS↗

DESI peculiar velocity survey – Fundamental Plane

The Dark Energy Spectroscopic Instrument (DESI) peculiar velocity survey aims to measure the peculiar velocities of early- and late-type galaxies within the DESI footprint using both the Fundamental Plane and optical Tully–Fisher relations. Direct measurements of peculiar velocities can significantly improve constraints on the growth rate of structure, reducing uncertainty by a factor of approximately 2.5 at redshift 0.1 compared to the DESI Bright Galaxy Survey’s redshift space distortion measurements alone. We assess the quality of stellar velocity dispersion measurements from DESI spectroscopic data. These measurements, along with photometric data from the Legacy Survey, establish the Fundamental Plane relation and determine distances and peculiar velocities of early-type galaxies. During survey validation, we obtain spectra for 6698 unique early-type galaxies, up to a photometric redshift of 0.15. 64 per cent of observed galaxies (4267) have relative velocity dispersion errors below 10 per cent. This percentage increases to 75 per cent if we restrict our sample to galaxies with spectroscopic redshifts below 0.1. We use the measured central velocity dispersion, along with photometry from the DESI Legacy Imaging Surveys, to fit the Fundamental Plane parameters using a 3D Gaussian maximum likelihood algorithm that accounts for measurement uncertainties and selection cuts. In addition, we conduct zero-point calibration using the absolute distance measurements to the Coma cluster, leading to a value of the Hubble constant, H 0 = 76.05 ± 0.35 (statistical) ±0.49 (systematic Fundamental Plane) ±4.86 (statistical due to calibration) km s –1 Mpc –1 ⁠. This H 0 value is within 2σ of Planck cosmic microwave background results and within 1σ of other low-redshift distance indicator-based measurements.

cosmological parameters↗

Essay: Quantum Sensing with Atomic, Molecular, and Optical Platforms for Fundamental Physics

Atomic, molecular, and optical (AMO) physics has been at the forefront of the development of quantum science while laying the foundation for modern technology. With the growing capabilities of quantum control of many atoms for engineered many-body states and quantum entanglement, a key question emerges: what critical impact will the second quantum revolution with ubiquitous applications of entanglement bring to bear on fundamental physics? In this Essay, we argue that a compelling long-term vision for fundamental physics and novel applications is to harness the rapid development of quantum information science to define and advance the frontiers of measurement physics, with strong potential for fundamental discoveries. As quantum technologies, such as fault-tolerant quantum computing and entangled quantum sensor networks, become much more advanced than today’s realization, we wonder what doors of basic science can these tools unlock. We anticipate that some of the most intriguing and challenging problems, such as quantum aspects of gravity, fundamental symmetries, or new physics beyond the minimal standard model, will be tackled at the emerging quantum measurement frontier. . Published by the American Physical Society 2024

Physics↗

Fundamental Physics at the Intensity Frontier: Report of the Workshop held December 2011 in Rockville, MD

Particle physics aims to understand the universe around us. The Standard Model of particle physics describes the basic structure of matter and forces, to the extent we have been able to probe thus far. However, it leaves some big questions unanswered. Some are within the Standard Model itself, such as why there are so many fundamental particles and why they have different masses. In other cases, the Standard Model simply fails to explain some phenomena, such as the observed matter-antimatter asymmetry in the universe, the existence of dark matter and dark energy, and the mechanism that reconciles gravity with quantum mechanics. These gaps lead us to conclude that the universe must contain new and unexplored elements of Nature. Most of particle and nuclear physics is directed towards discovering and understanding these new laws of physics. These questions are best pursued with a variety of approaches, rather than with a single experiment or technique. Particle physics uses three basic approaches, often characterized as exploration along the cosmic, energy, and intensity frontiers. Each employs different tools and techniques, but they ultimately address the same fundamental questions. This allows a multi-pronged approach where attacking basic questions from different angles furthers knowledge and provides deeper answers, so that the whole is more than a sum of the parts. A coherent picture or underlying theoretical model can more easily emerge, to be proven correct or not. The intensity frontier explores fundamental physics with intense sources and ultra-sensitive, sometimes massive detectors. It encompasses searches for extremely rare processes and for tiny deviations from Standard Model expectations. Intensity frontier experiments use precision measurements to probe quantum effects. They typically investigate very large energy scales, even higher than the kinematic reach of high energy particle accelerators. The science addresses basic questions, such as: Are there new sources of CP violation? Is there CP violation in the leptonic sector? Are neutrinos their own antiparticles? Do the forces unify? Is there a weakly coupled hidden sector that is related to dark matter? Do new symmetries exist at very high energy scales? To identify the most compelling science opportunities in this area, the workshop Fundamental Physics at the Intensity Frontier was held in December 2011, sponsored by the Office of High Energy Physics in the US Department of Energy Office of Science. Participants investigated the most promising experiments to exploit these opportunities and described the knowledge that can be gained from such a program. The workshop generated much interest in the community, as witnessed by the large and energetic participation by a broad spectrum of scientists. This document chronicles the activities of the workshop, with contributions by more than 450 authors. The workshop organized the intensity frontier science program along six topics that formed the basis for working groups: experiments that probe (i) heavy quarks, (ii) charged leptons, (iii) neutrinos, (iv) proton decay, (v) light, weakly interacting particles, and (vi) nucleons, nuclei, and atoms. The conveners for each working group included an experimenter and a theorist working in the field and an observer from the community at large. The working groups began their efforts well in advance of the workshop, holding regular meetings and soliciting written contributions. Specific avenues of exploration were identified by each working group. Experiments that study rare strange, charm, and bottom meson decays provide a broad program of measurements that are sensitive to new interactions. Charged leptons, particularly muons and taus, provide a precise probe for new physics because the Standard Model predictions for their properties are very accurate. Research at the intensity frontier can reveal CP violation in the lepton sector, and elucidate whether neutrinos are their own antiparticles. A very weakly coupled hidden-sector that may comprise the dark matter in the universe could be discovered. The search for proton decay can probe the unification of the forces with unprecedented reach and test sacrosanct symmetries to very high scales. Detecting an electric dipole moment for the neutron, or neutral atoms, could establish a clear signal for new physics, while limits on such a measurement would place severe constraints on many new theories. This workshop marked the first instance where discussion of these diverse programs was held under one roof. As a result, it was realized that this broad effort has many connections; a large degree of synergy exists between the different areas and they address similar questions. Results from one area were found to be pertinent to experiments in another domain.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Fundamental Science with Pulsed Power: Research Opportunities and User Meeting.

The fifth Fundamental Science with Pulsed Power: Research Opportunities and User Meeting was held in Albuquerque, NM, July 20-­23, 2014. The purpose of the workshop was to bring together leading scientists in four research areas with active fundamental science research at Sandia’s Z facility: Magnetized Liner Inertial Fusion (MagLIF), Planetary Science, Astrophysics, and Material Science. The workshop was focused on discussing opportunities for high-­impact research using Sandia’s Z machine, a future 100 GPa class facility, and possible topics for growing the academic (off-Z-campus) science relevant to the Z Fundamental Science Program (ZFSP) and related projects in astrophysics, planetary science, MagLIF- relevant magnetized HED science, and materials science. The user meeting was for Z collaborative users to: a) hear about the Z accelerator facility status and plans, b) present the status of their research, and c) be provided with a venue to meet and work as groups. Following presentations by Mark Herrmann and Joel Lash on the fundamental science program on Z and the status of the Z facility where plenary sessions for the four research areas. The third day of the workshop was devoted to breakout sessions in the four research areas. The plenary-­ and breakout sessions were for the four areas organized by Dan Sinars (MagLIF), Dylan Spaulding (Planetary Science), Don Winget and Jim Bailey (Astrophysics), and Thomas Mattsson (Material Science). Concluding the workshop were an outbrief session where the leads presented a summary of the discussions in each working group to the full workshop. A summary of discussions and conclusions from each of the research areas follows and the outbrief slides are included as appendices.

99 GENERAL AND MISCELLANEOUS↗

Reactor Fundamentals Handbook

The objective of the Knowledge Transfer Workshop is to transfer selected fundamental nuclear energy technology knowledge and experience to the nuclear industry’s next generation of leaders. The course provides the original bases for fundamental safety concepts, design features, and reactor technologies. The course discusses the “why” and the “how” for decisions that led to the current commercial nuclear reactor designs and regulatory framework. Various accidents and their attributes as well as other events that have strongly affected the evolution of the safety case, plant design, and operations are discussed. To prepare the course participant for the topics discussed, this handbook provides a crash course into the current state of commercialized Light Water Reactor technology. The material is introductory for the interested layperson and also serves as a refresher for scientists and engineers that may have studied Light Water Reactors at one time, but are currently not an expert in this field of nuclear engineering. This handbook is a brief tutorial and refresher training material on basic Light Water Reactor (LWR) core physics and plant systems. It is reference material for attendees of the Knowledge Transfer Workshop. There are two types of LWR technologies, Pressurized Water Reactor (PWR) and Boiling Water Reactors (BWR). This handbook discusses fundamental design traits of each providing contrasts between performance and safety features. The intent is to provide the participants with an understanding of nuclear terminology associated with LWR technology, including fundamentals, systems, safety, and regulations. This handbook is not an original textbook. Many authors have contributed collegiate level introduction to nuclear engineering texts. Rather, this material is intended to be a graded summary of important aspects of LWR reactor core and plant systems. It draws heavily on other resources. The interested reader is encouraged to follow citations made in this handbook to more thorough or detailed public references.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

The radio/X-ray correlation and black hole fundamental plane for young radio sources: Implications for X-ray origin and accretion mode

We find that the young radio sources (gigahertz-peaked spectrum and compact steep spectrum radio sources) follow in the radio/X-ray correlation with b=0.61±0.07 (L{sub R}∝L{sub X}{sup b}), and the fundamental plane of black hole activity with the form logL{sub R}=0.58{sub −0.03}{sup +0.03}logL{sub X}+0.42{sub −0.07}{sup +0.09}logM{sub BH}+13.83{sub −0.97}{sup +0.91} and the intrinsic scatter σ=0.29. The flatter coefficient between radio and X-ray bands denies the jet origin of the X-ray emission in these types of sources. Meanwhile, the higher ratio of X-ray luminosity to Eddington luminosity (L{sub X}/L{sub Edd}) suggests that the X-ray emission is produced by the hot corona coupling with the standard thin disk. The deviation with the radiative efficient fundamental plane proposed by Dong et al. is mainly due to the extended radio emission in young radio sources. This fundamental plane manifests that even the kiloparsec-scaled radio emission has a tight connection with the accretion process, and could be suitable for the radio-loud active galactic nuclei whose radio and X-ray emission are dominated by the extended jets and the radiative efficient accretion flow, respectively. Otherwise, the high-excitation galaxies and low-excitation galaxies do not have obvious distinctions in the radio/X-ray correlation and the fundamental plane.

79 ASTRONOMY AND ASTROPHYSICS↗

The X-Ray Fundamental Plane of the Platinum Sample, the Kilonovae, and the SNe Ib/c Associated with GRBs

A large fraction of gamma-ray burst (GRB) lightcurves (LCs) show X-ray plateaus. We analyze all GRBs with known redshifts presenting plateaus observed by The Neil Gehrels Swift Observatory from its launch until 2019 August. The fundamental plane relation between the rest-frame time and X-ray luminosity at the end of the plateau emission and the peak prompt luminosity holds for all the GRB classes when selection biases and cosmological evolutions are applied. We have discovered two important findings: (1) a new class of long GRBs with good data coverage: the platinum sample; and (2) the platinum, the SNe-LGRB, and the KN-SGRB samples, yield the smallest intrinsic scatter with σ platinum , GRB-SNe = 0.22 ± 0.10 and σ KN-SGRB = 0.24 ± 0.12. The SNe-LGRBs are composed of GRBs associated spectroscopically with the SNe Ib,c, the KN-SGRBs are composed by eight GRBs associated with kilonovae or where there could have been such an association. The highest correlation coefficients are yielded for the SN-LGRB-ABC sample, which includes GRBs spectroscopically associated with SNe Ib/c or with a clear optical bump in the LC resembling the SNe Ib/c, ( ), the SN-LGRBs ( ), and the KN-SGRBs ( ) when the redshift evolution is considered. We find that these category planes are reliable candidates to use as cosmological tools. Furthermore, the distance from the gold fundamental plane is a crucial discriminant among classes. In fact, we find that the distributions of the distances of the SNe-LGRB, SNe-LGRB-ABC, KN-SGRB, and SGRB samples from the gold fundamental plane are statistically different from the distribution of the gold GRBs' distances from the gold fundamental plane with and without considering evolution cases. <

79 ASTRONOMY AND ASTROPHYSICS↗

Combustion Fundamentals Research

Increased emphasis is placed on fundamental and generic research at Lewis Research Center with less systems development efforts. This is especially true in combustion research, where the study of combustion fundamentals has grown significantly in order to better address the perceived long term technical needs of the aerospace industry. The main thrusts for this combustion fundamentals program area are as follows: analytical models of combustion processes, model verification experiments, fundamental combustion experiments, and advanced numeric techniques.

Source record↗

The Location of the CO2, Fundamental in Clathrate Hydrates and its Application to Infrared Spectra of Icy Solar System Objects

CO2 is present on the surface of many Solar System objects, but not always as a segregated, pure ice. In pure CO2-ice, the fundamental absorption is located near 4.268 micron (2343.3 wavenumbers). However, on several objects, the CO2 fundamental is shifted to higher frequency. This shift may be produced by CO2 gas trapped in another material, or adsorbed onto minerals. We have seen that a mixture of H2O, CH3OH4 and CO2 forms a type II clathrate when heated to 125 K and produces a CO2 fundamental near 4.26 micron. The exact location of the feature is strongly dependent on the initial ratio of the three components. We are currently exploring various starting ratios relevant to the Solar System to determine the minimum amount of CH3OH needed to convert all of the CO2 to the clathrate, i.e. eliminate the splitting of the CO2 fundamental. We are testing the stability of the clathrate to thermal processing and UV photolysis, and documenting the changes seen in the spectra in the wavelength range from 1-5 micron. We acknowledge financial support from the Origins of Solar Systems Program, the Planetary Geology and Geophysics and the NASA Postdoctoral Program.

Sandford, S. A.↗

System and method for optimizing fundamental frequency modulation for a cascaded multilevel inverter

A system and a method for optimizing fundamental frequency modulation in a cascaded multilevel inverter (CMI) are provided. The CMI includes at least a first H-bridge module and a second H-bridge module connected in series with the first H-bridge module. The first H-bridge module is operated according to a first duty cycle and the second H-bridge module is operated according to a second duty cycle. The first duty cycle is greater than the second duty cycle. The first and second H-bridge modules are controlled utilizing fundamental frequency modulation. A portion of the first duty cycle is transferred to the second duty cycle thereby optimizing fundamental frequency modulation by at least improving power sharing between the first and second H-bridge modules and improving equalization of DC capacitor currents and voltage ripples while maintaining the same fundamental modulation to the output voltage waveform.

42 ENGINEERING↗

A Novel Method for Determination of Equivalence Factor of External Neutron Source to Fundamental-Mode Source

External neutron sources, such as {sup 252}Cf source, D-T source, D-D source or Am-Be source, are often used in the startup and operation of reactors and in some physics experiments like pulsed neutron method in accelerator-driven- subcritical systems (ADS). Due to the difference of spectra and space distributions between various sources, some crucial characteristics of the reactor are significantly different. In the research of neutron initiation probability, the pulse initial time is strongly dependent on the neutron importance of external source neutrons. It is necessary to find a standard measure to evaluate the effect of different sources. G. D. Spriggs proposed the concept of equivalent fundamental-mode source and established the equivalent relationship of any sources to the fundamental- mode source of the reactor with the converter factor g*, which was the ratio of neutron multiplication of the external source to that of the fundamental source. The method by G. D. Spriggs considered the effect of delayed neutrons. In this paper, a new method based on analysis of prompt neutron time distribution is presented and a new parameter is defined, which differs from g* in that delayed neutrons are not considered. The method to determine the equivalence factor of external source neutrons to the reactor fundamental mode source neutrons based on the time distribution of prompt neutron time distribution was presented. Currently the method has been realized in calculation and next we will implement the methodology in experiments after the absolute efficiencies of the neutron detectors are calibrated. (authors)

07 ISOTOPE AND RADIATION SOURCES↗

Equivalent Fundamental-Mode Source Simulations for Spherical Uranium and Plutonium Systems [Abstract]

The equivalent fundamental-mode source refers to a “source” which is identically distributed in space, energy, and angle as that of a fundamental-mode fission source distribution. It has previously been shown that the system fixed source multiplication ($M_{fs}$) relates to the effective multiplication factor ($\kappa_{eff}$) as $M_{fs} = \frac{g^*}{1-k_{eff}}$ The term $\mathcal{g}$* therefore relates the system source distribution to the system equivalent fundamental-mode source. As previously shown, the $\mathcal{g}$* term is approximately 1 for deeply subcritical systems and then diverges as the system multiplication increases. For a system with a point source located in the center of an assembly (such a sphere), $\mathcal{g}$* will be greater than 1; this happens because there is a higher probability of induced fission when all of the starter neutrons originate from the center of the sphere. For a uniform source, $\mathcal{g}$* is less than 1, but does not diverge from 1 as dramatically as seen by a point source. One reason that $\mathcal{g}$* is an important parameter is that it is used in measurement methods to infer reactor kinetics parameters ($β_{eff}$ being one example). This work will discuss multiple ways to simulate $\mathcal{g}$* using MCNP®6.2, which include use of traditional methods versus a single input file method that was recently published. A discussion related to methods to simulate $M_{fs}$ will be presented. Spherical systems of Highly Enriched Uranium (HEU) will be compared with previous works. In addition, results of plutonium including multiple reflector materials will be investigated. Simulated systems will include both parametric studies as well as configurations used in recent experiments performed at the National Criticality Experiments Research Center (NCERC). These studies will include subtleties associated with system geometry that have not been previously shown. Last, this work will investigate the relationship between $\mathcal{g}$* and reactor kinetics parameters (such as $β_{eff}$).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Preliminary Compendium of the Initial Conditions and Evolution of the Fundamental Interactions of SiC with Ag and Pd

Tri-structural isotropic (TRISO) particles are the fuel of choice for very-high temperature reactors. At the core, these spherical particles consist of an inner fuel kernel of UO{sub 2}, UC{sub 2} or a combination of both, which is coated radially outward by successive layers of low density pyrolytic graphite, an inner high density pyrolytic graphite layer, silicon carbide (SiC) and an outer high density pyrolytic graphite layer. SiC is the main diffusion barrier against the release of fission products due to its hardness and high melting point. Irradiation testing of TRISO particles indicates that trace amounts of metallic fission products can damage or potentially escape through the barrier layer. Surrogate experimental studies have previously been performed by various methods seeking to shed light on and explain the diffusion behavior of Ag and Pd. Although some of these experiments have yielded realistic diffusion coefficients the discrepancy of results between different groups is such that the essential details of the diffusive behavior are still to be fully understood. This work aims to understand the fundamental physical and chemical interactions that take place at the interface of SiC and Ag/Pd, and which give rise to the observed diffusion behavior of these metallic species in TRISO particles. Theoretical simulations of the diffusion of Ag through SiC have been exhaustive but typically yield bulk diffusion coefficients that due to the nature of bulk diffusion phenomena (i.e. slow diffusion) the diffusion coefficients are calculated to be orders of magnitude lower than what experimental observations suggest. This in part is due to the difficulty in simulating realistic models that include various polymorphs of SiC, and the dynamical structural transformations that SiC undergoes in the TRISO environment (which are also to be explained). The result is a particularly challenging problem to solve given that the initial conditions of the interactions of Ag and Pd with SiC are difficult to address, both in theoretical models and surrogate experiments. In order to improve these models the approach taken here is to consider fundamental interactions between Ag and SiC that take place in short time scales by varying the initial environmental conditions, i.e. annealing temperature and time, initial amounts of the metallic species (M) Ag, Pd in SiC/M/SiC multilayers. This work aims to understand the fundamental physical and chemical interactions that take place at the interface of SiC and Ag/Pd, and which give rise to the observed diffusion behavior of these metallic species in TRISO particles. In order to do so we have synthesized SiC/Ag/SiC and SiC/Pd/SiC multilayers of various thicknesses by PLD and characterized them using SEM/EDS. Initial results show that upon annealing Ag agglomerates and ruptures the SiC layer to be released. In the case of Pd a strong chemical interaction is deduced from the slow interlayer diffusion and limited release. Further studies using photoelectron spectroscopy and RHEED will be carried out in order obtain detailed information on the chemical and physical transitions that undergo upon annealing of these systems. (authors)

36 MATERIALS SCIENCE↗