Interrogating the Interplay between Hydrogen and Halogen Bonding in Graphitic Carbon Nitride Building Blocks
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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Transient hydroperoxyalkyl intermediates (•QOOH) in isopentane oxidation. II. Isomer-resolved unimolecular dynamics
Transient carbon-centered hydroperoxyalkyl intermediates (•QOOH) in isopentane oxidation are characterized by their time- and energy-resolved unimolecular dissociation dynamics to hydroxyl (OH) and cyclic ether products. Two distinct •QOOH isomers are examined with radical sites at a primary carbon of one of the methyl groups (β-Me) or a secondary carbon (β-Et) of the ethyl group. Energy-dependent unimolecular rates are obtained from the time-dependent appearance of OH products for the two isomers and compared with statistical microcanonical rates computed using RRKM theory, including heavy-atom tunneling, based on high-level theoretical calculations. A benchmark-corrected approach is utilized to compute high-accuracy stationary-point energies, most importantly, transition-state barriers, for the •QOOH_Me and •QOOH_Et isomers in isopentane oxidation, building on higher-level reference calculations for the oxidation of ethane (C 2 H 5 O 2 ) and propane (C 3 H 7 O 2 ), respectively. Here, the measured rates are compared with RRKM calculations incorporating the benchmark-corrected transition-state parameters, a vibrationally adiabatic multidimensional hindered-rotor treatment of key torsions, and quantum tunneling. Agreement between experiment and theory validates the statistical description and shows faster decay for •QOOH_Et due to its lower barrier. Both β-QOOH isomers decay almost exclusively to OH + cyclic ether products under the conditions studied.
Oxidation processes↗
Turbine airfoil gas side heat transfer
Work is currently underway to develop and characterize an analytical approach, based on boundary layer theory, for predicting the effects of leading edge (showerhead) film cooling on downstream gas side heat transfer rates. Parallel to this work, experiments are being conducted to build a relevant data base for present and future methods verification.
Turner, E. R.↗
A Theory of Growing Crystalline Nanorods
Energy harvesting and storage benefit from and depend on the design of nanomaterials such nanorods. Without design, the nanorods can take numerous configurations that correspond to local minima of energy. Focusing on the science of nanorod growth, the PI has developed a theoretical framework of nanorod growth, and designed and experimentally grown small and well-separated nanorods using physical vapor deposition. Building on the framework, this project in the next three years will focus on: (1) Identifying atomic mechanisms of step bunching and dissociation; (2) Analytically formulating the competition of monolayer and multiple-layer steps to derive closed-form expressions of monolayer and multiple-layer step populations and nanorod diameters; (3) Designing nanorods by using the scientific insights from the closed-form theory (as well as atomistic simulations); and (4) Exploring technological benefits of the scientific advancements. This research relies on the synergy of analytical formulations, atomistic simulations (density-functional-theory or DFT based ab initio, classical molecular dynamics, lattice kinetic Monte Carlo), and experiments; the prototype material is face-centered-cubic Cu. If successful, the proposed research will result in a scientific theory of nanorod growth, which in turn enables discoveries of new nanorods and subsequently innovations of energy technologies. As one example, the enabled discovery of small and well-separated metallic nanorods has subsequently led to the innovation of a technology - metallic glue in ambient. This technology has been covered in ~200 news reports in 20-30 countries during the first two months of 2016; examples of new agencies include Fortune Magazine, Popular Mechanics, Yahoo News, and Fox News.
36 MATERIALS SCIENCE↗
Nonempirical Range-Separated Hybrid Functional with Spatially Dependent Screened Exchange
Electronic structure calculations based on density functional theory (DFT) have successfully predicted numerous ground-state properties of a variety of molecules and materials. However, exchange and correlation functionals currently used in the literature, including semilocal and hybrid functionals, are often inaccurate to describe the electronic properties of heterogeneous solids, especially systems composed of building blocks with large dielectric mismatch. Here, in this study, we present a dielectric-dependent range-separated hybrid functional, screened-exchange range-separated hybrid (SE-RSH), for the investigation of heterogeneous materials. We define a spatially dependent fraction of exact exchange inspired by the static Coulomb-hole and screened-exchange (COHSEX) approximation used in many-body perturbation theory, and we show that the proposed functional accurately predicts the electronic structure of several nonmetallic interfaces, three- and two-dimensional, pristine, and defective solids and nanoparticles.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Sensor and Actuator Attacks on Hierarchical Control Systems with Domain-Aware Operator Theory
Cyber-Physical Systems (CPSs) provide opportunities for cyber attacks to have physical impacts. Advanced Persistent Threats (APTs) are a subclass of cyber threats that act stealthily to avoid detection and enable long-term attacks. Here, we build on our past work in APT modelling to combine deception-based sensor bias attacks and direct actuator manipulations in attacks against a hierarchical control system. That past work used the Koopman operator to develop a data-driven, domain-aware, optimization-based attacker model. Using an expansion of this model, we compute several different attacks, including multiple simultaneous attacks, against a high-fidelity commercial building emulator and compare the impacts of those attacks to each other. One next step of interest is to construct a defender system, built on the same modelling approach, designed to detect and mitigate such attacks.
koopman operator, Cyber-Physical Security, machine↗
The spectrum of random magnetic fields in the mean field dynamo theory of the Galactic magnetic field
The fluctuation spectrum that must arise in a mean field dynamo generation of galactic fields if the initial field is weak is considered. A kinetic equation for its evolution is derived and solved. The spectrum evolves by transfer of energy from one magnetic mode to another by interaction with turbulent velocity modes. This kinetic equation is valid in the limit that the rate of evolution of the magnetic modes is slower than the reciprocal decorrelation time of the turbulent modes. This turns out to be the case by a factor greater than 3. Most of the fluctuation energy concentrates on small scales, shorter than the hydrodynamic turbulent scales. The fluctuation energy builds up to equipartition with the turbulent energy in times that are short compared to the e-folding time of the mean field. The turbulence becomes strongly modified before the dynamo amplification starts. Thus, the kinematic assumption of the mean dynamo theory is invalid. Thus, the galactic field must have a primordial origin, although it may subsequently be modified by dynamo action.
Kulsrud, Russell M.↗
Fission with Exotic Nuclei (Abbreviated Report)
Nuclear fission is a key mechanism involved in the synthesis of heavy elements in the Cosmos and is the primary explanation for the stability of superheavy elements. Nevertheless, our knowledge of fission remains extremely fragmented. Most experiments have been conducted only on a tiny number of stable actinide nuclei and are often incomplete, leading to gaps in our basic understanding of the process. For many radioactive isotopes, basic fission data such as the charge or mass distribution of the fragments is unknown. These gaps cannot always be filled by simulation alone. Common fission models contain too many free parameters and lack predictive power. In contrast, the fundamental theory of fission under development at LLNL is much more predictive, but its current computational cost is too high to be used extensively for data evaluations. A unique window of opportunity to resolve these limitations has recently opened: the U.S. nuclear science community is ramping up major experimental programs at the Facility for Rare Isotope Beams (FRIB, the DOE flagship facility in low-energy nuclear science), and techniques from machine learning have shown great potential to simplify the use of a fundamental, quantum-mechanical theory of fission. This project has two components. On the experimental side, we acquired and deployed at the HIGS facility a new dual Frisch-Grid ionization chamber to measure correlated fragment-mass, kinetic energy, and angular distributions of fission fragments from induced fission. This new device was used to perform measurements of charge, mass and total kinetic energy of fission fragments in the photofission of 238 U and eight gamma-ray beam energies between 6.2 and 13 MeV, which allowed extracting high-precision independent yields for this reaction. The device was also used to perform measurements of the same quantities in the neutron-induced fission of 234 U with monoenergetic beams of energy between 5 and 8 MeV. In parallel, we collaborated with a team at Commissariat à l’énergie atomique et aux énergies alternatives (CEA) to perform a series of measurements of fission yields in inverse kinematics for the two isotopes of 236 U and 240 Pu. The experiment took place at the Grand Accélérateur National d’Ions Lourds in France in June 2023. The deployment of the VAMOS spectrometer with a new array called PISTA allowed determining the excitation energy of the fissioning system within 1 Mega-electronvolts. The second component of the project involved using deep neural networks to build fast and reliable emulators of our current fission models. In an invited paper published in Frontier in Physics, we showed that autoencoders could successfully compress nuclear wavefunctions in nuclear density functional theory. We achieved a dimensionality reduction of the order of two orders of magnitude while keeping the error in the total energy to less than 0.01%. In a second paper submitted to Physical Review Letters in June 2023 with our collaborators at CEA, we showed that variational autoencoders can learn the collective degrees of freedom driving the fission process.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Predictive Design of Hybrid Improper Ferroelectric Double Perovskite Oxides
The computational design of suitable multiferroic double perovskite oxides requires finding materials that exhibit sizable polarization, magnetization, and coupling between them. Oxides with the chemical formula of AA'BB'O 6 with building blocks of ABO 3 single perovskite oxides in centrosymmetric Pnma symmetry are strong candidates that have been reported to satisfy such criteria. The system lowers to noncentrosymmetric, polar P2 1 symmetry if A/A' layered and B/B' rocksalt cation orderings are imposed. A detailed compositional search over a variety of chemical spaces followed by evaluating their polarization may lead to the identification of more of these compounds with ferroelectric ordering. The standard density functional theory practices to estimate polarization within the Berry phase formalism require the systems to be perfectly insulating. The number of compounds that can be evaluated using this method is therefore limited. In this work, we introduce a predictive learning strategy based on importance sampling to build a series of machine learning models using results from first-principles simulations to predict polarization and the corresponding switching barrier. The geometry-driven features related to charge states and cationic radii play key roles in predicting the switching barrier with complementary contributions from the key structural mode-based order parameters. These modes become important to draw reasonable predictions of polarization components from machine learning models. In conclusion, our predictive models identify candidates with high polarizations and low switching barriers from a pool of double perovskite oxides, suitable for future investigation for their potential applications in spintronic devices.
36 MATERIALS SCIENCE↗
Resolving the ($\mathscr{g}$-2)$_μ$ discrepancy with $\mathcal{F}$–SU(5) intersecting D-branes
A discrepancy between the measured anomalous magnetic moment of the muon (g - 2) μ and computed Standard Model value now stands at a combined 4.2σ following experiments at Brookhaven National Lab (BNL) and the Fermi National Accelerator Laboratory (FNAL). A solution to the disagreement is uncovered in flipped SU(5) with additional TeV-Scale vector-like 10 +$\bar{10}$ multiplets and charged singlet derived from local F-Theory, collectively referred to as $\mathcal {F}$-SU(5). Here we engage general No-Scale supersymmetry (SUSY) breaking in $\mathcal {F}$-SU(5) D-brane model building to alleviate the (g-2)μ. tension between the Standard Model and observations. A robust Δa μ (SUSY) is realized via mixing of M 5 and M 1X at the secondary SU(5) x U(1) X unification scale in $\mathcal {F}$-SU(5) emanating from SU(5) breaking and U(1) X flux effects. Calculations unveil Δa μ (SUSY) = 19.0-22.3 x 10 -10 for gluino masses of M($\tilde{g}$ = 2.25-2.56 TeV nd higgsino dark matter, aptly residing within the BNL+FNAL 1σ mean. This (g – 2)μ favorable region of the model space also generates the correct light Higgs boson mass and branching ratios of companion rare decay processes, and is further consistent with all LHC Run 2 constraints. Finally, we also examine the heavy SUSY Higgs boson in light of recent LHC searches for an extended Higgs sector.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Mean-Field Ring Polymer Rates Using a Population Dividing Surface
Mean-field Ring Polymer Molecular Dynamics (MF-RPMD) offers a computationally efficient method for the simulation of reaction rates in multi-level systems. Previous work has established that, to model a nonadiabatic state-to-state reaction accurately, the dividing surface must be chosen to explicitly sample kinked ring polymer configurations where at least one bead is in a different electronic state than the others. Building on this, we introduce a population difference coordinate and a kink-constrained dividing surface, and we test the accuracy of the resulting mean-field rate theory on a series of bilinear coupling model systems. Here, we demonstrate that this new MF-RPMD rate approach is efficient to implement and quantitatively accurate for models over a wide range of driving forces, coupling strengths, and temperatures.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Terahertz Dirac Hyperbolic Metamaterial
Hyperbolic metamaterials (HMMs) are engineered materials with a hyperbolic isofrequency surface, enabling a range of interesting phenomena and applications including negative refraction, enhanced sensing, and subdiffraction imaging, focusing, and waveguiding. Existing HMMs primarily work in the visible and infrared spectral range due to the inherent properties of their constituent materials. Here, we demonstrate a THz-range Dirac HMM using topological insulators as the building blocks. Here, we find that the structure houses up to three high-wavevector volume plasmon polariton (VPP) modes, consistent with transfer matrix modeling and effective medium theory calculations. The VPPs have mode indices greater than 100, significantly larger than observed for VPP modes in HMMs made from metals or doped semiconductors while maintaining comparable quality factors. We attribute these properties to the two-dimensional Dirac nature of the electrons occupying the topological insulator surface states. Because these are van der Waals materials, these structures can be grown at a wafer-scale on a variety of substrates, allowing them to be integrated with existing THz structures and enabling next-generation THz optical devices.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Superstructural phase transitions in polymer-grafted nanooctahedra
Superlattices of polyhedral nanocrystals exhibit emergent properties defined by their structural arrangements, but native nanocrystal ligands often limit their programmability. Polymeric ligands address this limitation by enabling tunable nanocrystal softness through modifications of polymer molecular weight and grafting density. Here, we investigate phase transitions in polymer-grafted nanooctahedra by varying polymer length, nanocrystal size, truncation, and ligand density. In two-dimensional superlattices, longer polymers or smaller nanooctahedra induce a transition from orientationally ordered to hexagonal rotator lattices. In three-dimensional superlattices, increasing polymer length drives transitions from Minkowski to body-centered cubic and plastic hexagonal close-packed phases, while higher grafting densities further enable transitions to simple hexagonal phases. Polymer brush and thermodynamic perturbation theories, supported by Monte Carlo simulations, uncover the entropic and enthalpic forces that govern these transitions. This work highlights the versatility of polymer-grafted anisotropic nanocrystals as building blocks for designing hierarchical superstructures and metamaterials with customizable properties.
36 MATERIALS SCIENCE↗
Materials in Extremes [Slides]
Goals: Realization of advanced predictive models that capture aspects of processing structure-properties-performance (PSPP) in ways that build on scale bridging, data science, and transformational physics insights from experiments; Based on a robust and seamless integration of sample manufacturing, characterization (pre- and post-mortem), theory and simulation, and novel experiments; Ultimately we want to be able to reliably predict performance, and control the functionality of materials in extreme environments.
36 MATERIALS SCIENCE↗
One-Turn Delay Feedback (OTFB) Implementation for the EIC
This paper discusses the implementation of the One-Turn Delay Feedback (OTFB) for the Electron-Ion Collider (EIC). The theory of the OTFB is well documented, therefore, this paper will mainly discuss the details of the implementation. After a short introduction, the paper will discuss the building-blocks of the OTFB, simulation testing of the OTFB, and finally hardware validation of the OTFB.
43 PARTICLE ACCELERATORS↗
On the tesseral-harmonics resonance problem in artificial-satellite theory
The longitude-dependent part of the geopotential usually gives rise only to short-period effects in the motion of an artificial satellite. However, when the motion of the satellite is commensurable with that of the earth, the path of the satellite repeats itself relative to the earth and perturbations build up at each passage of the satellite in the same spot, so that there can be important long-period effects. In order to take these effects into account in deriving a theoretical solution to the equations of motion of an artificial satellite, it is necessary to select terms in the longitude-dependent part of the geopotential that will contribute significantly to the perturbations. Attempts made to obtain a selection that is valid in a general case, regardless of the initial eccentricity of the orbit and of the order of the resonance, are reported. The solution to the equations of motion of an artificial satellite, in a geopotential thus determined, is then derived by using Hori's method by Lie series, which, by its properties regarding canonical invariance, has proved advantageous in the classical theory.
Romanowicz, B. A.↗
Fuzzy sets predict flexural strength and density of silicon nitride ceramics
In this work, we utilize fuzzy sets theory to evaluate and make predictions of flexural strength and density of NASA 6Y silicon nitride ceramic. Processing variables of milling time, sintering time, and sintering nitrogen pressure are used as an input to the fuzzy system. Flexural strength and density are the output parameters of the system. Data from 273 Si3N4 modulus of rupture bars tested at room temperature and 135 bars tested at 1370 C are used in this study. Generalized mean operator and Hamming distance are utilized to build the fuzzy predictive model. The maximum test error for density does not exceed 3.3 percent, and for flexural strength 7.1 percent, as compared with the errors of 1.72 percent and 11.34 percent obtained by using neural networks, respectively. These results demonstrate that fuzzy sets theory can be incorporated into the process of designing materials, such as ceramics, especially for assessing more complex relationships between the processing variables and parameters, like strength, which are governed by randomness of manufacturing processes.
Cios, Krzysztof J.↗
Factorization at subleading power and endpoint divergences in h → γγ decay. Part II. Renormalization and scale evolution
Building on the recent derivation of a bare factorization theorem for the b-quark induced contribution to the h → γγ decay amplitude based on soft-collinear effective theory, we derive the first renormalized factorization theorem for a process described at subleading power in scale ratios, where λ = m b /M h « 1 in our case. We prove two refactorization conditions for a matching coefficient and an operator matrix element in the endpoint region, where they exhibit singularities giving rise to divergent convolution integrals. The refactorization conditions ensure that the dependence of the decay amplitude on the rapidity regulator, which regularizes the endpoint singularities, cancels out to all orders of perturbation theory. We establish the renormalized form of the factorization formula, proving that extra contributions arising from the fact that “endpoint regularization” does not commute with renormalization can be absorbed, to all orders, by a redefinition of one of the matching coefficients. We derive the renormalization-group evolution equation satisfied by all quantities in the factorization formula and use them to predict the large logarithms of order $αα^2_sL^k$ in the three-loop decay amplitude, where $L=ln(-M^2_h/m^2_b)$ and k = 6, 5, 4, 3. We find perfect agreement with existing numerical results for the amplitude and analytical results for the three-loop contributions involving a massless quark loop. On the other hand, we disagree with the results of previous attempts to predict the series of subleading logarithms $~αα^n_sL^{2n+1}$
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗