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At least 145 records · Page 8

Exploring the Neutron Substructure with Advanced Polarized Helium-3 Targets (Or: How I Learned to Stop Worrying and Love Spectroscopy)

As we seek to understand the smallest, physical aspects of our universe, we cannot simply rely on our senses to probe the world around us as we did in the past. The smallest physical elements of our universe behave in strange, probabilistic ways and are completely invisible to the naked eye/ear/etc. So, we design clever experiments (such as scattering experiments) to probe these minute realms. Then, just as with the larger, observable world, we devise models and equations to describe what we think is happening. Due to the nature of the physical universe at the quantum scale and with the aid of symmetries such as Lorentz invariance, we can write down equations that describe the scattering, but the expressions contain functions, which we call ?form factors? and ?structure functions?, that we cannot compute from first principles. We can, however, formulate models that make predictions for these functions. By comparing our predictions with the observed data, we can gain insight into the validity of our models and thus a better physical understanding of what is happening at these minuscule scales. Studying the constituents inside of the nucleus of an atom adds another layer of difficulty if we can?t remove those components from the nucleus. This is the case with the neutron. When not bound in the nucleus with protons and other neutrons, the neutron will decay into a proton after about 15 minutes. So, we?re forced to study the neutron while it is still bound in the nucleus of an atom such as helium-3 (3He). For the last 1,000 years (rounding up), our group has developed high quality, polarized 3He targets made of an aluminosilicate glass. These targets are made in order to perform experiments at Jefferson Lab (JLab), experiments which let us determine the form factors and structure functions of the neutron by scattering polarized electrons from polarized neutrons (or rather polarized 3He). The specific experiments reported on in this thesis push the bounds of our understanding of the internal structure of the neutron. Good science is often about pushing experimental techniques to a new level. Toward that goal we study our polarized 3He targets both to advance the technology and to choose the best ones for our experiments. We do this using a process called nuclear magnetic resonance (NMR) to gauge the maximum polarization of a target and how fast the polarization decays with time. While these tests primarily provide us information that make analysis of our experimental scattering data possible, they also let us determine whether or not a target-cell is useful or even, dare I say, of spectacular quality. Our latest targets utilize a novel convection design allowing 3He to be polarized and quickly moved in front of the electron-beam, making it possible to use larger targets with higher electron-beam currents than ever before. This means more electrons scatter and we get more data. And by studying our targets in detail prior to using them in our experiments, we have found techniques to take effects which could have been detrimental to target quality and turn them to our advantage! It?s a real case of making lemonade out of lemons. We also use laser spectroscopy to study the absorption lines of alkali-metals in the target (potassium and rubidium, specifically). We add these alkali-metals to our target to facilitate polarizing the 3He. We can use the measurement of these pressure broadened absorption lines to determine the 3He density inside of the target with great precision. Historically, we understood the width of these lines would be dependent on the temperature of the target. Specifically, if I raise the temperature, the width should get bigger. I found that was not the case, which was very confusing at first, though very exciting now that I realize the data are self-consistent and suggestive of unexpected behavior. This thesis details the development of high quality, glass, polarized 3He targets for the 2020 An 1 /dn 2 and 2023 Gn E experiments, which utilized the first 3He convection targets and broke records in target quality. This thesis also covers the initial development of metal windows for the next-generation of 3He target-cells. Finally, this thesis documents the temperature dependence of the width of potassium (K) and rubidium (Rb) absorption lines as measured with laser spectroscopy.

Jantzi, Christopher↗

Amine-Containing Membranes with Functionalized Multi-Walled Carbon Nanotubes for CO2/H2 Separation

Amine-containing mixed-matrix membranes incorporated with amino-functionalized multi-walled carbon nanotubes (AF-MWNTs) were synthesized for CO2/H2 separation based on the facilitated transport mechanism. AF-MWNTs were chosen primarily as the mechanical reinforcing filler to enhance the membrane stability. At 107 °C and 0.2-MPa feed pressure, the membrane incorporated with 10 wt.% AF-MWNTs showed a CO2 permeability of 3196 Barrers and a CO2/H2 selectivity of 205. At the higher feed pressure of 1.5 MPa, owing to the carrier saturation phenomenon, the same membrane exhibited reduced transport performance with a CO2 permeability of 776 Barrers and a CO2/H2 selectivity of 31. These separation performances at both the low and high feed pressures were well above the theoretical upper bound. Furthermore, the incorporation of 10 wt.% AF-MWNTs led to a significant improvement on membrane stability. The transport performance and selective layer thickness of this membrane maintained for 100 h, which suggested that the incorporation of AF-MWNTs improved the resistance to membrane compaction upon a high feed pressure. Therefore, this work is considered as one of the crucial steps to enable the application of facilitated transport membranes to high-pressure gas processing such as syngas purification.

59 BASIC BIOLOGICAL SCIENCES↗

Applying generalized stochastic Petri nets to manufacturing systems containing nonexponential transition functions

Generalized stochastic Petri nets (GSPNs) are applied to flexible manufacturing systems (FMSs). Throughput subnets and s-transitions are presented. Two FMS examples containing nonexponential distributions which were analyzed in previous papers by queuing theory and probability theory, respectively, are treated using GSPNs developed using throughput subnets and s-transitions. The GSPN results agree with the previous results, and developing and analyzing the GSPN models are straightforward and relatively easy compared to other methodologies.

Watson, James F., III↗

Understanding the Re-entrant Phase Transition in a Non-magnetic Scheelite

We report the stereochemical activity of lone pair electrons plays a central role in determining the structural and electronic properties of both chemically simple materials such as H 2 O, as well as more complex condensed phases such as photocatalysts or thermoelectrics. TlReO 4 is a rare example of a non-magnetic material exhibiting a re-entrant phase transition and emphanitic behavior in the long-range structure. Here, we describe the role of the Tl + 6s 2 lone pair electrons in these unusual phase transitions and illustrate its tunability by chemical doping, which has broad implications for functional materials containing lone pair bearing cations. First-principles density functional calculations clearly show the contribution of the Tl + 6s 2 in the valence band region. Local structure analysis, via neutron total scattering, revealed that changes in the long-range structure of TlReO 4 occur due to changes in the correlation length of the Tl + lone pairs. This has a significant effect on the anion interactions, with long-range ordered lone pairs creating a more densely packed structure. This resulted in a trade-off between anionic repulsions and lone pair correlations that lead to symmetry lowering upon heating in the long-range structure, whereby lattice expansion was necessary for the Tl + lone pairs to become highly correlated. Similarly, introducing lattice expansion through chemical pressure allowed long-range lone pair correlations to occur over a wider temperature range, demonstrating a method for tuning the energy landscape of lone pair containing functional materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Application of Density Functional Theory to Systems Containing Metal Atoms

The accuracy of density functional theory (DFT) for problems involving metal atoms is considered. The DFT results are compared with experiment as well as results obtained using the coupled cluster approach. The comparisons include geometries, frequencies, and bond energies. The systems considered include MO2, M(OH)+(sub n), MNO+, and MCO+(sub 2). The DFT works well for frequencies and geometries, even in cases with symmetry breaking; however, some examples have been found where the symmetry breaking is quite severe and the DFT methods do not work well. The calculation of bond energies is more difficult and examples of the successes as well as failures of DFT will be given.

Bauschlicher, Charles W., Jr.↗

Application of Density Functional Theory to Systems Containing Metal Atoms

The accuracy of density functional theory (DFT) for problems involving metal atoms is considered. The DFT results are compared with experiment as well as results obtained using the coupled cluster approach. The comparisons include geometries, frequencies, and bond energies. The systems considered include MO2, M(OH)+n, MNO+, and MCO+2. The DFT works well for frequencies and geometries, even in case with symmetry breaking; however, some examples have been found where the symmetry breaking is quite severe and the DFT methods do not work well. The calculation of bond energies is more difficult and examples of successes as well as failures of DFT will be given.

Bauschlicher, Charles W., Jr.↗

Synthesis and Surface Attachment of Molecular Re(I) Hydride Species with Silatrane Functionalized Bipyridyl Ligands

Three molecular Re hydrides of the form ( R bpy)Re(CO) 3 H with 2,2′-bipyridine (bpy) ligands containing silatrane functional groups for surface attachment on metal oxide surfaces were synthesized. IR spectroscopy and cyclic voltammetry (CV) demonstrated that the complexes containing the silatrane functional groups have electronic properties similar to those of a control compound, which did not contain functional groups for attachment. Additionally, in a similar fashion to the control compound, the silatrane containing Re hydrides are electrocatalysts for the reduction of CO 2 to CO in solution. The silatrane containing complexes were immobilized on a thin layer of TiO 2 on Si, and the resulting composites were characterized using X-ray photoelectron and IR spectroscopy as well as cyclic voltammetry in the dark and under illumination. Control experiments indicated that the hydride complexes are not stable on the surface and degrade to species which contain a bpy ligand, three CO ligands, and an unknown ligand in the sixth site. Similarly, when one of the silatrane containing Re hydride complexes was immobilized on Si nanoparticles with a thin layer of SiO 2 or silica nanoparticles, the hydride ligand was lost. Density functional theory calculations were used to corroborate the observed behavior of hydride species on a surface. Altogether, this work demonstrates the difficulties associated with attaching well-defined molecular hydride complexes to metal oxide surfaces.

Anions↗

Influence functions for the Delaware Oil and Gas Basin Tower Network

This data consists of influence functions created for the Delaware tower network for the purpose of calculating methane enhancements in the region. Two different footprint models were used. The Lagrangian Particle Dispersion model (LPDM, Uliasz 1993) was run from March 2020-May 2023. The model uses in-house WRF simulations for the meteorological transport as described in Barkley et al., (2023). Nine hundred (900) particles were released during each hourly period and are traced back 72 hours backwards in time. A static binning height of 110 m AGL was used to calculate surface influence. After May 2023, the LPDM simulations were phased out and replaced with influence functions created using HYSPLIT under the STILT configuration (Lin et al., 2003). The STILT influence functions use HRRR for the meteorological transport (Dowell et al., 2022). Nine hundred (900) particles were released during each hourly period and are traced back 72 hours backwards in time. A binning height of half the boundary layer height was used to calculate surface influence. Footprints are currently available from Sept 2020-December 2024 and will be updated periodically as more are generated in time. No STILT influence functions were created for tower site Maljimar, which was decommissioned in March 2022. Lat/Lon grid information for the LPDM influence functions is contained in lpdm-lat-lon-grid.nc. STILT grid information is contained within the influence functions themselves. Tower coordinates and heights can be found in tower-info.csv

Barkley, Z. R.↗

MIRADS-2 user's manual

An on-line data storage and retrieval system which allows the user to extract and process information from stored data bases is described. The capabilities of the system are provided by a general purpose computer program containing several functional modules. The modules contained in MIRADS are briefly described along with user terminal operation procedures and MIRADS commands.

Source record↗

GDB-9-Ex_TD-DFT-PBE0: Dataset containing Time Dependent Density Functional Theory (TDDFT) calculations for organic molecules of the GDB-9-Ex dataset.

This dataset contains data-intensive quantum chemical electronic structure calculations for 96,766 organic molecules of the GDB-9-Ex dataset. Calculations were performed using the Time Dependent Density Functional Theory (TDDFT) first principles method using the ORCA software. It provides UV-vis spectra calculations of molecules with a high level of accuracy. The optical spectra behavior was collected based on the optimized molecular geometries in the DFTB method with 3ob parameters. All calculations utilized the def2-TZVP basis sets with the auxiliary def2/J and def2-TZVP/C basis sets. The time-dependent density-functional theory (TDDFT) approach with the PBE0 exchange-correlation functional and ORCAs default integration grid was employed. For the excitation energy calculations, the lowest 50 excitation states were calculated.

AI dataset↗

A three-point form factor through five loops

We bootstrap the three-point form factor of the chiral part of the stress­tensor supermultiplet in planar $\mathcal{N}$ = 4 super-Yang-Mills theory, obtaining new results at three, four, and five loops. Our construction employs known conditions on the first, second, and final entries of the symbol, combined with new multiple-final-entry conditions, “extended-Steinmann-like” conditions, and near-collinear data from the recently-developed form factor operator product expansion. Our results are expected to give the maximally transcendental parts of the gg → Hg and H → ggg amplitudes in the heavy-top limit of QCD. At two loops, the extended-Steinmann-like space of functions we describe contains all transcendental functions required for four-point amplitudes with one massive and three massless external legs, and all massless internal lines, including processes such as gg → Hg and γ * → $q\overline{q}g$. We expect the extended-Steinmann-like space to contain these amplitudes at higher loops as well, although not to arbitrarily high loop order. We present evidence that the planar $\mathcal{N}$ = 4 three-point form factor can be placed in an even smaller space of functions, with no independent ζ values at weights two and three.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Extremum seeking control of distributed energy resources with decaying dither and equilibrium-based switching

Embodiments relate to an operating system coupled to and controlling at least one Distributed Energy Resource (DER) in a smart grid and includes an electricity distribution network and a 2-dimensional Extremum Seeking (2D-ES) controller coupled to network. The electricity distribution network has first and second inputs and one output and maps all active power and reactive power inputs to the smart grid providing measurements of an objective function. The 2D-ES controller controls the DER and includes an active power loop and a reactive power loop. The active power loop is in communication with the first input and the output, governs active power contribution, and receives measurements of the objective function which contain static and oscillatory components. The reactive power loop is in communication with the second input and the output, governs reactive power contribution, and receives measurements of the objective function which contain static and oscillatory components.

Arnold, Daniel↗

Three-color resonance ionization spectroscopy of Zr in Si

As our society becomes technologically more complex, computers are being used in greater and greater numbers of high consequence systems. Giving a machine control over the lives of humans can be disturbing, especially if the software that is run on such a machine has bugs. Formal reasoning is one of the most powerful techniques available to demonstrate the correctness of a piece of software. When reasoning about software and its development, one frequently encounters expressions that contain partial functions. As might be expected, the presence of partial functions introduces an additional dimension of difficulty to the reasoning framework. This difficulty produces an especially strong impact in the case of high consequence systems. An ability to use formal methods for constructing software is essential if we want to obtain greater confidence in such systems through formal reasoning. This is only reasonable under automation of software development and verification. However, the ubiquitous presence of partial functions prevents a uniform application to software of any tools not specifically accounting for partial functions. In this paper we will describe a framework for reasoning about software, based on the nonstrict explicit domain approach, that is applicable to a large class of software/hardware systems. In this framework the Hoare triples containing partial functions can be reasoned about automatically in a well-defined and uniform manner.

Hansen, C. S.↗

Iodine Capture with Metal-Functionalized Polyacrylonitrile Composite Beads Containing Ag 0 , Bi 0 , Cu 0 , or Sn 0 Particles

The capture of radioiodine from nuclear processes and the mitigation of environmental release are important topic areas of research. Some of the more commonly employed chemisorption-type iodine scavengers reported in the literature are based on metal-exchanged porous sorbents such as Ag-zeolites or metal-functionalized aerogels and xerogels. However, another option is to use zero-valent metals directly that have known high affinities for iodine gas [i.e., I2(g)]. In this study, fine metal particles of Ag0, Bi0, Cu0, and Sn0 were embedded in porous polyacrylonitrile (PAN) substrates at 75 mass% metal loadings within the form of ellipsoidal beads with maximum diameters of ~2–3 mm. These composite beads showed extremely high iodine loadings that are directly related to the metal particle loadings. The X-ray diffraction (XRD) analyses of Ag0, Bi0, Cu0, and Sn0 particles as well as metal-PAN composite beads reacted with iodine gas at 120 ± 1 °C showed phases of AgI, BiI3, CuI, and SnI4, respectively. For the Ag-PAN, Cu-PAN, and Sn-PAN beads, no other crystalline peaks were observed in XRD for unreacted metal or oxidized metals after 48 h in saturated I2(g) at 120 ± 1 °C, whereas unreacted metallic Bi0 was observed within the Bi-PAN composites. However, after a 72 h exposure at 120 ± 1 °C, both the Bi0 particles and the Bi-PAN composites showed full conversion from Bi0 to BiI3 with XRD. Comparisons between mass uptake data and X-ray absorption spectroscopy were used to better understand the phase distribution of the Bi phases present in the Bi-PAN+I composites. The iodine loadings (mg iodine per g sorbent, or qe) for these materials were 1120 (Ag-Particle), 1382 (Bi-Particle-72h), 1033 (Cu-Particle), 3000 (Sn-Particle), 753 (Ag-PAN), 1012 (Bi-PAN-72h), 1457 (Cu-PAN), and 1669 (Sn-PAN). It is possible that inexpensive sorbents such as these could be deployed to help limit or prevent release of radioiodine to the environment.

36 MATERIALS SCIENCE↗