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At least 667 records · Page 37

Glycerol Electrooxidation over Precision-Synthesized Gold Nanocrystals with Different Surface Facets

Electrochemical glycerol oxidation (EGO) emerges as a promising route to valorize glycerol, an underutilized byproduct from biodiesel production, into value-added chemicals. This study employed three types of gold (Au) nanocrystals with controlled shapes to elucidate the facet-dependent electrocatalytic behavior in EGO. Octahedral, rhombic dodecahedral, and cubic Au nanocrystals with {111}, {110}, and {100} facets, respectively, were precisely synthesized with uniform size and shape. Rhombic dodecahedra exhibited the lowest onset potential for EGO due to facile AuOH formation, while octahedra showed enhanced electrochemical activity for glycerol oxidation and resistance to poisoning. In-situ FTIR analysis revealed that Au {111} surfaces selectively favored C 2 products, whereas Au {100} surfaces promoted C 3 product formation, highlighting the significant effect of facet orientation on EGO performance and informing catalyst design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A practical approach to calculating magnetic Johnson noise for precision measurements

Magnetic Johnson noise is an important consideration for many applications involving precision magnetometry, and its significance will only increase in the future with improvements in measurement sensitivity. The fluctuation–dissipation theorem can be utilized to derive analytic expressions for magnetic Johnson noise in certain situations, but when used in conjunction with finite element analysis tools, the combined approach is particularly powerful as it provides a practical means to calculate the magnetic Johnson noise arising from conductors of arbitrary geometry and permeability. In this paper, we demonstrate this method to be one of the most comprehensive approaches presently available to calculate thermal magnetic noise. In particular, its applicability is shown to not be limited to cases where the noise is evaluated at a point in space but also can be expanded to include cases where the magnetic field detector has a more general shape, such as a finite-size loop, a gradiometer, or a detector that consists of a polarized atomic species trapped in a volume. Furthermore, some physics insights gained through studies made using this method are discussed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

New precision measurements of free neutron beta decay with cold neutrons

Precision measurements in free neutron beta decay serve to determine the coupling constants of beta decay, and offer several stringent tests of the standard model. This study describes the free neutron beta decay program planned for the Fundamental Physics Beamline at the Spallation Neutron Source at Oak Ridge National Laboratory, and finally puts it into the context of other recent and planned measurements of neutron beta decay observables.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Recent advancements in atomic many-body methods for high-precision studies of isotope shifts

The development of atomic many-body methods, capable of incorporating electron correlation effects accurately, is required for isotope shift (IS) studies. In combination with precise measurements, such calculations help to extract nuclear charge radii differences, and to probe for signatures of physics beyond the Standard Model of particle physics. Here, we review here a few recently-developed methods in the relativistic many-body perturbation theory (RMBPT) and relativistic coupled-cluster (RCC) theory frameworks for calculations of IS factors in the highly charged ions (HCIs), and neutral or singly-charged ions, respectively. The results are presented for a wide range of atomic systems in order to demonstrate the interplay between quantum electrodynamics (QED) and electron correlation effects. In view of this, we start our discussions with the RMBPT calculations for a few HCIs by rigorously treating QED effects; then we outline methods to calculate IS factors in the one-valence atomic systems using two formulations of the RCC approach. Then we present calculations for two valence atomic systems, by employing the Fock-space RCC methods. For completeness, we briefly discuss theoretical input required for the upcoming experiments, their possibilities to probe nuclear properties and implications to fundamental physics studies.

QED effects↗

High-precision phase control of an optical lattice with up to 50 dB noise suppression

An optical lattice is a periodic light crystal constructed from the standing-wave interference patterns of laser beams. It can be used to store and manipulate quantum degenerate atoms and is an ideal platform for the quantum simulation of many-body physics. A principal feature is that optical lattices are flexible and possess a variety of multidimensional geometries with modifiable band structure. An even richer landscape emerges when control functions can be applied to the lattice by modulation of the position or amplitude with Floquet driving. However, the desire of realizing high-modulation bandwidths while preserving extreme lattice stability has been difficult to achieve. In this paper, we demonstrate an effective solution that consists of overlapping two counterpropagating lattice beams and controlling the phase and intensity of each with independent acousto-optic modulators. Our phase controller mixes sampled light from both lattice beams with a common optical reference. This dual heterodyne locking method allows exquisite determination of the lattice position, while also removing parasitic phase noise accrued as the beams travel along separate paths. Here, we report up to 50 dB suppression in lattice phase noise in the 0.1–1 Hz band, along with significant suppression spanning more than 4 decades of frequency. The absolute phase diffusion of the lattice position is only 10 Å when integrated over 10 s. This method permits precise, high-bandwidth modulation (greater than 50 kHz) of the optical lattice intensity and phase. We demonstrate the efficacy of this approach by executing intricate time-varying phase profiles for atom interferometry.

Atom interferometry↗

High-precision mass measurement of 103 Sn restores smoothness of the mass surface

As a step towards the ultimate goal of a high-precision mass measurement of doubly magic 100 Sn, the mass of 103 Sn was measured at the Low Energy Beam and Ion Trap (LEBIT) located at the Facility for Rare Isotope Beams (FRIB). Utilizing the time-of-flight ion cyclotron resonance technique, a mass uncertainty of 3.7 keV was achieved, an improvement by more than an order of magnitude compared to a recent measurement performed in 2023 at the Cooler Storage Ring (CSRe) in Lanzhou. Although the LEBIT and CSRe mass measurements of 103 Sn are in agreement, they diverge from the experimental mass value reported in the 2016 version of the Atomic Mass Evaluation (AME2016), which was derived from the measured 𝑄 𝛽 + value and the mass of 103 In. In AME2020, this indirectly measured 103 Sn mass was classified as a “seriously irregular mass” and replaced with an extrapolated value, which aligns with the most recent measured values from CSRe and LEBIT. As such, the smoothness of the mass surface is confidently reestablished for 103 Sn. Here, LEBIT's mass measurement of 103 Sn enabled a significant reduction in the mass uncertainties of five parent isotopes which are now dominated by uncertainties in their respective 𝑄 values.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Experimental determination of precision, resolution, accuracy and trueness of time-of-flight neutron diffraction strain measurements

We discuss a simple statistical analysis which yields the precision, resolution, accuracy and trueness of diffraction-based lattice strain measurements. The procedure consists of measuring the thermal expansion induced in each component of an ideal, non-reacting, two-component, crystalline powder sample in situ. One component, with a high coefficient of thermal expansion (CTE), serves as an internal thermometer. The quantities of interest are obtained by determining the smallest, statistically significant, thermal lattice strain which can be detected through diffraction analysis in the second, low CTE, component in response to controlled temperature changes. This procedure also provides a robust check of the alignment of the diffraction system and is able to reveal the presence of systematic errors. The application of this technique to a time-of-flight engineering diffractometer/strain scanner is presented.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Automating High-Precision X-Ray and Neutron Imaging Applications with Robotics

Los Alamos National Laboratory and the University of Texas at Austin recently implemented a robotically controlled nondestructive testing (NDT) system for X-ray and neutron imaging. This system is intended to address the need for accurate measurements for a variety of parts and, be able to track measurement geometry at every imaging location, and is designed for high-throughput applications. This system was deployed in a beam port at a nuclear research reactor and in an operational inspection X-ray bay. The nuclear research reactor system consisted of a precision industrial seven-axis robot, 1.1-MW TRIGA research reactor, and a scintillator-mirror-camera-based imaging system. The X-ray bay system incorporated the same robot, a 225-keV microfocus X-ray source, and a custom flat panel digital detector. The robotic positioning arm is programmable and allows imaging in multiple configurations, including planar, cylindrical, as well as other user defined geometries that provide enhanced engineering evaluation capability. The imaging acquisition device is coupled with the robot for automated image acquisition. The robot can achieve target positional repeatability within 17 μm in the 3-D space. Flexible automation with nondestructive imaging saves costs, reduces dosage, adds imaging techniques, and achieves better quality results in less time. Specifics regarding the robotic system and imaging acquisition and evaluation processes are presented. In conclusion, this paper reviews the comprehensive testing and system evaluation to affirm the feasibility of robotic NDT, presents the system configuration, and reviews results for both X-ray and neutron radiography imaging applications.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Atomically precise digital e-beam lithography

Hydrogen Depassivation Lithography (HDL) is a version of electron beam lithography that uses scanning tunneling microscope (STM) instrumentation to expose a self–developing resist that is a monolayer of H chemisorbed to a Si (100) 2x1 H-passivated surface. Developed in the 1990s it has been largely a laboratory tool used in research for nanofabrication. Here, the technique is capable of atomic resolution, the ability to remove single H atoms from the Si surface and has much higher precision than the best conventional e-beam lithography can possibly achieve exposing polymeric resists. However, its most promising attribute is that it can be used as a digital fabrication tool and is the first of a class of nanofabrication techniques that can be considered digital atomic scale fabrication technologies. Digital Atomic Scale Fabrication can be shown to have similar advantages over analog fabrication techniques that digital information technology has over analog information technology.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

A Flexure-Based Mechanism for Precision Adjustment of National Ignition Facility Target Shrouds in Three Rotational Degrees of Freedom

This study presents the design of a flexure-based mount allowing adjustment in three rotational degrees of freedom (DOFs) through high-precision set-screw actuators. The requirements of the application called for small but controlled angular adjustments for mounting a cantilevered beam. The proposed design is based on an array of parallel beams to provide sufficiently high stiffness in the translational directions while allowing angular adjustment through the actuators. A simplified physical model in combination with standard beam theory was applied to estimate the deflection profile and maximum stresses in the beams. A finite element model was built to calculate the stresses and beam profiles for scenarios in which the flexure is simultaneously actuated in more than one DOF.

3 DOF↗

Establishing precision and accuracy in PDV results

We need to know uncertainties and systematic errors because we create and compare against archival weapons data, we constrain the models, and we provide scientific results. Good estimates of precision from the data record are available and should be incorporated into existing results; reanalysis of valuable data is suggested. Estimates of systematic errors are largely absent. The original work by Jensen et al. using gun shots for window corrections, and the integrated velocity comparison with X-rays by Schultz are two examples where any systematic errors appear to be <1% level.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

Atomically Precise Metal Nanoclusters for Catalytic Application

The central goal of this project is to explore the catalytic application of atomically precise gold nanoclusters. By solving the total structures of ligand-protected nanoclusters, we aim to correlate the catalytic properties of metal nanoclusters with their atomic/electronic structures. Such correlation unravel some fundamental aspects of nanocatalysis, such as the nature of particle size effect, origin of catalytic selectivity, particle-support interactions, the identification of catalytically active centers, etc. The well-defined nanocluster catalysts mediate the knowledge gap between single crystal model catalysts and real-world conventional nanocatalysts. These nanoclusters also hold great promise in catalyzing certain types of reactions with extraordinarily high selectivity. These aims are in line with the overall goals of the catalytic science and technology of DOE and advance the BES mission “to support fundamental research to understand, predict, and ultimately control matter and energy at the level of electrons, atoms, and molecules”. Our group has successfully prepared different sized, robust gold nanoclusters protected by thiolates, such as Au 25 (SR) 18 , Au 28 (SR) 20 , Au 38 (SR) 24 , Au 99 (SR) 42 , Au 144 (SR) 60 , etc. Some of these nanoclusters have been crystallographically characterized through X-ray crystallography. These ultrasmall nanoclusters (< 2 nm diameter) exhibit discrete electronic structures due to quantum size effect, as opposed to quasicontinuous band structure of conventional metal nanoparticles or bulk metals. The available atomic structures (metal core plus surface ligands) of nanoclusters serve as the basis for structure-property correlations. We have investigated the unique catalytic properties of nanoclusters (i.e. not observed in conventional nanogold catalysts) and revealed the structure-selectivity relationships. Highlights of our works include: i) Effects of ligand, cluster charge state, and size on the catalytic reactivity in CO oxidation, semihydrogenation of alkynes; ii) Size-controlled synthesis of Au-n clusters and structural elucidation; iii) Catalytic mechanisms and correlation with structures of cluster catalyst; iv) Catalytic properties of Au nanorods in chemoselective hydrogenation of nitrobenzaldehyde and visible light driven photocatalytic reactions.

02 PETROLEUM↗

Mixed precision efficiency improvements for multi-physics flow simulations

This report summarizes research activities at Cascade Technologies during February 2020 - November 2020 to support DOE SBIR phase I contract DE-SC0020548. The primary technical objectives of the work are two-fold: a) to establish a theoretical framework to understand the propagation and impact of finite-precision-related errors and b) to quantify the trade-offs between accelerator throughput and solution accuracy through a series of validation tests involving multi-physics flow phenomena.

97 MATHEMATICS AND COMPUTING↗

Improving RNA-Seq Precision with MapAl

With currently available RNA-Seq pipelines, expression estimates for most genes are very noisy. We here introduce MapAl, a tool for RNA-Seq expression profiling that builds on the established programs Bowtie and Cufflinks. In the post-processing of RNA-Seq reads, it incorporates gene models already at the stage of read alignment, increasing the number of reliably measured known transcripts consistently by 50%. Adding genes identified de novo then allows a reliable assessment of double the total number of transcripts compared to other available pipelines. This substantial improvement is of general relevance: Measurement precision determines the power of any analysis to reliably identify significant signals, such as in screens for differential expression, independent of whether the experimental design incorporates replicates or not.

59 BASIC BIOLOGICAL SCIENCES↗

Predictive Risk Mapping of Schistosomiasis in Madagascar Using Ecological Niche Modeling and Precision Mapping

Schistosomiasis is a neglected tropical disease (NTD) found throughout tropical and subtropical Africa. In Madagascar, the condition is widespread and endemic in 74% of all administrative districts in the country. Despite the significant burden of the disease, high-resolution risk maps have yet to be produced to guide national control programs. This study used an ecological niche modeling (ENM) and precision mapping approach to estimate environmental suitability and disease transmission risk. The results show that suitability for schistosomiasis is widespread and covers 264,781 km 2 (102,232 sq miles). Covariates of significance to the model were the accessibility to cities, distance to water, enhanced vegetation index (EVI), annual mean temperature, land surface temperature (LST), clay content, and annual precipitation. Disease transmission risk is greatest in the central highlands, tropical east coast, arid-southwest, and northwest. An estimated 14.9 million people could be at risk of schistosomiasis; 11.4 million reside in rural areas, while 3.5 million are in urban areas. This study provides valuable insight into the geography of schistosomiasis in Madagascar and its potential risk to human populations. Because of the focal nature of the disease, these maps can inform national surveillance programs while improving understanding of areas in need of medical interventions.

60 APPLIED LIFE SCIENCES↗

Precise Manipulation of Multilength Scale Morphology and Its Influence on Eco‐Friendly Printed All‐Polymer Solar Cells

Significant efforts have lead to demonstrations of nonfullerene solar cells (NFSCs) with record power conversion efficiency up to ≈13% for polymer:small molecule blends and ≈9% for all‐polymer blends. However, the control of morphology in NFSCs based on polymer blends is very challenging and a key obstacle to pushing this technology to eventual commercialization. The relations between phases at various length scales and photovoltaic parameters of all‐polymer bulk‐heterojunctions remain poorly understood and seldom explored. Here, precise control over a multilength scale morphology and photovoltaic performance are demonstrated by simply altering the concentration of a green solvent additive used in blade‐coated films. Resonant soft X‐ray scattering is used to elucidate the multiphasic morphology of these printed all‐polymeric films and complements with the use of grazing incidence wide‐angle X‐ray scattering and in situ spectroscopic ellipsometry characterizations to correlate the morphology parameters at different length scales to the device performance metrics. Benefiting from the highest relative volume fraction of small domains, additive‐free solar cells show the best device performance, strengthening the advantage of single benign solvent approach. This study also highlights the importance of high volume fraction of smallest domains in printed NFSCs and organic solar cells in general.

Ye, Long↗

On the Importance of Chemical Precision in Organic Electronics: Fullerene Intercalation in Perfectly Alternating Conjugated Polymers

Abstract The true structure of alternating conjugated polymers—the state‐of‐the‐art materials for many organic electronics—often deviates from the idealized picture. Homocoupling defects are in fact inherent to the widely used cross‐coupling polymerization methods. Nevertheless, many polymers still perform excellently in the envisaged applications, which raises the question if one should really care about these imperfections. This article looks at the relevance of chemical precision (and lack thereof) in conjugated polymers covering the entire spectrum from the molecular scale, to the micro and mesostructure, up to the device level. The different types of polymerization errors for the alkoxylated variant of the benchmark (semi)crystalline polymer poly[2,5‐bis(3‐tetradecylthiophen‐2‐yl)thieno[3,2‐ b ]thiophene (PBTTT) are identified, visualized, and quantified and a general strategy to avoid homocoupling is introduced. Through a combination of experiments and supported by simulations, it is shown that these coupling defects hinder fullerene intercalation and limit device performance as compared to the homocoupling‐free analog. This clearly demonstrates that structural defects do matter and should be generally avoided, in particular when the geometrical regularity of the polymer is essential. These insights likely go beyond the specific PBTTT derivatives studied here and are of general relevance for the wider organic electronics field.

36 MATERIALS SCIENCE↗