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At least 1,585 records · Page 88

Tip-Enhanced Raman Nanospectroscopy of Smooth Spherical Gold Nanoparticles

We record nanoscale-resolved chemical images of thiobenzonitrile (TBN)-functionalized smooth gold nanospheres on silicon via tip-enhanced Raman (TER) nano-spectroscopy. The recorded images trace the nascence of the familiar doughnut-shaped scattering profile of nanoparticles on silicon at its origin (the particle surface), which appears as a horseshoe-shaped scattering pattern under our experimental conditions. The local optical field maps are in agreement with their simulated finite-difference time-domain analogues. Analysis of the recorded spectra with the aid of ab initio molecular dynamics-based Raman spectral simulations further suggests that optical rectification and molecular charging take place throughout the course of atomic force microscopy-based TER nanoscale chemical imaging.

Bhattarai, Ashish↗

Hydride and Seek: Comparing Crystallographic Hydride Placement Techniques with an Open-Shell Cobalt Complex

Locating hydrides is crucial in organometallic chemistry but difficult to do accurately using X-ray diffraction. Electron diffraction has been proposed as a way to overcome this problem but has not been systematically compared to neutron diffraction and to quantum crystallography (Hirshfeld atom refinement, HAR) to test this hypothesis. Here, we present a comparative analysis of methods for a terminal cobalt hydride complex by comparing a single-crystal neutron diffraction reference structure to results from single-crystal X-ray diffraction with and without Hirshfeld atom refinement (HAR, NoSpherA2), density functional theory (DFT), and electron diffraction (3D-ED/MicroED) refined under kinematical and dynamical formalisms. Conventional X-ray diffraction gives lower precision than neutron diffraction as expected. Despite expected improvements, HAR gives systematic deviation from the neutron benchmark. Interestingly, optimized DFT equilibrium geometries are closer to the neutron value than the value from HAR. On the other hand, electron diffraction with a high-quality data set coupled with dynamical refinement localizes the hydride in difference maps and gives excellent agreement with the neutron data. Dynamical refinement is crucial, as kinematical refinement does not allow assignment of a hydride peak. This cross-modal comparison defines the conditions under which 3D-ED/MicroED delivers high-precision metal–hydride distances for this open-shell cobalt hydride.

anions↗

Effect of Solvent Composition on Non-DLVO Forces and Oriented Attachment of Zinc Oxide Nanoparticles

Oriented attachment (OA) occurs when nanoparticles in solution align their crystallographic axes prior to colliding and subsequently fuse into single crystals. Traditional colloidal theories such as DLVO provide a framework for evaluating OA but fail to capture key particle interactions due to the atomistic details of both the crystal structure and the interfacial solution structure. Using zinc oxide as a model system, we investigated the effect of the solvent on short-ranged and long-ranged particle interactions and the resulting OA mechanism. In situ TEM imaging showed that ZnO nanocrystals in toluene undergo long-range attraction comparable to 1kT at separations of 10 nm and 3kT near particle contact. These observations were rationalized by considering non-DLVO interactions, namely dipole-dipole forces and torques between the polar ZnO nanocrystals. Langevin dynamics simulations showed stronger interactions in toluene compared to methanol solvents, consistent with the experimental results. Concurrently, we performed atomic force microscopy measurements using ZnO-coated probes for the short-ranged interaction. Our data provided valuable insights into another type of non-DLVO interaction, namely the repulsive solvation force. Specifically, the solvation force was stronger in water compared to ethanol and methanol, due to the stronger hydrogen bonding and denser packing of water molecules at the interface. In conclusion, our results highlight the importance of non-DLVO forces in a general framework for understanding and predicting particle aggregation and attachment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Structural basis underlying the synergism of NADase and SLO during group A Streptococcus infection

Group A Streptococcus (GAS) is a strict human pathogen possessing a unique pathogenic trait that utilizes the cooperative activity of NAD + -glycohydrolase (NADase) and Streptolysin O (SLO) to enhance its virulence. How NADase interacts with SLO to synergistically promote GAS cytotoxicity and intracellular survival is a long-standing question. Here, the structure and dynamic nature of the NADase/SLO complex are elucidated by X-ray crystallography and small-angle scattering, illustrating atomic details of the complex interface and functionally relevant conformations. Structure-guided studies reveal a salt-bridge interaction between NADase and SLO is important to cytotoxicity and resistance to phagocytic killing during GAS infection. Furthermore, the biological significance of the NADase/SLO complex in GAS virulence is demonstrated in a murine infection model. Overall, this work delivers the structure-functional relationship of the NADase/SLO complex and pinpoints the key interacting residues that are central to the coordinated actions of NADase and SLO in the pathogenesis of GAS infection.

59 BASIC BIOLOGICAL SCIENCES↗

Delayed Neutron Precursor Group Parameter and Spectra Generation from Fast Fission of 235U in SCALE

Delayed neutron precursor (DNP) group data are important for modeling reactor dynamics. Although the data for individual DNPs have been developed over time, the DNP group data present in the Evaluated Nuclear Data Files (ENDF) have not been updated in the past 20 years. In this work, we use SCALE to recreate the Godiva experiment that was used to generate the original DNP group structure for fast fission of 235U. However, each DNP is modeled using up-to-date data, and the results are then converted into a newly updated group structure. This conversion uses an iterative linear least squares solver to minimize chi-squared. The approaches used in this work also enable energy spectrum generation and uncertainty tracking. The method used in this paper for fast 235U fission DNP group structure updating can be applied to different energies and fissile nuclides. Demonstration of the uncertainty tracking in reactor kinetics and dynamics simulations is shown using point reactor kinetics simulations. Results show that there are data discrepancies between the International Atomic Energy Agency database and data used in ORIGEN, which are currently being fixed. Results also show that the proposed method for group spectra generation performs well.

Seifert, Luke [University of Illinois]↗

A transient site balance model for atomic layer etching

We present a transient site balance model of plasma-assisted atomic layer etching of silicon (Si) with alternating exposure to chlorine gas (Cl 2 ) and argon ions (Ar + ). Molecular dynamics (MD) simulation results are used to provide parameters for the model. The model couples the dynamics of a top monolayer surface region ('top layer') and a perfectly mixed subsurface region ('mixed layer'). The differential equations describing the rates of change of the Cl coverage in the two layers are transient mass balances. Model predictions include Cl coverages and rates of etching of various species from the surface as a function of Cl 2 or Ar + fluence. The simplified phenomenological model reproduces the MD simulation results well over a range of conditions. Comparing model predictions directly to experimental optical emission spectroscopy data, as reported in a previous paper, provides further evidence of the accuracy of the model.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Spectral density reconstruction with Chebyshev polynomials

Accurate calculations of the spectral density in a strongly correlated quantum many-body system are of fundamental importance to study its dynamics in the linear response regime. Typical examples are the calculation of inclusive and semiexclusive scattering cross sections in atomic nuclei and transport properties of nuclear and neutron star matter. Integral transform techniques play an important role in accessing the spectral density in a variety of nuclear systems. However, their accuracy is in practice limited by the need to perform a numerical inversion which is often ill-conditioned. Here, in the present work we extend a recently proposed quantum algorithm which circumvents this problem. We show how to perform controllable reconstructions of the spectral density over a finite energy resolution with rigorous error estimates. An appropriate expansion in Chebyshev polynomials allows for efficient simulations also on classical computers. We apply our idea to obtain the local density of states for graphene in a magnetic field as a proof of principle. This paves the way for future applications in nuclear and condensed matter physics.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Relationship between molecular structure and corrugations in self-assembled polypeptoid nanosheets revealed by cryogenic electron microscopy

Designing conformationally dynamic molecules that self-assemble into predictable nanostructures remains an important unmet challenge. This paper describes how atomic-scale cryogenic transmission electron microscopy (cryo-TEM) can be used to explore the relationship between molecular structure and self-assembly of block copolymers. We examined sheetlike micelles formed in water using a series of diblock copolypeptoids with the same hydrophilic block and three distinct crystalline hydrophobic blocks. Our cryo-TEM images revealed all the structures share nansoscale features, but differ in their intermolecular packing geometries. Different molecular arrangements, parallel and antiparallel V-shaped crystal motifs, were revealed by two-dimensional atomic-scale through-plane images. However, images from tilted samples revealed an unexpected feature when the hydrophobic polypeptoid block comprised phenyl rings with substituted bromine atoms at the para position. The nanosheets contained atomic-scale corrugations that were absent in the other systems which comprised unsubstituted aliphatic and aromatic side chains. We hypothesize that these corrugations are due to the dipolar characteristics of the brominated phenyl group and interactions between this group and water molecules. Published by the American Physical Society 2024

36 MATERIALS SCIENCE↗

Real-time time-dependent density functional theory in Quantum Espresso and related codes

A set of subroutines that interact with an existing computer program, Quantum Espresso (QE), that takes a set of electronic orbitals from QE and propagates them forward in time in response to a number of perturbations. These perturbations include the motion of ions and a wide spectrum of applied electromagnetic fields (e.g., static magnetic fields, slowly-varying electric fields, x-rays, etc.). From the time evolution of the electronic orbitals comes time-varying values of physical observables like the electronic charge and current densities and atomic forces. These are further post-processed to yield properties of interest like stopping powers, conductivities, and the dynamic structure factor. The electronic orbitals are described in a plane wave basis and the equations of motion are carried out using a unitary or approximately unitary time propagation algorithm. Related work will include subroutines for interfacing this capability, as well as others that already exist within QE, with a fork of QE that is more extensible and modular.SAND2019-12611 M Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-NA0003525.

Baczewski, Andrew↗

Machine-learning interatomic potentials for interfaces in all-solid-state batteries: Perspectives on training data, model selection, and validation

Interfaces play a pivotal role in dictating the performance and reliability of all-solid-state batteries (ASSBs), where complex electro-chemo-mechanical phenomena at grain boundaries (GBs) and interfaces can lead to degradation and failure. Traditional atomistic simulation methods, such as first-principles calculations and classical molecular dynamics, face limitations in modeling these interfaces due to either high computational cost or insufficient transferability to the diverse atomic environments evolving at interfaces. Machine-learning interatomic potentials (MLIPs) have emerged as a transformative approach, enabling large-scale, high-accuracy simulations of disordered and chemically complex systems by leveraging the predictability of machine learning models trained on first-principles data. Recent applications of MLIPs have demonstrated their ability to capture intricate behaviors at ASSB interfaces, including ion transport, interfacial evolution, and degradation mechanisms, with accuracy and efficiency unattainable by conventional methods. This prospective paper presents comprehensive analysis and practical guidance for MLIP development for GBs and interfaces in ASSBs, with a focus on three key pillars: data generation, model selection, and validation. Here, we review the current state of MLIP applications for GBs and interfaces in both general and ASSB-specific materials, highlighting best practices and challenges in constructing diverse and representative datasets, choosing appropriate machine learning architectures, and rigorously validating model performance. We also discuss emerging strategies and opportunities for improved reliability and efficiency of MLIPs to simulate realistic interfaces in ASSBs.

Energy - Storage↗

Pre-Flight Testing of Spaceborne GPS Receivers using a GPS Constellation Simulator

The NASA Goddard Space Flight Center (GSFC) Global Positioning System (GPS) applications test facility has been established within the GSFC Guidance Navigation and Control Center. The GPS test facility is currently housing the Global Simulation Systems Inc. (GSSI) STR2760 GPS satellite 40-channel attitude simulator and a STR4760 12-channel navigation simulator. The facility also contains a few other resources such as an atomic time standard test bed, a rooftop antenna platform and a radome. It provides a new capability for high dynamics GPS simulations of space flight that is unique within the aerospace community. The GPS facility provides a critical element for the development and testing of GPS based technologies i.e. position, attitude and precise time determination used on-board a spacecraft, suborbital rocket balloon. The GPS simulation system is configured in a transportable rack and is available for GPS component development as well as for component, spacecraft subsystem and system level testing at spacecraft integration and tests sites. The GPS facility has been operational since early 1996 and has utilized by space flight projects carrying GPS experiments, such as the OrbView-2 and the Argentine SAC-A spacecrafts. The SAC-A pre-flight test data obtained by using the STR2760 simulator and the comparison with preliminary analysis of the GPS data from SAC-A telemetry are summarized. This paper describes pre-flight tests and simulations used to support a unique spaceborne GPS experiment. The GPS experiment mission objectives and the test program are described, as well as the GPS test facility configuration needed to verify experiment feasibility. Some operational and critical issues inherent in GPS receiver pre-flight tests and simulations using this GPS simulation, and test methodology are described. Simulation and flight data are presented. A complete program of pre-flight testing of spaceborne GPS receivers using a GPS constellation simulator is detailed.

Kizhner, Semion↗

Pre-Flight Testing of Spaceborne GPS Receivers Using a GPS Constellation Simulator

The NASA Goddard Space Flight Center (GSFC) Global Positioning System (GPS) applications test facility has been established within the GSFC Guidance Navigation and Control Center. The GPS test facility is currently housing the Global Simulation Systems Inc. (GSSI) STR2760 GPS satellite 40-channel attitude simulator and a STR4760 12-channel navigation simulator. The facility also contains a few other resources such as an atomic time standard test bed, a rooftop antenna platform and a radome. It provides a new capability for high dynamics GPS simulations of space flight that is unique within the aerospace community. The GPS facility provides a critical element for the development and testing of GPS based technologies i.e. position, attitude and precise time determination used on-board a spacecraft, suborbital rocket or balloon. The GPS simulator system is configured in a transportable rack and is available for GPS component development as well as for component, spacecraft subsystem and system level testing at spacecraft integration and test sites. The GPS facility has been operational since early 1996 and has been utilized by space flight projects carrying GPS experiments, such as the OrbView-2 and the Argentine SAC-A spacecrafts. The SAC-A pre-flight test data obtained by using the STR2760 simulator and the comparison with preliminary analysis of the GPS data from SAC-A telemetry are summarized. This paper describes pre-flight tests and simulations used to support a unique spaceborne GPS experiment. The GPS experiment mission objectives and the test program are described, as well as the GPS test facility configuration needed to verify experiment feasibility. Some operational and critical issues inherent in GPS receiver pre-flight tests and simulations using this GPS simulator, and test methodology are described. Simulation and flight data are presented. A complete program of pre-flight testing of spaceborne GPS receivers using a GPS constellation simulator is detailed.

Kizhner, Semion↗

Pre-Flight Testing of Spaceborne GPS Receivers Using a GPS Constellation Simulator

The NASA Goddard Space Flight Center (GSFC) Global Positioning System (GPS) test facility has been established within the GSFC Guidance Navigation and Control Center. The GPS test facility is currently housing the STR2760 GPS satellite 40-channel attitude simulator and an STR4760 12-channel navigation simulator. The facility also contains a few other Goddard resources such as an atomic time standard test bed, a rooftop antenna platform and a radome. It provides a new capability of high dynamics GPS simulations for space flight that is unique within the aerospace community. The GPS facility gives a significant advantage in the development and support of GPS based technologies for position, attitude and precise time determination on-board a spacecraft, sounding rocket or balloon. The GPS simulator system is configured in a transportable rack and is available for GPS applications' component development as well as for spacecraft subsystem and system level testing at spacecraft integration and test sites. The GPS facility has been operational since early 1996 and has been already utilized by a few successful flight projects carrying GPS experiments, such as USA Seastar satellite and the first Argentine satellite SAC-A. The experience in the SAC-A pre-flight testing using the STR2760 simulator is summarized as well as the comparison with preliminary analysis of the GPS data from SAC-A telemetry.

Kizhner, Semion↗

Theoretical Study of Decomposition Pathways for HArF and HKrF

To provide theoretical insights into the stability and dynamics of the new rare gas compounds HArF and HKrF, reaction paths for decomposition processes HRgF to Rg + HF and HRgF to H + Rg + F (Rg = Ar, Kr) are calculated using ab initio electronic structure methods. The bending channels, HRgF to Rg + HF, are described by single-configurational MP2 and CCSD(T) electronic structure methods, while the linear decomposition paths, HRgF to H + Rg + F, require the use of multi-configurational wave functions that include dynamic correlation and are size extensive. HArF and HKrF molecules are found to be energetically stable with respect to atomic dissociation products (H + Rg + F) and separated by substantial energy barriers from Rg + HF products, which ensure their kinetic stability. The results are compatible with experimental data on these systems.

Chaban, Galina M.↗

A Sounding Rocket Mission Concept to Acquire High-Resolution Radiometric Spectra Spanning the 9 nm - 31 nm Wavelength Range

When studying Solar Extreme Ultraviolet (EUV) emissions, both single-wavelength, two- dimensional (2D) spectroheliograms and multi-wavelength, one-dimensional (1D) line spectra are important, especially for a thorough understanding of the complex processes in the solar magnetized plasma from the base of the chromosphere through the corona. 2D image data are required for a detailed study of spatial structures, whereas radiometric (i.e., spectral) data provide information on relevant atomic excitation/ionization state densities (and thus temperature). Using both imaging and radiometric techniques, several satellite missions presently study solar dynamics in the EUV, including the Solar Dynamics Observatory (SDO), Hinode, and the Solar-Terrestrial Relations Observatory (STEREO). The EUV wavelengths of interest typically span 9 nm to 31 nm, with the shorter wavelengths being associated with the hottest features (e.g., intense flares and bright points) and the longer wavelengths associated with cooler features (e.g., coronal holes and filaments). Because the optical components of satellite instruments degrade over time, it is not uncommon to conduct sounding rocket underflights for calibration purposes. The authors have designed a radiometric sounding rocket payload that could serve as both a calibration underflight for and a complementary scientific mission to the upcoming Solar Ultraviolet Imager (SUVI) mission aboard the GOES-R satellite (scheduled for a 2015 launch). The challenge to provide quality radiometric line spectra over the 9-31 nm range covered by SUVI was driven by the multilayer coatings required to make the optical components, including mirrors and gratings, reflective over the entire range. Typically, these multilayers provide useful EUV reflectances over bandwidths of a few nm. Our solution to this problem was to employ a three-telescope system in which the optical components were coated with multilayers that spanned three wavelength ranges to cover the three pairs of SUVI bands. The complete system was designed to fit within the Black Brandt-IX 22.-diameter payload skin envelope. The basic optical path is that of a simple parabolic telescope in which EUV light is focused onto a slit and shutter assembly and imaged onto a normal-incidence diffraction grating, which then disperses the light onto a 2048 2048 CCD sensor. The CCD thus records 1D spatial information along one axis and spectral information along the other. The slit spans 40 arc-minutes in length, thus covering a solar diameter out to +/- 1.3 solar radii. Our operations concept includes imaging at three distinct positions: the north-south meridian, the northeast-southwest diagonal, and real-time pointing at an active region. Six 10-second images will be obtained at each position. Fine pointing is provided by the SPARCS-VII attitude control system typically employed on Black Brandt solar missions. Both before and after launch, all three telescopes will be calibrated with the EUV line emission source and monochromater system at NASA's Stray Light Facility at Marshall Spaceflight Center. Details of the payload design, operations concept, and data application will be presented.

Krause, L. Habash↗

The Ring Current ENA Instrument on the NASA STORIE Mission

NASA has recently selected the Storm Time O+ Ring current Imaging Evolution (STORIE) mission to study the evolution of Earth’s ring current and the role of composition and dynamics during geomagnetic storms. STORIE addresses this inner magnetospheric science through the use of a Ring current Energetic Neutral Atom (RENA) instrument hosted on the International Space Station (ISS). This novel vantage point for ENA imaging has a number of scientific and implementation advantages. RENA is a high sensitivity remote sensing ENA imager and composition instrument with a field of view of 90 x 2 degrees, and an angular resolution of 2 x 2 degrees. The instrument aperture points zenith and its long dimension is oriented perpendicular to the ISS ram direction. As a result, RENA acts as a “push broom” imager building up a complete sky scan of the ring current in a single 90-minute ISS orbit. The instrument employs electrostatic optics along with a foil-MCP TOF x PHA x Delay-Line position measurement technique to resolve H and O energy spectra in the energy range 10-500 KeV for each look direction. Furthermore, it employs triple+ time and position coincidence to effectively reduce background noise from geocoronal and black sky UV as well as penetrating radiation. The abundant mass, power, and telemetry, resources of the ISS allow for large instrument aperture, very high sensitivity, complex data product and simplified operations, altogether contributing towards a high signal to noise (S/N) measurement.

Space Science↗

Framework for simulating gauge theories with dipolar spin systems

Gauge theories appear broadly in physics, ranging from the standard model of particle physics to long-wavelength descriptions of topological systems in condensed matter. However, systems with sign problems are largely inaccessible to classical computations and also beyond the current limitations of digital quantum hardware. In this work, we develop an analog approach to simulating gauge theories with an experimental setup that employs dipolar spins (molecules or Rydberg atoms). We consider molecules fixed in space and interacting through dipole-dipole interactions, avoiding the need for itinerant degrees of freedom. Each molecule represents either a site or gauge degree of freedom, and Gauss's law is preserved by a direct and programmatic tuning of positions and internal state energies. This approach can be regarded as a form of analog systems programming and charts a path forward for near-term quantum simulation. As a first step, we numerically validate this scheme in a small-system study of U(1) quantum link models in (1+1) dimensions with link spin S = 1/2 and S =1 and illustrate how dynamical phenomena such as string inversion and string breaking could be observed in near-term experiments. Our work brings together methods from atomic and molecular physics, condensed matter physics, high-energy physics, and quantum information science for the study of nonperturbative processes in gauge theories.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

A nonequilibrium model for a moderate pressure hydrogen microwave discharge plasma

This document describes a simple nonequilibrium energy exchange and chemical reaction model to be used in a computational fluid dynamics calculation for a hydrogen plasma excited by microwaves. The model takes into account the exchange between the electrons and excited states of molecular and atomic hydrogen. Specifically, electron-translation, electron-vibration, translation-vibration, ionization, and dissociation are included. The model assumes three temperatures, translational/rotational, vibrational, and electron, each describing a Boltzmann distribution for its respective energy mode. The energy from the microwave source is coupled to the energy equation via a source term that depends on an effective electric field which must be calculated outside the present model. This electric field must be found by coupling the results of the fluid dynamics and kinetics solution with a solution to Maxwell's equations that includes the effects of the plasma permittivity. The solution to Maxwell's equations is not within the scope of this present paper.

Scott, Carl D.↗