Results for “atomic ordering” — Page 74

DOE OSTI2022

KATRIN background due to surface radioimpurities

The goal of the KArlsruhe TRItrium Neutrino (KATRIN) experiment is the determination of the effective electron antineutrino mass with a sensitivity of 0.2 eV/c 2 at 90 % C.L. 1 . This goal can only be achieved with a very low background level in the order of 10 mcps 2 in the detector region of interest. A possible background source are α-decays on the inner surface of the KATRIN Main Spectrometer. Rydberg atoms, produced in sputtering processes accompanying the α-decays, are not influenced by electric or magnetic fields and freely propagate inside the vacuum of the Main Spectrometer. Here, they can be ionized by thermal radiation and the released electrons directly contribute to the KATRIN background. Two α-sources, 223 Ra and 228 Th, were installed at the Main Spectrometer with the purpose of temporarily increasing the background in order to study α-decay induced background processes. In this paper, we present a possible background generation mechanism and measurements performed with these two radioactive sources. Our results show a clear correlation between α-activity on the inner spectrometer surface and background from the volume of the spectrometer. Two key characteristics of the Main Spectrometer background – the dependency on the inner electrode offset potential, and the radial distribution – could be reproduced with this artificially induced background. These findings indicate a high contribution of α-decay induced events to the residual KATRIN background.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Impact of a minority relativistic electron tail interacting with a thermal plasma containing high-atomic-number impurities

A minority relativistic electron component can arise in both laboratory and naturally-occurring plasmas. In the presence of high-atomic-number ion species, the ion charge state distribution at low bulk electron temperature can be dominated by relativistic electrons, even though their density is orders of magnitude lower. This is due to the relativistic enhancement of the collisional excitation and ionization cross sections. The resulting charge state effect can dramatically impact the radiative power loss rate and the related Bethe stopping power of relativistic electrons in a dilute plasma.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Triangular lattice quantum dimer model with variable dimer density

Abstract Quantum dimer models are known to host topological quantum spin liquid phases, and it has recently become possible to simulate such models with Rydberg atoms trapped in arrays of optical tweezers. Here, we present large-scale quantum Monte Carlo simulation results on an extension of the triangular lattice quantum dimer model with terms in the Hamiltonian annihilating and creating single dimers. We find distinct odd and even $${{\mathbb{Z}}}_{2}$$ Z 2 spin liquids, along with several phases with no topological order: a staggered crystal, a nematic phase, and a trivial symmetric phase with no obvious broken symmetry. We also present dynamic spectra of the phases, and note implications for experiments on Rydberg atoms.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Hierarchical Self-Assembly Pathways of Peptoid Helices and Sheets

Peptoids (N-substituted glycines) are a class of tailorable synthetic peptidomic polymers. Amphiphilic diblock peptoids have been engineered to assemble 2D crystalline lattices with applications in catalysis and molecular separations. Assembly is induced in an organic solvent/water mixture by evaporating the organic phase, but the assembly pathways remain uncharacterized. We conduct all-atom molecular dynamics simulations of Nbrpe6Nc6 as a prototypical amphiphilic diblock peptoid comprising an NH 2 -capped block of six hydrophobic N-((4-bromophenyl)ethyl)glycine residues conjugated to a polar NH 3 (CH 2 ) 5 CO tail. We identify a thermodynamically controlled assembly mechanism by which monomers assemble into disordered aggregates that self-order into 1D chiral helical rods then 2D achiral crystalline sheets. We support our computational predictions with experimental observations of 1D rods using small-angle X-ray scattering, circular dichroism, and atomic force microscopy and 2D crystalline sheets using X-ray diffraction and atomic force microscopy. Furthermore, this work establishes a new understanding of hierarchical peptoid assembly and principles for the design of peptoid-based nanomaterials.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2023

Active Learning Framework

Machine learning (ML) of interatomic potentials show great promise to accelerate scientific simulation, e.g., by emulating expensive computations at a high accuracy but much reduced computational cost. Training datasets are calculated from computationally expensive ab initio quantum mechanics methods, density functional theory (DFT). Trained on this data, an ML model can be very successful in predicting energy and forces for new atomic configurations. A critical factor is the quality and diversity of the training dataset. Thus, a highly automated approach to dataset construction based on active learning framework is designed suitable for material physics. The active learning scheme begins with fully randomized atomic configurations. Then, many Molecular Dynamics (MD) trajectories are simulated using current ML potentials, where each MD trajectory is initialized to a random disordered configuration. The temperature is varied in order to diversify the sampled configuration during these simulations. The variance of predictions for eight neural networks within an ensemble is analyzed to determine whether the model is operating as expected. This helps in determining whether collecting more data would be helpful to the model by checking the ensemble variance is greater than the threshold. In this case, the MD trajectory is terminated and the final atomic configuration is placed on a queue (SQL database) for DFT calculations and added to training dataset. Periodically, ML model is retrained to the updated training model. This Active Learning loop is iterated until the cost of MD simulations becomes prohibitively expensive. The MD simulations will hopefully be sufficiently robust to support nucleation after many active learning iterations. In this sense, active learning scheme must automatically discover the important low energy and nonequilibrium physics.

Nebgen, Benjamin↗

NASA NTRS2016

Reflectivity Around the Gold L-Edges of X-Ray Reflector of the Soft X-Ray Telescope Onboard ASTRO-H

We report the atomic scattering factor in the 11.215.4 keV for the ASTRO-H Soft X-ray Telescope (SXT) obtained in the ground based measurements. The large effective area of the SXT covers above 10 keV. In fact, the flight data show the spectra of the celestical objects in the hard X-ray band. In order to model the area, the reflectivity measurements in the 11.2-15.4 keV band with the energy pitch of 0.4-0.7 eV were made in the synchrotron beamline Spring-8 BL01B1. We obtained atomic scattering factors f1 and f2 by the curve fitting to the reflectivities of our witness sample. The edges associated with the golds L-I, II, and III transitions are identified, of which the depths are found to be roughly 60 percent shallower than those expected from the Henke's atomic scattering factor.

X-rays↗

DOE OSTI2025

Slimmer Geminals For Accurate F12 Electronic Structure Models

The Slater-type F12 geminal length scales originally tuned for the second-order Mo̷ller-Plesset F12 method are too large for higher-order F12 methods formulated using the SP (diagonal fixed-coefficient spin-adapted) F12 ansatz. The new geminal parameters reported herein reduce the basis set incompleteness errors (BSIEs) of absolute coupled-cluster singles and doubles F12 correlation energies by a significant─and increase with the cardinal number of the basis─margin. The effect of geminal reoptimization is especially pronounced for the cc-pVXZ-F12 basis sets (specifically designed for use with F12 methods) relative to their conventional aug-cc-pVXZ counterparts. The BSIEs of relative energies are less affected, but substantial reductions can be obtained, especially for atomization energies and ionization potentials with the cc-pVXZ-F12 basis sets. The new geminal parameters are therefore recommended for all applications of high-order F12 methods, such as coupled-cluster F12 methods and transcorrelated F12 methods.

Powell, Samuel R. [Virginia Polytechnic Inst. and ↗

NASA NTRS2023

Experimental and Semiclassical Stark Widths and Shifts for Spectral Lines of Neutral and Ionized Atoms (A Critical Review of Experimental and Semiclassical Data for the Period 2008 through 2020)

This Review Article compares new experimental and corresponding semiclassical Stark broadened data for non-hydrogenic spectral lines of neutral atoms and positive ions. This Review covers the period 2008 until the end of 2020 and presents the continuation of previous critical reviews from 1976 (two), 1984 (two), 1990, 2002, and one from 2009. This Review reports the Stark broadening parameters of 1665 spectral lines belonging to 35 elements with 61 different atomic and ion species. The data are taken from 60 papers. Experimental data are arranged by elements and spectra, and these are reported in tables in alphabetical and numerical order, respectively. Each experimental Stark broadening parameter is followed with estimated accuracy. The experimental Stark broadening and shift data presented in the tables are compared with the corresponding semiclassical results available in the literature. In addition, for comparison experiments versus semiclassical theoretical Stark broadening parameters, a numerically improved theoretical approach developed based on Griem and co-workers’ theory is used to evaluate Stark widths and shifts of all studied lines whenever required atomic energy levels data and transition probabilities are available. At the end of the text report, for each analyzed neutral or ion species, the information about the location of the same species data in preceding reviews is given.

Plasma line broadening↗

DOE OSTI2023

Exploring the formation of gold/silver nanoalloys with gas-phase synthesis and machine-learning assisted simulations

While nanoalloys are of paramount scientific and practical interest, the main processes leading to their formation are still poorly understood. Key structural features in the alloy systems, including the crystal phase, chemical ordering, and morphology, are challenging to control at the nanoscale, making it difficult to extend their use to industrial applications. Here, in this contribution, we focus on the gold/silver system that has two of the most prevalent noble metals and combine experiments with simulations to uncover the formation mechanisms at the atomic level. Nanoparticles were produced using a state-of-the-art inert-gas aggregation source and analyzed using transmission electron microscopy and energy-dispersive X-ray spectroscopy. Machine-learning-assisted molecular dynamics simulations were employed to model the crystallization process from liquid droplets to nanocrystals. Our study finds a preponderance of nanoparticles with five-fold symmetric morphology, including icosahedra and decahedra which is consistent with previous results on mono-metallic nanoparticles. However, we observed that gold atoms, rather than silver atoms, segregate at the surface of the obtained nanoparticles for all the considered alloy compositions. These segregation tendencies are in contrast to previous studies and have consequences on the crystallization dynamics and the subsequent crystal ordering. We finally showed that the underpinning of this surprising segregation dynamics is due to charge transfer and electrostatic interactions rather than surface energy considerations.

36 MATERIALS SCIENCE↗

NASA NTRS1986

High intensity 5 eV O-atom exposure facility for material degradation studies

An atomic oxygen exposure facility was developed for studies of material degradation. The goal of these studies is to provide design criteria and information for the manufacture of long life (20 to 30 years) construction materials for use in low Earth orbit. The studies that are being undertaken will provide: (1) absolute reaction cross sections for the engineering design problems, (2) formulations of reaction mechanisms for use in the selection of suitable existing materials and the design of new more resistant ones, and (3) the calibration of flight hardware (mass spectrometers, etc.) in order to directly relate experiments performed in low Earth orbit to ground based investigations. The facility consists of a CW laser sustained discharge source of O-atoms, an atomic beam formation and diagnostics system, a spinning rotor viscometer, and provision for using the system for calibration of actual flight instruments.

Cross, J. B.↗

NASA NTRS2006

Sensitivity Analysis Applied to Atomic Data Used for X-ray Spectrum Synthesis

A great deal of work has been devoted to the accumulation of accurate quantities describing atomic processes for use in analysis of astrophysical spectra. But in many situations of interest the interpretation of a quantity which is observed, such as a line flux, depends on the results of a modeling- or spectrum synthesis code. The results of such a code depends in turn on many atomic rates or cross sections, and the sensitivity of the observable quantity on the various rates and cross sections may be non-linear and if so cannot easily be derived analytically. In such cases the most practical approach to understanding the sensitivity of observables to atomic cross sections is to perform numerical experiments, by calculating models with various rates perturbed by random (but known) factors. In addition, it is useful to compare the results of such experiments with some sample observations, in order to focus attention on the rates which are of the greatest relevance to real observations. In this paper I will present some attempts to carry out this program, focussing on two sample datasets taken with the Chandra HETG. I will discuss the sensitivity of synthetic spectra to atomic data affecting ionization balance, temperature, and line opacity or emissivity, and discuss the implications for the ultimate goal of inferring astrophysical parameters.

Kallman, Tim↗

NASA NTRS2006

Sensitivity Analysis Applied to Atomic Data Used for X-ray Spectrum Synthesis

A great deal of work has been devoted to the accumulation of accurate quantities describing atomic processes for use in analysis of astrophysical spectra. But in many situations of interest the interpretation of a quantity which is observed, such as a line flux, depends on the results of a modeling- or spectrum synthesis code. The results of such a code depends in turn 011 many atomic rates or cross sections, and the sensitivity of the observable quantity on the various rates and cross sections may be non-linear and if so cannot easily be derived analytically. In such cases the most practical approach to understanding the sensitivity of observables to atomic cross sections is to perform numerical experiments, by calculating models with various rates perturbed by random (but known) factors. In addition, it is useful to compare the results of such experiments with some sample observations, in order to focus attention on the rates which are of the greatest relevance to real observations. In this paper I will present some attempts to carry out this program, focussing on two sample datasets taken with the Chandra HETG. I will discuss the sensitivity of synthetic spectra to atomic data affecting ionization balance, temperature, and line opacity or emissivity, and discuss the implications for the ultimate goal of inferring astrophysical parameters.

Kallman, Tim↗

NASA NTRS2008

Testing Photoionization Calculations Using Chandra X-ray Spectra

A great deal of work has been devoted to the accumulation of accurate quantities describing atomic processes for use in analysis of astrophysical spectra. But in many situations of interest the interpretation of a quantity which is observed, such as a line flux, depends on the results of a modeling- or spectrum synthesis code. The results of such a code depends in turn on many atomic rates or cross sections, and the sensitivity of the observable quantity on the various rates and cross sections may be non-linear and if so cannot easily be derived analytically. In such cases the most practical approach to understanding the sensitivity of observables to atomic cross sections is to perform numerical experiments, by calculating models with various rates perturbed by random (but known) factors. In addition, it is useful to compare the results of such experiments with some sample observations, in order to focus attention on the rates which are of the greatest relevance to real observations. In this paper I will present some attempts to carry out this program, focussing on two sample datasets taken with the Chandra HETG. I will discuss the sensitivity of synthetic spectra to atomic data affecting ionization balance, temperature, and line opacity or emissivity, and discuss the implications for the ultimate goal of inferring astrophysical parameters.

Kallman, Tim↗

DOE OSTI2022

Atomic layer epitaxy of kagome magnet Fe 3 Sn 2 and Sn-modulated heterostructures

Magnetic materials with kagome crystal structure exhibit rich physics, such as frustrated magnetism, skyrmion formation, topological flat bands, and Dirac/Weyl points. Until recently, most studies on kagome magnets have been performed on bulk crystals or polycrystalline films. Here, we report the atomic layer molecular beam epitaxy synthesis of high-quality thin films of topological kagome magnet Fe 3 Sn 2 . The structural and magnetic characterization of Fe 3 Sn 2 on epitaxial Pt(111) identifies highly ordered films with c-plane orientation and an in-plane magnetic easy axis. Studies on the local magnetic structure by anomalous Nernst effect imaging reveal in-plane oriented micrometer size domains. Superlattice structures consisting of Fe 3 Sn 2 and Fe 3 Sn are also synthesized by atomic layer molecular beam epitaxy, demonstrating the ability to modulate the sample structure at the atomic level. The realization of high-quality films by atomic layer molecular beam epitaxy opens the door to explore the rich physics of this system and investigate novel spintronic phenomena by interfacing Fe 3 Sn 2 with other materials.

36 MATERIALS SCIENCE↗

NASA NTRS1986

Hot hydrogen atom reactions moderated by H2 and He

Photolysis experiments were performed on the H2-CD4-NH3 and He-CD4-NH3 systems. The photolysis (1849 A) involved only NH3. Mixtures of H2:CD4:NH3 included all combinations of the ratios (200,400,800):(10,20,40):4. Two He:CD4:NH3 mixtures were examined where the ratios equalled the combinations 100:(10,20):4. Abstraction of a D from CD4 by the photolytically produced hot hydrogen from ammonia was monitored by mass spectrometric determination of HD. Both experiment and semiempirical hot-atom theory show that H2 is a very poor thermalizer of hot hydrogens with excess kinetic energy of about 2 eV. Applications of the hard-sphere collision model to the H2-CD4-NH3 system resulted in predicted ratios of net HD production to NH3 decomposition that were two orders of magnitude smaller than the experimental ratios. On the other hand, helium is found to be a very efficient thermalizer; here, the classical model yields reasonable agreement with experiments. Application of a semiempirical hot-atom program gave quantitative agreement with experiment for either system.

Aronowitz, S.↗

DOE OSTI2022

Impact of 2D-3D heterointerface on remote epitaxial interaction through graphene

Remote epitaxy has drawn attention as it offers epitaxy of functional materials that can be released from the substrates with atomic precision. The realization of remote epitaxy leads to profound impact on production and heterointegration of flexible, transferrable, and stackable freestanding single-crystalline membranes, which can be extremely useful in manufacturing next generation electronic and photonic devices. In addition, the remote interaction of atoms and adatoms through two-dimensional (2D) materials in remote epitaxy allows investigation and utilization of electrical/chemical/physical coupling of bulk (3D) materials via 2D materials (3D-2D-3D coupling). Here, we unveil the respective roles and impacts of the substrate material, graphene, substrate-graphene interface, and epitaxial material for electrostatic coupling of these materials. The coupling governs cohesive ordering and can lead to single-crystal epitaxy in the overlying film. We show that simply coating a graphene layer on wafers does not guarantee successful implementation of remote epitaxy, since atomically precise control of the graphene-coated interface is required. Also, it provides key considerations for maximizing the remote electrostatic interaction between the substrate and adatoms. This was enabled by exploring various material systems and processing conditions, and we demonstrate that the rules of remote epitaxy vary significantly depending on the ionicity of material systems as well as the graphene-substrate interface and the epitaxy environment. The general rule of thumb discovered here enables expanding 3D material libraries that can be stacked in freestanding form.

Lu, Kuangye↗

DOE OSTI2022

Impact of 2D-3D heterointerface on remote epitaxial interaction through graphene

Remote epitaxy has drawn attention as it offers epitaxy of functional materials that can be released from the substrates with atomic precision. The realization of remote epitaxy leads to profound impact on production and heterointegration of flexible, transferrable, and stackable freestanding single-crystalline membranes, which can be extremely useful in manufacturing next generation electronic and photonic devices. In addition, the remote interaction of atoms and adatoms through two-dimensional (2D) materials in remote epitaxy allows investigation and utilization of electrical/chemical/physical coupling of bulk (3D) materials via 2D materials (3D-2D-3D coupling). Here, we unveil the respective roles and impacts of the substrate material, graphene, substrate-graphene interface, and epitaxial material for electrostatic coupling of these materials. The coupling governs cohesive ordering and can lead to single-crystal epitaxy in the overlying film. We show that simply coating a graphene layer on wafers does not guarantee successful implementation of remote epitaxy, since atomically precise control of the graphene-coated interface is required. Also, it provides key considerations for maximizing the remote electrostatic interaction between the substrate and adatoms. This was enabled by exploring various material systems and processing conditions, and we demonstrate that the rules of remote epitaxy vary significantly depending on the ionicity of material systems as well as the graphene-substrate interface and the epitaxy environment. The general rule of thumb discovered here enables expanding 3D material libraries that can be stacked in freestanding form.

Lu, KUANGYE↗

DOE OSTI2023

Giant Nonlinear Optical Response via Coherent Stacking of In-Plane Ferroelectric Layers

Thin ferroelectric materials hold great promise for compact nonvolatile memory and nonlinear optical and optoelectronic devices. Herein, an ultrathin in-plane ferroelectric material that exhibits a giant nonlinear optical effect, group-IV monochalcogenide SnSe, is reported. Nanometer-scale ferroelectric domains with ≈90°/270° twin boundaries or ≈180° domain walls are revealed in physical-vapor-deposited SnSe by lateral piezoresponse force microscopy. Atomic structure characterization reveals both parallel and antiparallel stacking of neighboring van der Waals ferroelectric layers, leading to ferroelectric or antiferroelectric ordering. Ferroelectric domains exhibit giant nonlinear optical activity due to coherent enhancement of second-harmonic fields and the as-resulted second-harmonic generation was observed to be 100 times more intense than monolayer WS 2 . This work demonstrates in-plane ferroelectric ordering and giant nonlinear optical activity in SnSe, which paves the way for applications in on-chip nonlinear optical components and nonvolatile memory devices.

36 MATERIALS SCIENCE↗