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At least 19 records

Machine Learning Predictions of Transition Probabilities in Atomic Spectra

Forward modeling of optical spectra with absolute radiometric intensities requires knowledge of the individual transition probabilities for every transition in the spectrum. In many cases, these transition probabilities, or Einstein A-coefficients, quickly become practically impossible to obtain through either theoretical or experimental methods. Complicated electronic orbitals with higher order effects will reduce the accuracy of theoretical models. Experimental measurements can be prohibitively expensive and are rarely comprehensive due to physical constraints and sheer volume of required measurements. Due to these limitations, spectral predictions for many element transitions are not attainable. In this work, we investigate the efficacy of using machine learning models, specifically fully connected neural networks (FCNN), to predict Einstein A-coefficients using data from the NIST Atomic Spectra Database. For simple elements where closed form quantum calculations are possible, the data-driven modeling workflow performs well but can still have lower precision than theoretical calculations. For more complicated nuclei, deep learning emerged more comparable to theoretical predictions, such as Hartree–Fock. Unlike experiment or theory, the deep learning approach scales favorably with the number of transitions in a spectrum, especially if the transition probabilities are distributed across a wide range of values. It is also capable of being trained on both theoretical and experimental values simultaneously. In addition, the model performance improves when training on multiple elements prior to testing. The scalability of the machine learning approach makes it a potentially promising technique for estimating transition probabilities in previously inaccessible regions of the spectral and thermal domains on a significantly reduced timeline.

74 ATOMIC AND MOLECULAR PHYSICS↗

Preliminary look at CARS spectra from atomic oxygen

Contains fundamental spectroscopic results regarding atomic oxygen. Data represent basic science contributions and are not associated with an application or defense article.

Kearney, Sean Patrick [Sandia National Laboratorie↗

Small energy gap revealed in CrBr 3 by scanning tunneling spectroscopy

CrBr 3 is a layered van der Waals material with magnetic ordering down to the 2D limit. For decades, based on optical measurements, it is believed that the energy gap of CrBr 3 is in the range of 1.68–2.1 eV. However, controversial results have indicated that the band gap of CrBr 3 is possibly smaller than that. An unambiguous determination of the energy gap is critical to the correct interpretations of the experimental results of CrBr 3 . Here, we present the scanning tunneling microscopy and spectroscopy (STM/S) results of CrBr 3 thin and thick flakes exfoliated onto highly ordered pyrolytic graphite (HOPG) surfaces and density functional theory (DFT) calculations to reveal the small energy gap (peak-to-peak energy gap to be 0.57 ± 0.04 eV; or the onset signal energy gap to be 0.29 ± 0.05 eV from dI/dV spectra). Atomic resolution topography images show the defect-free crystal structure and the dI/dV spectra exhibit multiple peak features measured at 77 K. The conduction band – valence band peak pairs in the multi-peak dI/dV spectrum agree very well with all reported optical transitions. STM topography images of mono- and bi-layer CrBr 3 flakes exhibit edge degradation due to short air exposure (~15 min) during sample transfer. The unambiguously determined small energy gap settles the controversy and is the key in better understanding CrBr 3 and similar materials.

36 MATERIALS SCIENCE↗

A lumped particle direct simulation Monte-Carlo method combined with the collisional-radiative model for simulations of non-equilibrium laser-induced plasma plumes

Collisional plasma plumes induced by laser irradiation of material targets exhibit large variations in local density as well as ionization and excitation states, making purely hydrodynamic or kinetic simulations inaccurate or infeasible. To address this challenge and capture non-equilibrium effects in laser-induced plasma plumes at arbitrary degrees of ionization, we develop a hybrid computational approach that combines the kinetic direct simulation Monte Carlo (DSMC) method with a collisional-radiative model (CRM). This ℓDSMC-CRM approach utilizes a lumped particle method to represent minor fractions of excited ions in particle-based simulations and a special coarse-graining technique for atomic spectra and photoionization rates, ensuring numerical convergence at reduced computational cost. The hybrid approach is applied to simulate spatially homogeneous relaxation as well as one- and two-dimensional expansions of plasma plumes induced by irradiation of a copper target by a nanosecond laser pulse in a vacuum or background gas. The comparison with an equilibrium model, where local Saha-Boltzmann equilibrium is enforced, shows that the non-equilibrium effects play a dominant role. The equilibrium model can fail to predict the flow structure and strongly underestimate the degree of absorption of laser radiation by the plume. The ℓDSMC-CRM approach is validated against experimental data demonstrating reasonable agreement with the experimental electron density and temperature, while the equilibrium model is found to dramatically underestimate electron density and temperature. The flexibility of the ℓDSMC-CRM approach allows for its seamless integration into existing DSMC frameworks, making it a valuable tool for high-fidelity plasma modeling in laser-material interactions, laser-based manufacturing, and beyond.

97 MATHEMATICS AND COMPUTING↗

A new generation of effective core potentials from correlated and spin–orbit calculations: Selected heavy elements

We introduce new correlation consistent effective core potentials (ccECPs) for the elements I, Te, Bi, Ag, Au, Pd, Ir, Mo, and W with 4d, 5d, 6s, and 6p valence spaces. These ccECPs are given as a sum of spin-orbit averaged relativistic effective potential (AREP) and effective spin–orbit (SO) terms. The construction involves several steps with increasing refinements from more simple to fully correlated methods. The optimizations are carried out with objective functions that include weighted many-body atomic spectra, norm-conservation criteria, and SO splittings. Transferability tests involve molecular binding curves of corresponding hydride and oxide dimers. The constructed ccECPs are systematically better and in a few cases on par with previous effective core potential (ECP) tables on all tested criteria and provide a significant increase in accuracy for valence-only calculations with these elements. Our study confirms the importance of the AREP part in determining the overall quality of the ECP even in the presence of sizable spin–orbit effects. The subsequent quantum Monte Carlo calculations point out the importance of accurate trial wave functions that, in some cases (mid-series transition elements), require treatment well beyond a single-reference.

Wang, Guangming (ORCID:0000000231327925)↗

Correlation consistent effective core potentials for late 3 d transition metals adapted for plane wave calculations

We construct a new modification of correlation consistent effective core potentials (ccECPs) for late 3d elements Cr–Zn with Ne-core that are adapted for efficiency and low energy cut-offs in plane wave calculations. The decrease in accuracy is rather minor, so that the constructions are in the same overall accuracy class as the original ccECPs. The resulting new constructions work with energy cut-offs at or below ≈400 Ry and, thus, make calculations of large systems with transition metals feasible for plane wave codes. We also provide the basic benchmarks for atomic spectra and molecular tests of this modified option that we denote as ccECP-soft.

Chemistry↗

Sensitivity of EDM experiments in paramagnetic atoms and molecules to hadronic CP violation

Experiments searching for the electric dipole moment (EDM) of the electron d e utilize atomic/molecular states with one or more uncompensated electron spins, and these paramagnetic systems have recently achieved remarkable sensitivity to d e . If the source of CP violation resides entirely in the hadronic sector, the two-photon exchange processes between electrons and the nucleus induce CP-odd semileptonic interactions, parametrised by the Wilson coefficient C SP , and provide the dominant source of EDMs in paramagnetic systems instead of d e . We evaluate the C SP coefficients induced by the leading hadronic sources of CP violation, namely nucleon EDMs and CP-odd pion-nucleon couplings, by calculating the nucleon-number-enhanced CP-odd nuclear scalar polarisability, employing chiral perturbation theory at the nucleon level and the Fermi-gas model for the nucleus. This allows us to translate the ACME EDM limits from paramagnetic ThO into novel independent constraints on the QCD theta term |$\bar θ$| < 3 × 10 –8 , proton EDM |d p | < 2 × 10 –23 e cm, isoscalar CP-odd pion-nucleon coupling |$\bar g$$^{(1)}_{πNN}$| < 4 × 10 –10 , and color EDMs of quarks |$\tilde d$ u -$\tilde $d d | < 2 × 10 –24 cm. We note that further experimental progress with EDM experiments in paramagnetic systems may allow them to rival the sensitivity of EDM experiments with neutrons and diamagnetic atoms to these quantities.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Visualizing Anisotropic Oxygen Diffusion in Ceria under Activated Conditions

Oxygen reactivity plays a key role in the performance of ceria-based catalysts. Aberration-corrected transmission electron microscopy and molecular dynamics simulations were used to study the oxygen atom diffusion in ceria under activated conditions. Reactive oxygen atom and its real-time diffusion were visualized. Additionally, the interplay between cerium and oxygen atoms originating from a Coulomb interaction was revealed by the out-of-plane buckling of cerium atoms associated with oxygen transport. Anisotropic oxygen atom diffusion that depends on crystal orientations was discovered, demonstrating a preferential [001] crystallographic diffusion pathway. These findings reveal prospects for applications of anisotropic orientation-relevant fluorite-structured oxides.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Probing New Bosons and Nuclear Structure with Ytterbium Isotope Shifts

In this Letter, we present mass-ratio measurements on highly charged Yb 42+ ions with a precision of 4 ×10 -12 and isotope-shift measurements on Yb + on the 2 S 1/2 → 2 D 5/2 and 2 S 1/2 → 2 F 7/2 transitions with a precision of 4 ×10 -9 for the isotopes 168,170,172,174,176 Yb. We present a new method that allows us to extract higher-order changes in the nuclear charge distribution along the Yb isotope chain, benchmarking ab initio nuclear structure calculations. Additionally, we perform a King plot analysis to set bounds on a fifth force in the keV/c 2 to MeV/c 2 range coupling to electrons and neutrons.

74 ATOMIC AND MOLECULAR PHYSICS↗

Doppler-Free Saturation Spectroscopy (DFSS) for Magnetic and Electric Field Measurements in an FRC plasma

The Cooperative Research and Development Agreement (CRADA) between Oak Ridge National Laboratory (ORNL) and TAE Technologies (TAE) focused on a feasibility study of Doppler-free saturation spectroscopy (DFSS) as a diagnostic strategy to measure the internal magnetic and electric fields of TAE’s C-2W field-reversed configuration (FRC) fusion device. Non-perturbative measurements of magnetic and electric fields in the core of FRCs can provide critical information needed to constrain equilibrium models and for the continued advancement of the fusion research program at TAE. DFSS is a well-established, laser-based absorption spectroscopy technique used to suppress inhomogeneous (Doppler) broadening linewidths and reveal Zeeman/Stark split hyperfine structures of target emission lines. The collaboration involved the use of ORNL’s suite of experimentally validated quantum mechanical modelling codes to simulate theoretical atomic spectra for a variety of machine parameters and laser beam configurations. TAE’s expertise was heavily used to provide measurements/models of the required machine parameters needed as inputs to the simulations. Results of an all-encompassing error analysis demonstrate the favourable capabilities of the diagnostic and provided invaluable insights as to how DFSS can be best used to accurately measure internal B/E-fields in C-2W.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

On the instrument-dependent appearance of ion dissociation events in atom probe tomography mass spectra

The successful application of atom probe tomography (APT) relies on the accurate interpretation of the mass spectrum (i.e. m/z histogram) from a sample. Some materials yield mass spectra that are amenable to a straightforward peak assignment/ranging, however, there are many materials that produce mass spectra with features that defy simple interpretation. One such example is Ga 2 O 3 which yields mass spectra containing several broad and difficult to interpret features. Herein, we study the GaO 2+ → O 1+ + Ga 1+ dissociation and we explain how this dissociation process gives rise to broad and previously unassigned features in the mass spectrum. Trajectory simulations are performed for the dissociation reaction utilizing realistic electrostatic models and compared to experiments using commercially available straight flight and reflectron based local electrode (LE) APT instruments. It is shown that the appearance of these features is strongly dependent on the specific design of the time-of-flight (ToF) mass analyzer. Additionally, we explore how various experimental parameters can affect the appearance of the dissociation process in the one-dimensional (1D) mass spectrum and in the two-dimensional (2D) correlation histogram. While the focus of this work is on a particular dissociation process related to Ga 2 O 3 , the understanding gained in the course of these simulations and experiments should be applicable to the interpretation of dissociation processes in other materials.

47 OTHER INSTRUMENTATION↗

Ionization and temperature measurements in warm dense copper using x-ray absorption spectroscopy

We detail experimental results inferring ionization and temperature for warm dense copper plasmas at several times solid density (15–25 g/cm 3 ) and temperatures of 10–21 eV. Experiments performed at the OMEGA Laser Facility generate uniform warm dense matter conditions via symmetric shock compression of a buried copper layer. The plasma is probed with a laser-generated x-ray source to collect the K-shell x-ray absorption spectrum. Fitting bound-bound absorption contributions from constituent charge states of copper provides an estimated $\overline{Z}$ of approximately 4–7 for these warm dense copper plasmas. We find that these partially ionized plasmas have K-edge shifts of 12–30 eV and bound-bound resonance 1s → 3p absorption shifts of 4–26 eV with respect to the cold K edge. This study provides necessary experimental data to improve ionization and opacity models in the warm dense matter regime.

42 ENGINEERING↗

Laser-Plasma Spatiotemporal Cyanide Spectroscopy and Applications

This article reports new measurements of laser-induced plasma hypersonic expansion measurements of diatomic molecular cyanide (CN). Focused, high-peak-power 1064 nm Q-switched radiation of the order of 1 TW/cm 2 generated optical breakdown plasma in a cell containing a 1:1 molar gas mixture of N 2 and CO 2 at a fixed pressure of 1.1 × 10 5 Pascal and in a 100 mL/min flow of the mixture. Line-of-sight (LOS) analysis of recorded molecular spectra indicated the outgoing shockwave at expansion speeds well in excess of Mach 5. Spectra of atomic carbon confirmed increased electron density near the shockwave, and, equally, molecular CN spectra revealed higher excitation temperature near the shockwave. Results were consistent with corresponding high-speed shadowgraphs obtained by visualization with an effective shutter speed of 5 nanoseconds. In addition, LOS analysis and the application of integral inversion techniques allow inferences about the spatiotemporal plasma distribution.

36 MATERIALS SCIENCE↗

All-Order Full-Coulomb Quantum Spectral Line-Shape Calculations

Understanding how atoms interact with hot dense matter is essential for astrophysical and laboratory plasmas. Interactions in high-density plasmas broaden spectral lines, providing a rare window into interactions that govern, for example, radiation transport in stars. However, up to now, spectral line-shape theories employed at least one of three common approximations: second-order Taylor treatment of broadening operator, dipole-only interactions between atom and plasma, and classical treatment of perturbing electrons. In this Letter, we remove all three approximations simultaneously for the first time and test the importance for two applications: neutral hydrogen and highly ionized magnesium and oxygen. Finally, we found 15%–50% change in the spectral line widths, which are sufficient to impact applications including white-dwarf mass determination, stellar-opacity research, and laboratory plasma diagnostics.

79 ASTRONOMY AND ASTROPHYSICS↗

Emission Spectra of Uranium Particulates at High Temperature

The emission spectrum of micron-scale uranium particulates at high temperatures in the ultraviolet, visible, and near-infrared spectral regions is investigated using a heterogeneous shock tube. Temperatures from 3000 to 9000 K are characterized in an inert argon environment and with incremental amounts of added oxygen. Atomic line spectra do not emerge above the continuum emission spectrum until between 4500 and 5000 K in pure argon, and 6100 and 6600 K in 1% oxygen. For 5% oxygen, however, the threshold for atomic emission drops below 3800 K. Uranium monoxide molecular emission in the strongest visible band at 595.4 nm is not observed at any condition. Uncertainties in particle temperature determination in high-temperature shock tube environments are discussed, and limitations to such measurements are presented, such as those from experimental factors such as the powder loading method and expected detection limits of uranium species in relevant conditions.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Nano-spectroscopy of excitons in atomically thin transition metal dichalcogenides

Abstract Excitons play a dominant role in the optoelectronic properties of atomically thin van der Waals (vdW) semiconductors. These excitons are amenable to on-demand engineering with diverse control knobs, including dielectric screening, interlayer hybridization, and moiré potentials. However, external stimuli frequently yield heterogeneous excitonic responses at the nano- and meso-scales, making their spatial characterization with conventional diffraction-limited optics a formidable task. Here, we use a scattering-type scanning near-field optical microscope (s-SNOM) to acquire exciton spectra in atomically thin transition metal dichalcogenide microcrystals with previously unattainable 20 nm resolution. Our nano-optical data revealed material- and stacking-dependent exciton spectra of MoSe 2 , WSe 2 , and their heterostructures. Furthermore, we extracted the complex dielectric function of these prototypical vdW semiconductors. s-SNOM hyperspectral images uncovered how the dielectric screening modifies excitons at length scales as short as few nanometers. This work paves the way towards understanding and manipulation of excitons in atomically thin layers at the nanoscale.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Machine learning in analytical spectroscopy for nuclear diagnostics [Invited]

Analytical spectroscopy methods have shown many possible uses for nuclear material diagnostics and measurements in recent studies. In particular, the application potential for various atomic spectroscopy techniques is uniquely diverse and generates interest across a wide range of nuclear science areas. Over the last decade, techniques such as laser-induced breakdown spectroscopy, Raman spectroscopy, and x-ray fluorescence spectroscopy have yielded considerable improvements in the diagnostic analysis of nuclear materials, especially with machine learning implementations. These techniques have been applied for analytical solutions to problems concerning nuclear forensics, nuclear fuel manufacturing, nuclear fuel quality control, and general diagnostic analysis of nuclear materials. The data yielded from atomic spectroscopy methods provide innovative solutions to problems surrounding the characterization of nuclear materials, particularly for compounds with complex chemistry. Implementing these optical spectroscopy techniques can provide comprehensive new insights into the chemical analysis of nuclear materials. In particular, recent advances coupling machine learning methods to the processing of atomic emission spectra have yielded novel, robust solutions for nuclear material characterization. This review paper will provide a summation of several of these recent advances and will discuss key experimental studies that have advanced the use of analytical atomic spectroscopy techniques as active tools for nuclear diagnostic measurements.

Rao, Ashwin P. (ORCID:0000000319312568)↗