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At least 199 records · Page 11

Formation of the infrared emission lines of Mg I in the solar atmosphere

A non-LTE radiative transfer investigation of the emission lines is conducted at 7 and 12 microns using a realistic atomic model for neutral magnesium. An average quiet sun atmospheric model is used to calculate emission-line profiles that resemble the observed ones, i.e., broad absorption troughs with narrow central emission, and significant limb brightening. The charge exchange rates are found to be significant, but the effects of high-n coupling between Mg and Mg(+) together with radiative low-n transitions are of greater importance. It is confirmed that the emission cores are formed no higher than the temperature minimum region, and that the emission is caused by non-LTE effects rather than by the chromospheric temperature rise. It is inferred from the model calculations that the line core is sensitive to magnetic fields located almost 400 km above those measured in ordinary magnetograms; the gas pressure decreases 20-fold between these two heights.

Chang, E. S.↗

Quantum Enhanced Cavity QED Interferometer with Partially Delocalized Atoms in Lattices

Herein, we propose a quantum enhanced interferometric protocol for gravimetry and force sensing using cold atoms in an optical lattice supported by a standing-wave cavity. By loading the atoms in partially delocalized Wannier-Stark states, it is possible to cancel the undesirable inhomogeneities arising from the mismatch between the lattice and cavity fields and to generate spin squeezed states via a uniform one-axis twisting model. The quantum enhanced sensitivity of the states is combined with the subsequent application of a compound pulse sequence that allows us to separate atoms by several lattice sites. This, together with the capability to load small atomic clouds in the lattice at micrometric distances from a surface, make our setup ideal for sensing short-range forces. We show that for arrays of 10 4 atoms, our protocol can reduce the required averaging time by a factor of 10 compared to unentangled lattice-based interferometers after accounting for primary sources of decoherence.

74 ATOMIC AND MOLECULAR PHYSICS↗

Deep Learning Enabled Strain Mapping of Single-Atom Defects in Two-Dimensional Transition Metal Dichalcogenides with Sub-Picometer Precision

Two-dimensional (2D) materials offer an ideal platform to study the strain fields induced by individual atomic defects, yet challenges associated with radiation damage have so far limited electron microscopy methods to probe these atomic-scale strain fields. In this work, we demonstrate an approach to probe single-atom defects with sub-picometer precision in a monolayer 2D transition metal dichalcogenide, WSe 2–2x Te 2x . We utilize deep learning to mine large data sets of aberration-corrected scanning transmission electron microscopy images to locate and classify point defects. By combining hundreds of images of nominally identical defects, we generate high signal-to-noise class averages which allow us to measure 2D atomic spacings with up to 0.2 pm precision. Our methods reveal that Se vacancies introduce complex, oscillating strain fields in the WSe 2–2x Te 2x lattice that correspond to alternating rings of lattice expansion and contraction. These results indicate the potential impact of computer vision for the development of high-precision electron microscopy methods for beam-sensitive materials.

2D materials↗

A new sunspot umbral model and its variation with the solar cycle

Semiempirical model atmospheres are presented for the darkest parts of large sunspot umbrae, regions have called umbral cores. The approach is based on general-purpose computational procedures that are applicable to different types of stellar atmospheres. It is shown that recent umbral intensity measurements of the spectral energy distribution may be accounted for by an umbral core atmospheric model that varies with time during the solar cycle; the observed center-limb variation can be accounted for by the properties of the model. Three umbral core models are presented, corresponding to the early, middle, and late phases of the solar cycle. These three models also may be regarded as having the properties of dark, average, and bright umbral cores respectively. The effects of atomic, opacity, and abundance data uncertainties on the model calculations are briefly discussed. For comparison, a new reference model for the average quiet solar photosphere is given.

Maltby, P.↗

Photoionization of the O 2 molecule

Ground state total and partial photoionization cross sections of the O 2 molecule have been produced with the configuration-average distorted-wave (CADW) approximation, and an energy-corrected pseudo independent-atom (PIA) method. The PIA approach is based on molecular orbitals expressed as a linear combination of atomic orbitals, and utilizes the corresponding atomic-orbital photoionization cross sections. Here we use an energy-corrected PIA approach with atomic photoionization cross sections computed using a CADW method. Our results are found to be in good agreement with photoionization measurements across a wide photon energy range, and in reasonably good agreement with the CADW calculations.

74 ATOMIC AND MOLECULAR PHYSICS↗

Loss of oxygen from Venus

Ionization of thermal and nonthermal oxygen atoms above the plasmapause on Venus supplies an escape flux for O averaging 6 x 10 to the 6th atoms/sq cm-sec. Hydrogen and oxygen atoms escape with stoichiometry characteristic of water. It is argued that escape of H is controlled by the oxidation state of the atmosphere, regulated by escape of O.

Mcelroy, M. B.↗

Effect of substrate tilt on sputter-deposited AuTa films

Gold-tantalum alloy films are of interest for biomedical and magnetically-assisted inertial confinement fusion applications. However, growth mechanisms of such Au-Ta alloy films are not well understood. Here, we systematically study the effect of substrate tilt on properties of films deposited by direct current magnetron sputtering from a AuTa alloy target. Experimental data is correlated with distributions of landing energies and incident angles of sputtered and backscattered species calculated by Monte Carlo simulations of ballistic collisions and gas phase atomic transport. Results reveal that the deposition rate and film density monotonically decrease with increasing substrate tilt. Properties are similar for films with a tilt of 40° and below: films are amorphous, with an average compressive stress of 0.5 GPa, a density of 16 g/cm 3 , and electrical resistivity of 200 μΩ cm. The critical substrate tilt angle for the onset of porosity, a transition to a reduced stress state, and an increase in electrical resistivity lies between 40 and 60°. Based on Monte Carlo simulations, these changes in film properties are correlated with an increase in the average impact angle of the ballistic component of atomic flux. Implications of these results to deposition onto non-planar substrates are discussed.

36 MATERIALS SCIENCE↗

Implementation of variable time step stochastic dynamics for electronically inelastic gas-surface collisions

A variable time step algorithm has been implemented for solving the stochastic equations of motion for gas-surface collisions. It has been tested for a simple model of electronically inelastic collisions with an insulator surface in which the phonon manifold acts as a heat bath and electronic states are localized. In addition to reproducing the accurate nuclear dynamics of the surface atoms, numerical calculations have shown the algorithm to yield accurate ensemble averages of physical observables such as electronic transition probabilities and total energy loss of the gas atom to the surface. This new algorithm offers a gain in efficieny of up to an order of magnitude compared to fixed time step integration.

Garrett, Bruce C.↗

Origin of Stabilization of Ligand-Centered Mixed Valence Ruthenium Azopyridine Complexes: DFT Insights for Neuromorphic Applications

Redox-driven conductance changes are critical processes in molecular- and coordination-complex-based memristive thin films and devices that are envisioned for neuromorphic technologies, but fundamental mechanisms of conductance switching are not fully understood. Here, we explore charge disproportionation (CD) processes in [Ru II L 2 ](PF 6 ) 2 molecular systems that intrinsically involve interfragment charge transfer (IFCT). Using a combination of ab initio molecular dynamics simulation (AIMD), time-dependent density functional theory (TD-DFT), and density functional theory (DFT) calculations, we investigate the electron transfer mechanisms and the roles of temperature and cell volumetric expansion in facilitating the counterion movements and electronic transitions required for low-cost IFCT and charge redistribution. A detailed analysis of the density of states and TD-DFT calculations highlights that unpaired electrons play a crucial role in low-energy transitions, with the azo (N=N) groups of the ligand serving as the primary sites for electronic transport between molecular fragments, further stabilizing the asymmetric state. Localization of added electrons on azo ligands occurs with negligible change at the Ru centers, supported by atomic volume expansions up to +4.74 bohr 3 , and goes along with a progressive reduction of the HOMO−LUMO gap across redox states, suggesting enhanced conductivity. The TD-DFT analysis reveals a dominant IFCT excitation at 2082.76 nm in the doubly reduced (22) state, while a stabilization energy of 1.20 eV of the asymmetric (13) state relative to the symmetric (22) state is predicted by constrained DFT. Periodic DFT and AIMD simulations emulating a molecular film show that the stabilization of the asymmetric state, relative to a symmetric one, translates in net charge separation values (order of ∼0.33 e) that are strongly linked to increased counterion mobility (average counterion displacements exceeding 0.7 Å per atom during CD events) and the involvement of azo groups in electron redistribution. These findings, which align with previously reported experimental and computational data, provide key insights into the IFCT mechanisms and electronic transport facilitated by azo groups, with important implications for redox-driven memristive and neuromorphic technologies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Importance learning estimator for the site-averaged turnover frequency of a disordered solid catalyst

For disordered catalysts such as atomically dispersed “single-atom” metals on amorphous silica, the active sites inherit different properties from their quenched-disordered local environments. The observed kinetics are site-averages, typically dominated by a small fraction of highly active sites. Standard sampling methods require expensive ab initio calculations at an intractable number of sites to converge on the siteaveraged kinetics. We present a new method that efficiently estimates the site-averaged turnover frequency (TOF). The new estimator uses the same importance learning algorithm [Vandervelden et al., React. Chem. Eng. 5, 77 (2020)] that we previously used to compute the siteaveraged activation energy. We demonstrate the method by computing the site-averaged TOF for a simple disordered lattice model of an amorphous catalyst. The results show that with the importance learning algorithm, the site-averaged TOF and activation energy can now be obtained concurrently with orders of magnitude reduction in required ab initio calculations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Composition of interstellar clouds in the disk and halo. 2: Gamma(sup 2) Velorum

High-resolution observations of gamma(sup 2) Vel with the Goddard High-Resolution Spectrograph (GHRS) echelle on the Hubble Space Telescope reveal the presence of seven narrow absorption components, with LSR velocities between -23 and +9 km s(exp -1). Three of these show column density ratios N(S(++))/N(S(+)) and N(P(++))/N(P+)) of about 1 or more, and can be identified as H II regions, while the other four are H I regions, consistent with the O I profile and with the overall H(sup 0) column density of 5.9 x 10(exp 19) cm(exp -2), given the usual assumptions that S is undepleted while O has a depletion D(O) = -0.3 dex. The depletions of Fe, Si, and Mn, which could be measure accurately for two of the four H I regions (components 6 and 7), differ somewhat from the values of D(sub ws) found for slowly moving warm clouds in HD 93521; in particular, for the component at 4.0 km s(exp -1) (No. 6), abosolute of D exceeds absolute of D(sub ws) by 0.1-0.4 dex, while for that at 9.3 km s(exp -1) (No. 7), absolute of D equals absolute of D(sub ws) on the average. The observed ratio of Fe + Mg atoms to Si atoms in the grains of component 6 is 2.04 +/-0.10, consistent with an olivine grain composition; the Fe/Mg ratio is 1.5 +/- 0.2. The electron density in component 6, determined from the C II(sup *) feature, is 0.075 +/- 0.013 cm (exp -3), about two-thirds of that found for clouds of this velocity in HD 93521. In the two conspicuous H II regions, components 3 and 4, n(sub e), determined from the Si II(sup *) feature, is about 1 cm(exp -3). From the column density of S(+) + S(++) in these two components, the total H II path length is about 40 pc. With the radius of a wind-blown bubble around gamma(sup 2) Vel set equal to 60 pc, the effective Stromgren radius is about 100 pc, requiring that T approx. equal to 50,000 K for the Wolf-Rayet component of the gamma(sup 2) Vel binary. Since zeta Pup is a comparable source of ionizing radiation, this temperature is an upper limit. The profiles of the strongest H2 absorption features, from Copernicus archives, indicate that the absorbing molecules have a mean velocity identical with that of the strongest H II component (No. 4). We have no explanation for the possible presence of these H2 molecules in a region of ionized H. Alternatively, the H2 profiles can be explained by molecules in the two adjacent (in velocity) H I regions, components 2 and 5, provided their H I gas has densities and temperatures typical of normal cold clouds. The GHRS data show absorption by highly ionized atoms Si(3+) and C(3+), N(4+) in broad features, in addition to the narrow-line absorption by Si(3+) and C(3+) observed in the dominant H II components, Nos. 3 and 4. The broad C(3+) and N(4+) features have widths corresponding to T in the range (4-8) x 10(exp 5) K, consistent with the broad O(5+) line shown in Copernicus data. Despite some observational uncertainties, the ratios of column densities in the broad C(3+), N(4+), and O(5+) features agree to +/- 0.1 dex with theoretical values for warm gas, heating and evaporating by thermal conduction from an adjacent hot region. Outward evaporation from an isolated cloud in a hot ambient gas cannot be distinguished, on the basis of these data, from inward evaporation of a warm shell, compressed by an expanding, hot stellar-wind bubble. For several halo stars, the C IV/O VI ratio has a quite different average value, perhaps consistent with cooling of infalling hot gas instead of conductive heating and evaporation.

Fitzpatrick, Edward L.↗

Oblique and rippled heliosphere structures from the Interstellar Boundary Explorer

Abstract Past analysis has shown that the heliosphere structure can be deduced from correlations between long-scale solar wind pressure evolution and energetic neutral atom emissions. However, this required spatial and temporal averaging that smoothed out small or dynamic features of the heliosphere. In late 2014, the solar wind dynamic pressure increased by roughly 50% over a period of 6 months, causing a time and directional-dependent rise in around 2–6 keV energetic neutral atom fluxes from the heliosphere observed by the Interstellar Boundary Explorer. Here, we use the 2014 pressure enhancement to provide a simultaneous derivation of the three-dimensional heliospheric termination shock (HTS) and heliopause (HP) distances at high resolution from Interstellar Boundary Explorer measurements. The analysis reveals rippled HTS and HP surfaces that are oblique with respect to the local interstellar medium upwind direction, with significant asymmetries in the heliosphere structure compared to steady-state heliosphere models. We estimate that the heliosphere boundaries contain roughly ten astronomical unit-sized spatial variations, with slightly larger variations on the HTS surface than the HP and a large-scale, southwards-directed obliquity of the surfaces in the meridional plane. Comparisons of the derived HTS and HP distances with Voyager observations indicate substantial differences in the heliosphere boundaries in the northern versus southern hemispheres and their motion over time.

79 ASTRONOMY AND ASTROPHYSICS↗

Lamb shift in the

Energy difference between metastable levels of hydrogen-like atom determined by measuring lifetime in electrostatic field, yielding average Lamb shift in Li ion

STARK EFFECT↗

A study of interstellar lines in the rocket spectrum of delta Scorpii

Ten interstellar lines in the vacuum UV spectrum of delta Sco are analyzed which were recorded on rocket spectrograms. Two cloud components are resolved which have Doppler widths of 1.55 km/sec (larger cloud) and 2.16 km/sec (smaller cloud). Column densities are derived for C I, C II, N I, O I, Al II, Si II, and Fe II, and abundances relative to atomic hydrogen are determined from them. Silicon and iron are found to be slightly overabundant relative to the solar abundances, while the other elements are underabundant by factors ranging from 1.8 to 8.6. Mean cloud densities of 250 and 150 per cu cm (for the larger and smaller clouds, respectively) are determined, and the average ratios of electron density to hydrogen-atom density are derived using the column densities of C I and C II. It is shown that the iron abundance can be decreased to less than the solar abundance by doubling the velocity dispersion of the iron ions.

Smith, A. M.↗

Elucidating facet dependent electronic and electrochemical properties of Cu 2 O nanocrystals using AFM/SCEM and DFT

Cuprous oxide (Cu 2 O) has extensively been studied owing to its excellent optical, magnetic, and catalytic properties. Many of these properties are facet-dependent and have not been well elucidated. This work synthesized cubic, cuboctahedral, octahedral, and rhombic dodecahedral shaped Cu 2 O nanocrystals of ~300 nm in size to evaluate the facet-dependent electrochemical activities. Here, cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) were firstly used to reveal the average electrochemical activities at the ensemble level. Atomic force microscopy-scanning electrochemical microscopy (AFM-SECM) was further used to assess the electrochemical activities of different Cu 2 O nanocrystals at the facet level. Hexaammineruthenium (III) chloride ({Ru(NH 3 ) 6 }Cl 3 ) was employed as the probe molecules that reacted with four different Cu 2 O nanocrystals under —400mV and yielded ~300 pA current between the probing tip and the nanocrystal surface. The tip-current mapping results indicate that rhombic dodecahedral Cu 2 O exhibits higher electrocatalytic activity than other shaped Cu 2 O, due to the presence of dominant exposed facet of {110} as indicated by the relatively high tip current. Density-functional theory (DFT) calculations confirmed the facet dependence of local surface energy and electronic structure of Cu 2 O nanocrystals. Besides electrochemical activity, the surface work function and adsorptive properties were both observed to vary with the shape and dominant exposed facets of Cu 2 O. This study presented a unique experimental and computational chemistry approach to analyze surface electrochemical properties of Cu 2 O crystals at a crystalline facet level.

36 MATERIALS SCIENCE↗

Solar wind contributions to Earth’s oceans

The isotopic composition of water in Earth’s oceans is challenging to recreate using a plausible mixture of known extraterrestrial sources such as asteroids—an additional isotopically light reservoir is required. The Sun’s solar wind could provide an answer to balance Earth’s water budget. Here, we used atom probe tomography to directly observe an average ~1 mol% enrichment in water and hydroxyls in the solar-wind-irradiated rim of an olivine grain from the S-type asteroid Itokawa. We also experimentally confirm that H + irradiation of silicate mineral surfaces produces water molecules. These results suggest that the Itokawa regolith could contain ~20 l m -3 of solar-wind-derived water and that such water reservoirs are probably ubiquitous on airless worlds throughout our Galaxy. The production of this isotopically light water reservoir by solar wind implantation into fine-grained silicates may have been a particularly important process in the early Solar System, potentially providing a means to recreate Earth’s current water isotope ratios.

79 ASTRONOMY AND ASTROPHYSICS↗

Machine learning assisted prediction of the Young’s modulus of compositionally complex alloys

We identify compositionally complex alloys (CCAs) that offer exceptional mechanical properties for elevated temperature applications by employing machine learning (ML) in conjunction with rapid synthesis and testing of alloys for validation to accelerate alloy design. The advantages of this approach are scalability, rapidity, and reasonably accurate predictions. ML tools were implemented to predict Young’s modulus of refractory-based CCAs by employing different ML models. Our results, in conjunction with experimental validation, suggest that average valence electron concentration, the difference in atomic radius, a geometrical parameter λ and melting temperature of the alloys are the key features that determine the Young’s modulus of CCAs and refractory-based CCAs. The Gradient Boosting model provided the best predictive capabilities (mean absolute error of 6.15 GPa) among the models studied. Our approach integrates high-quality validation data from experiments, literature data for training machine-learning models, and feature selection based on physical insights. It opens a new avenue to optimize the desired materials property for different engineering applications.

36 MATERIALS SCIENCE↗

The isotopic composition of galactic cosmic-ray lithium, beryllium, and boron

The isotopes of cosmic-ray Li, Be, and B near 100 MeV per nucleon have been measured with cosmic-ray telescopes on board the IMP-7 and IMP-8 satellites during 1973 and 1974. The measured isotopic abundances provide a stringent test for models of interstellar propagation and solar modulation. It is found that the isotopic abundances can be explained using a steady-state interstellar propagation model with a 5-g/sq cm leakage mean free path. These results, taken along with Be-10 abundance measurements, indicate a longer lifetime for cosmic rays than that predicted by the usual assumption of an average interstellar density of 1 to 3 atoms per cu cm.

Garcia-Munoz, M.↗