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At least 1,153 records · Page 64

Transfer Learning Meets Embedded Correlated Wavefunction Theory for Chemically Accurate Molecular Simulations: Application to Calcium Carbonate Ion Pairing

Achieving chemical accuracy for molecular simulations remains a central challenge in computational chemistry. Here, we present an embedded correlated wavefunction transfer learning (ECW-TL) framework for accurately simulating molecular dynamics in the condensed phase. ECW-TL incorporates high-level electron exchange and correlation effects in ECW theory while preserving the training and computational efficiency of machine-learned interatomic potentials. We demonstrate the framework on Ca 2+ –CO 3 2– ion pairing in aqueous solution, a key process underlying CO 2 mineralization in seawater. As proof of principle, we first show that fine-tuning a DFT-revPBE-D3(BJ) baseline model with embedded-DFT-SCAN data reproduces the DFT-SCAN free-energy surface within 1 kcal/mol across all solvation states. Extending the framework to embedded MP2 and localized natural-orbital CCSD(T) further refines the free-energy profile, revealing the crucial role of exact electron exchange and correlation in determining ion-pair stability and structure. The computed ion-pair association free energy is in quantitative agreement with experimental measurements, further validating the accuracy of the ECW-TL framework. ECW-TL thus provides a general, data-efficient route for transferring CW accuracy to efficient simulations of complex aqueous and interfacial chemical processes.

cluster chemistry↗

Investigation of boosted proton energies through proton radiography of target normal sheath acceleration fields in the multi-ps regime

Multi-kilojoule, multi-picosecond short-pulse lasers, such as the National Ignition Facility-Advanced Radiographic Capability laser and the OMEGA-Extended Performance laser, which have been constructed over the last two decades, enable exciting opportunities to produce high-brightness, high-energy laser-driven proton sources for applications in high-energy-density science like proton fast ignition for inertial fusion energy, particle radiography, and materials science studies. Results on these platforms have demonstrated enhanced accelerated proton energies and electron temperatures when compared to established scaling laws. Recent work has developed a new scaling for proton TNSA in the multi-ps regime. However, this new physics in the multi-ps regime motivates the need to understand the origin of the enhancement in proton energies. Toward this goal, here this work presents the first measurements of the TNSA accelerating sheath field in the multi-ps regime for pulse durations of 0.6, 5, and 10 ps. This measurement was achieved by using a separate TNSA proton source to radiograph the spatiotemporal profile of the accelerating sheath that is responsible for proton acceleration. The use of stacked radiochromic film detectors allows for a discrete time profile of the radiographs, thus enabling the measurement of the temporal and spatial evolution of the accelerating field. In performing this measurement, we extract quantities such as the sheath strength as a function of time and pulse duration, which shows that longer pulse durations sustain a stronger electric field for a longer duration when compared to sub-ps laser pulses, which may enable the observed boosted proton energies and proton conversion efficiencies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Al III, Si IV, and C IV absorption toward zeta Ophiuchi: Evidence for photionized and collisionally ionized gas

We present Goddard High-Resolution Spectrograph observations at 3.5 km/s resolution and signal-to-noise ratios of 30 to 60 for the Al III, Si IV, and N V absorption lines in the far-ultraviolet spectrum of the O9.5 V star zeat Ophiuchi. The measurement reveal three types of highly ionized gas along the 140 pc line of sight. (1) Narrow components of Al III (b = 4.3 km/s, the mean value of (v(helio)) = -7.8 km/s; b = 3.2 km/s, the mean value of (v(sub helio)) = -14.4 km/s) and Si IV (b = 5.3 km/s, the mean value of (v(sub helio)) = -15.0 km/s) trace photionized gas in the expanding H II region surrounding zeta Oph. The observed magnitude and direction of the velocity offset between the Al III and Si IV profiles can be explained by models of H II regions that incorporate expansion. Narrow C IV absorption associated with the H II region is not detected. Predictions of the expected amounts of Si IV and C IV overestimate the column densities of these ions by factors of 30 and more than 10, respectively. The discrepancy may be due to the effects of elemental depletions in the gas and/or to the interaction of the stellar wind with surrounding matter. (2) Broad (b = 15 to 18 km/s) and weak Si IV and C IV absorption components are detected near the mean value of (v(sub helio)) = -26 km/s. The high-ionization species associated with these absorption components are probably produced by electron collisional ionization in a heated gas. This absorption may be physically related to the zeta Oph bow shock ot to a cloud complex situated within the local interstellar medium at d less than 60 pc. The C IV to Si IV column density ratio in this gas is 8, a factor of 6 less than conductive interface models predict, but this discrepancy may be removed by considering the effects of self-photoionization within the cooling gas in the model calculations. (3) A broad (b = 13 km/s) and weak C IV absorption feature detected at the mean value of (v(sub helio)) = -61 km/s is not seen in other species. We tentatively ascribe this absorption to gas in a postshock ragion of an optically thin shock in the zeta Oph stellar wind.

Sembach, Kenneth R.↗

Background and Pickup Ion Velocity Distribution Dynamics in Titan's Plasma Environment: 3D Hybrid Simulation and Comparison with CAPS T9 Observations

In this report we discuss the ion velocity distribution dynamics from the 3D hybrid simulation. In our model the background, pickup, and ionospheric ions are considered as a particles, whereas the electrons are described as a fluid. Inhomogeneous photoionization, electron-impact ionization and charge exchange are included in our model. We also take into account the collisions between the ions and neutrals. The current simulation shows that mass loading by pickup ions H(+); H2(+), CH4(+) and N2(+) is stronger than in the previous simulations when O+ ions are introduced into the background plasma. In our hybrid simulations we use Chamberlain profiles for the atmospheric components. We also include a simple ionosphere model with average mass M = 28 amu ions that were generated inside the ionosphere. The moon is considered as a weakly conducting body. Special attention will be paid to comparing the simulated pickup ion velocity distribution with CAPS T9 observations. Our simulation shows an asymmetry of the ion density distribution and the magnetic field, including the formation of the Alfve n wing-like structures. The simulation also shows that the ring-like velocity distribution for pickup ions relaxes to a Maxwellian core and a shell-like halo.

Lipatov, A. S.↗

Self-organized magnetic equilibria in tokamak plasmas with very low edge safety factor

Tokamak plasmas often exhibit self-organizing behavior in which internal modes shape the toroidal current density profile, a common example being the sawtooth instability. However, such behavior has not been studied in detail for edge safety factor below 2 due to disruptive kink instabilities that typically prevent operation in this regime. Now, steady tokamak plasmas with an edge safety factor down to 0.8 have been created in the Madison Symmetric Torus, where disruptions are prevented due to a thick, conductive wall and a feedback power supply that sustains the plasma current. Internal measurements and nonlinear magnetohydrodynamic modeling reveal a family of safety factor profiles with a central value clamped near unity as the edge safety factor decreases, indicating current profile broadening through a relaxation process. Furthermore, as the safety factor decreases, the magnetic fluctuations become irregular, and the electron energy confinement time decreases.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Analysis of coronal H I Lyman alpha measurements from a rocket flight on 1979 April 13

It is noted that measurements of the profiles of resonantly scattered hydrogen Lyman-alpha coronal radiation have been used in determining hydrogen kinetic temperatures from 1.5 to 4 solar radii from sun center in a quiet region of the corona. Proton temperatures derived using the line widths decrease with height from 2.6 x 10 to the 6th K at 1.5 solar radii to 1.2 x 10 to the 6th K at 4 solar radii. These measurements, together with temperatures for lower heights determined from earlier Skylab and eclipse data, suggest that there is a maximum in the quiet coronal proton temperature at about 1.5 solar radii. Comparison of measured Lyman-alpha intensities with those calculated using a representative model for the radial variation of the coronal electron density yields information on the magnitude of the electron temperature gradient and suggests that the solar wind flow was subsonic for distances less than 4 solar radii.

Withbroe, G. L.↗

Kinetic simulations of anomalous resistivity in high-temperature current carrying plasmas

Anomalous resistivity caused by lower hybrid drift instabilities (LHDIs) has been extensively studied in the literature, and has been invoked to explain the rates of magnetic diffusion and plasma profile evolution in the low-density plasma periphery of theta and screw pinch plasmas. In this article, we present a fully kinetic simulation study of LHDIs with a realistic mass ratio using the particle-in-cell code Chicago over a large range of drift speeds, 0.5 < v$^{2}_{di}$/v$^{2}_{ti}$ < 14.5, plasma β, β ≥ 2×10 –5 , and temperature ratios, 0.1 < T e /T i < 10. The resistivity quantified from the simulations is compared with the analytic estimates from the literature and a generalized resistivity expression is presented, which can be applied over the entire range of plasma environments that were simulated in this study. This expression uses the amplitude of the LHDI fluctuations resulting from instability saturation by electron resonance broadening rather than plateau formation, current relaxation, or ion trapping. The generalized resistivity expression is appropriate for full-scale fluid simulations that encounter a large range of plasma conditions, and has better agreement with the resistivity quantified from kinetic simulations than previous expressions in the literature, particularly at low plasma β. Anomalous resistivity has also been considered as an explanation of the rapid magnetic field dissipation during magnetic reconnection events at large plasma β. At a large β, the magnetic field fluctuations of LHDIs can dominate the electrostatic fluctuations and this article investigates enhanced collisionality due to the nonlinear magnetic force, δJ×δB/c.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Spatially and temporally resolved plasma parameter estimations of laser heated MagLIF relevant gas pipes at NIF

The ability to control laser pre-heat is an integral part of the inertial confinement fusion concept known as Magnetized Liner Inertial Fusion. This process is studied at the National Ignition Facility (NIF) where 4 of the 192 laser beams are propagated through a 1-cm long gas cell where they deposit >20 kJ of energy into the gaseous fuel via inverse bremsstrahlung absorption. This process ionizes the gas, producing a plasma that follows behind the laser front and expands over the radius of the cell. Emission from this plasma, as viewed by a gated x-ray detector, can be used to build spatially and temporally resolved estimations of the pre-heat plasma's density and temperature profiles. This can then be used to estimate the plasma pressure, internal energy, and radiation losses. Estimations show the evolution of the plasma in magnetized and unmagnetized gas cells filled with ambient temperature neopentane (C5H12) +1% Ar, as well as unmagnetized cryogenically cooled (32 K) deuterium +1% Ne filled targets. This analysis shows the effects of initial gas-fill density, composition, and axial magnetization on the time-dependent plasma parameters. Previously, these parameters at the NIF had not been experimentally characterized, and these estimations provided a potential new means of testing radiation magneto-hydrodynamic predictive capability models. Results in unmagnetized targets have strong agreement with simulations. However, in targets with a 19 T applied axial magnetic field, this method yields electron temperatures up to 100% hotter than those predicted by HYDRA codes.

Bremsstrahlung↗

Electron transport barrier and high confinement in configurations with internal islands close to the plasma edge of W7-X

The low magnetic shear in the Wendelstein 7-X (W7-X) stellarator makes it feasible to shape the separatrix by the large islands constituting an island-divertor, and this can be exploited to access various magnetic configurations, including samples of different internal island sizes and locations. To investigate the configuration effects on the plasma confinement, a configuration scan was performed by changing the coil currents to vary the rotational transform between values 5/4 and 5/6 at the plasma boundary with different power levels (2, 4, 6 MW) of electron cyclotron resonance heating (ECRH) at a maximum plasma density of 8 × 10 19 m -2 . neutral beam injection (NBI) heating was also applied during some configurations of the scan to create a density ramp and access high densities beyond the X2 ECRH cutoff. For the magnetic configurations, where the 5/5 and 5/6 island chains were moved closer to separatrix but remaining inside the last closed flux surface, the electron cyclotron emission shows that an electron temperature, T e , pedestal develops already during ECRH heated plasma buildup phase indicating a transport barrier, and the barrier sustains irrespective of changed plasma heating conditions such as NBI in the later part of discharge. The transport barrier is broken by subsequent fast crashes, observed with multiple plasma diagnostics with characteristics such as tokamak edge localized modes, and the corresponding crash amplitude and frequency vary with plasma pressure. The impact of the transport barrier on plasma confinement can be seen through the increased core T e profile, which could be responsible for the overall increase in the stored diamagnetic energy by approximately 10% for these configurations. After the plasma heating is terminated, a backwards transition to a degraded confinement state is also observed. These observations indicate a configuration triggered high confinement mode in low shear W7-X. This work focuses on the occurrence of this transport barrier for different magnetic configurations and its relation to internal magnetic islands.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Experimental and Theoretical Study of the Electronic Structures of Lanthanide Indium Perovskites LnInO 3

Ternary lanthanide indium oxides LnInO 3 (Ln = La, Pr, Nd, Sm) were synthesized by high-temperature solid-state reaction and characterized by Xray powder diffraction. Rietveld refinement of the powder patterns showed the LnInO 3 materials to be orthorhombic perovskites belonging to the space group Pnma, based on almost-regular InO 6 octahedra and highly distorted LnO 12 polyhedra. Experimental structural data were compared with results from density functional theory (DFT) calculations employing a hybrid Hamiltonian. Valence region X-ray photoelectron and K-shell X-ray emission and absorption spectra of the LnInO 3 compounds were simulated with the aid of the DFT calculations. Photoionization of lanthanide 4f orbitals gives rise to a complex final-state multiplet structure in the valence region for the 4f n compounds PrInO 3 , NdInO 3 , and SmInO 3 , and the overall photoemission spectral profiles were shown to be a superposition of final-state 4f n-1 terms onto the cross-section weighted partial densities of states from the other orbitals. The occupied 4f states are stabilized in moving across the series Pr-Nd-Sm. Band gaps were measured using diffuse reflectance spectroscopy. These results demonstrated that the band gap of LaInO 3 is 4.32 eV, in agreement with DFT calculations. This is significantly larger than a band gap of 2.2 eV first proposed in 1967 and based on the idea that In 4d states lie above the top of the O 2p valence band. However, both DFT and X-ray spectroscopy show that In 4d is a shallow core level located well below the bottom of the valence band. Band gaps greater than 4 eV were observed for NdInO 3 and SmInO 3 , but a lower gap of 3.6 eV for PrInO 3 was shown to arise from the occupied Pr 4f states lying above the main O 2p valence band.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Refining internal bilayer structure of bicelles resolved by extended-q small angle X-ray scattering

The internal profile across the bilayer reveals important structural information regarding the crystallinity of acyl chains or the positions of encapsulated species. Here, we demonstrate that a simple five-layer-core-shell discoidal model can be employed tobest fit the extended-qsmall angle X-ray scattering (SAXS) data and resolvethe bilayer internal structure (with sub-nanometer resolution) of a nanoscale discoidal system comprised of a mixture of long-and short-chain lipids(known as “bicelles”). In contrast to the traditional core-shell discoidal model, the detailed structure in the hydrophobic core such as the methylene and methyl groups can be distinguished via this model. The refined model is validated by the SAXS data of bicelles whose electron scattering length density of the hydrophobic core is adjusted by the addition of a long-chain lipid with a fluorine-end group.The higher resolution of the bilayer internal structure can be employed to advance our understanding of the interaction and conformation of the membrane and associated molecules, such as membrane-associated proteins and locations of entrapped species in the lipid nanoparticles.

36 MATERIALS SCIENCE↗

The P prime(f) to N(h) inversion problem in ionospheric soundings

A general review is given of the inversion techniques used to derive the ionospheric electron density N as a function of altitude h from group path P versus frequency f measurements obtained by vertical incidence ionospheric sounders. The paper discusses the medium under investigation, the experimental techniques used to obtain the P(f) data, the theoretical considerations leading to the integral equation relating P(f) to N(h), and the assumptions made in the inversion process. The lamination inversion technique is then presented, with special attention given to mathematical difficulties arising from discontinuities in the P(f) function, infinities in the integrand, and in some cases unknown integration limits. Methods outlined for minimizing the uncertainties due to discontinuities include the use of redundant information - that is the two distinct P(f) functions available for a given N(h) profile - and the use of models based on statistical data. Mathematical procedures are discussed that increase significantly the efficiency and accuracy of the required numerical integrations. The accuracy of the inversion technique is deduced by comparing the resulting N(h) profile with N(h) data obtained by simultaneous but independent observations.

Jackson, J. E.↗

Spacesuit Water Membrane Evaporator; An Enhanced Evaporative Cooling System for the Advanced Extravehicular Mobility Unit Portable Life Support System

Development of the Advanced Extravehicular Mobility Unit (AEMU) portable life support subsystem (PLSS) is currently under way at NASA Johnson Space Center. The AEMU PLSS features a new evaporative cooling system, the Generation 4 Spacesuit Water Membrane Evaporator (Gen4 SWME). The SWME offers several advantages when compared with prior crewmember cooling technologies, including the ability to reject heat at increased atmospheric pressures, reduced loop infrastructure, and higher tolerance to fouling. Like its predecessors, Gen4 SWME provides nominal crew member and electronics cooling by flowing water through porous hollow fibers. Water vapor escapes through the hollow fiber pores, thereby cooling the liquid water that remains inside of the fibers. This cooled water is then recirculated to remove heat from the crew member and PLSS electronics. Test results from the backup cooling system which is based on a similar design and the subject of a companion paper, suggested that further volume reductions could be achieved through fiber density optimization. Testing was performed with four fiber bundle configurations ranging from 35,850 fibers to 41,180 fibers. The optimal configuration reduced the Gen4 SWME envelope volume by 15% from that of Gen3 while dramatically increasing the performance margin of the system. A rectangular block design was chosen over the Gen3 cylindrical design, for packaging configurations within the AEMU PLSS envelope. Several important innovations were made in the redesign of the backpressure valve which is used to control evaporation. A twin-port pivot concept was selected from among three low profile valve designs for superior robustness, control and packaging. The backpressure valve motor, the thermal control valve, delta pressure sensors and temperature sensors were incorporated into the manifold endcaps, also for packaging considerations. Flight-like materials including a titanium housing were used for all components. Performance testing of the Gen4 SWME is underway.

Bue, Grant C.↗

Development of a Sodium LIDAR for Spaceborne Missions

We are currently developing laser and electro-optic technologies to remotely measure Sodium (Na) by adapting existing lidar technology with space flight heritage. The developed instrumentation will serve as the core for the planning of a Heliophysics mission targeted to study the composition and dynamics of Earths mesosphere based on a spaceborne lidar that will measure the mesospheric Na layer. There is a pressing need in the Ionosphere Thermosphere - Mesosphere (ITM) community for high-resolution measurements that can characterize small-scale dynamics (i.e. Gravity Waves with wavelengths smaller than a few hundred km) and their effects in the Mesosphere-Lower-Termosphere (MLT) on a global basis. This is compelling because they are believed to be the dominant contributors to momentum transport and deposition in the MLT, which largely drive the global circulation and thermal structure and interactions with the tides and planetary waves in this region. We are developing a spaceborne remote sensing technique that will enable acquisition of global Na density, temperature and wind measurements in the MLT with the spatial and temporal resolution required to resolve issues associated with the structure, chemistry, dynamics, and energetics of this regionA nadir-pointing spaceborne Na Doppler resonance fluorescence LIDAR on board of the ISS will essentially make high-resolution, in time and space, Na density, temperature and vertical wind measurements, from 75-115 km (MLT region). Our instrument concept consisted of a high-energy laser transmitter at 589 nm and highly sensitive photon counting detector that allows for range-resolved atmospheric-sodium-temperature profiles. The atmospheric temperature is deduced from the linewidth of the resonant fluorescence from the atomic sodium vapor D2 line as measured by our tunable laser. We are currently developing a high power energy laser that allows for some day time sodium lidar observations with the help of a narrow bandpass filter based on etalon or atomic sodium Faraday filter with 5 to 10 pm optical bandwidth. The current baseline detector for the lidar instrument is a 16-channel Photomultiplier Tube with receiver electronics that has been space-qualified for the ICESat-2ATLAS mission. Our technique uses the 16-channels as a photon-number-resolving single detector to provide the required full-spectroscopic sodium lineshape waveform for recovering Mesospheric temperature profiles. In this paper, we will describe our instrument concept for a future Heliophysics space mission based on board of the International Space Station (ISS).

lidar↗

The effect of intermediate-scale motions on line formation

The problem of LTE and non-LTE line formation in the presence of nonthermal velocity fields with geometric scales between the microscopic and macroscopic limits is investigated in the cases of periodic sinusoidal and sawtooth waves. For a fixed source function (the LTE case), it is shown that time-averaged line profiles progress smoothly from the microscopic to the macroscopic limits as the geometric scale of the motions increases, that the sinusoidal motions produce symmetric time-averaged profiles, and that the sawtooth motions cause a redshift. In several idealized non-LTE cases, it is found that intermediate-scale velocity fields can significantly increase the surface source functions and line-core intensities. Calculations are made for a two-level atom in an isothermal atmosphere for a range of velocity scales and non-LTE coupling parameters and also for a two-level atom and a four-level representation of Na I line formation in the Harvard-Smithsonian Reference Atmosphere (1971) solar model. It is found that intermediate-scale velocity fields in the solar atmosphere could explain the central intensities of the Na I D lines and other strong absorption lines without invoking previously suggested high electron densities.

Shine, R. A.↗

VHF power scattered from the mesosphere at mid-latitudes

Scattered power profiles from the Urbana VHF radar have been analyzed. Coherent power returns from the mesosphere (60-90 km) show that a large portion of these returns occur in well-defined stable layers lasting for more than 6 hours in some cases. It is concluded that some of these layers may be caused by standing diurnal tides. Short time variation in scattered power is attributed to internal gravity waves modifying the amplitude and altitude of maximum vertical shear in the horizontal wind. Correlation time of the scattered signal varies with altitude as well as with scattered power. Seasonal averages of the scattered power show a broad peak around 76 km. The decrease in scattered power below 76 km appears because of a decrease in the electron density gradient, while the decrease above 76 km is due to a decrease in the intensity of turbulence. The amplitude of short-period gravity waves shows a decrease with altitude below 66 km, attributed to the Brunt-Vaisala barrier, and a slight increase with altitude above 70 km. The dominant period of the vertical oscillations shows an increase above 63 km, giving further evidence that the high-frequency oscillations present below 63 km cannot propagate to higher altitudes.

Royrvik, O.↗

Arcminute fluctuations in the microwave background from clusters of galaxies

A method for computing arcmin microwave fluctuations produced by Compton scattering of the cosmic background photons by hot electrons in clusters of galaxies is described. Microwave images of the sky for a range of Omega and primordial fluctuation spectral index n are generated which are then 'observed' to determine Delta T/T in precisely the same manner as actual observations to determine if the cluster-induced fluctuations are consistent with the measured upper limit. The geometry used by Uson and Wilkinson (1984) in the NRAO experiment and Readhead et al. (1989) in the OVRO experiment are applied to the simulated images. The 95 percent confidence lower limit for Omega is found to be about 1/10 for n = -1 (which approximates the CDM mass spectrum for clusters), while for n = 0 it is 1/7; for n = +1 the limit is 1/5 if the gas density profile extends to five core radii.

Markevitch, M.↗

Unraveling the Stable Cathode Electrolyte Interface in all Solid‐State Thin‐Film Battery Operating at 5 V

Abstract Spinel‐type LiNi 0.5 Mn 1.5 O 4 (LNMO) is one of the most promising 5 V‐class cathode materials for Li‐ion batteries that can achieve high energy density and low production costs. However, in liquid electrolyte cells, the high voltage causes continuous cell degradation through the oxidative decomposition of carbonate‐based liquid electrolytes. In contrast, some solid‐state electrolytes have a wide electrochemical stability range and can withstand the required oxidative potential. In this work, a thin‐film battery consisting of an LNMO cathode with a solid lithium phosphorus oxynitride (LiPON) electrolyte is tested and their interface before and after cycling is characterized. With Li metal as the anode, this system can deliver stable performance for 600 cycles with an average Coulombic efficiency >99%. Neutron depth profiling indicates a slight overlithiated layer at the interface prior to cycling, a result that is consistent with the excess charge capacity measured during the first cycle. Cryogenic electron microscopy further reveals intimate contact between LNMO and LiPON without noticeable structure and chemical composition evolution after extended cycling, demonstrating the superior stability of LiPON against a high voltage cathode. Consequently, design guidelines are proposed for interface engineering that can accelerate the commercialization of a high voltage cell with solid or liquid electrolytes.

25 ENERGY STORAGE↗