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DOE OSTI2021

Mechanistic Pathways for N 2 O Elimination from trans -R 3 Sn-O-N=N-O-SnR 3 and for Reversible Binding of CO 2 to R 3 Sn-O-SnR 3 (R = Ph, Cy)

The rate and mechanism of the elimination of N 2 O from trans-R 3 Sn-O-N=N-O-SnR 3 (R = Ph ( 1 Ph ) and R = Cy ( 1 Cy )) to form R 3 Sn-O-SnR 3 (R = Ph ( 2 Ph ) and R = Cy ( 2 Cy )) have been studied using both NMR and IR techniques to monitor the reactions in the temperature range of 39–79 °C in C 6 D 6 . Activation parameters for this reaction are ΔH ‡ = 15.8 ± 2.0 kcal·mol –1 and ΔS ‡ = –28.5 ± 5 cal·mol –1 ·K –1 for 1 Ph and ΔH ‡ = 22.7 ± 2.5 kcal·mol –1 and ΔS ‡ = –12.4 ± 6 cal·mol –1 ·K –1 for 1 Cy . Addition of O 2 , CO 2 , N 2 O, or PPh 3 to sealed tube NMR experiments did not alter in a detectable way the rate or product distribution of the reactions. Computational DFT studies of elimination of hyponitrite from trans-Me 3 Sn-O-N=N-O-SnMe 3 ( 1 Me ) yield a mechanism involving initial migration of the R 3 Sn group from O to N passing through a marginally stable intermediate product and subsequent N 2 O elimination. Reactions of 1 Ph with protic acids HX are rapid and lead to formation of R 3 SnX and trans-H 2 N 2 O 2 . Reaction of 1 Ph with the metal radical •Cr(CO) 3 C 5 Me 5 at low concentrations results in rapid evolution of N 2 O. At higher •Cr(CO) 3 C 5 Me 5 concentrations, evolution of CO 2 rather than N 2 O is observed. Addition of 1 atm or less CO 2 to benzene or toluene solutions of 2 Ph and 2 Cy resulted in very rapid reaction to form the corresponding carbonates R 3 Sn-O-C(=O)-O-SnR 3 (R = Ph ( 3 Ph ) and R = Cy ( 3 Cy )) at room temperature. Evacuation results in fast loss of bound CO 2 and regeneration of 2 Ph and 2 Cy . Variable temperature data for formation of 3 Cy yield ΔH o = –8.7 ± 0.6 kcal·mol –1 , ΔS o = –17.1 ± 2.0 cal·mol –1 ·K –1 , and ΔG o 298K = –3.6 ± 1.2 kcal·mol –1 . Furthermore, DFT studies were performed and provide additional insight into the energetics and mechanisms for the reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

A Transferable Force Field for Simulating Adsorption in Metal–Organic Frameworks with Open Metal Sites Based on the 12–6–4 Lennard-Jones Potential

Metal−organic frameworks (MOFs) that contain coordinatively unsaturated open metal sites (OMSs) provide strong host− guest interactions, making them promising sorbents for low-concentration gas adsorption applications such as direct air capture and atmospheric water harvesting. However, accurately modeling host−guest interactions involving OMSs remains challenging for classical force fields (FFs) based on the 12−6 Lennard−Jones (LJ) potential, as the polarization effect of the guest molecule induced by the positively charged OMS is not considered. Here, we introduce an FF based on the 12−6−4 LJ potential, which incorporates charge−induced dipole interactions and is parametrized against a diverse set of host−guest potential energy surfaces (PESs) obtained from density functional theory (DFT). The resulting FF, trained on a generic trimetallic cluster, performs well in both host−guest binding energetics and gas adsorption isotherms across different OMS-containing MOFs, including MOF-74 series and Cu-BTC. These results highlight the excellent transferability of our approach and its potential to enhance the accuracy and robustness of high-throughput MOF discovery workflows, particularly for gas adsorption and separation in large and diverse MOF databases.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Mechanistic investigation of SARS-CoV-2 main protease to accelerate design of covalent inhibitors

Targeted covalent inhibition represents one possible strategy to block the function of SARS-CoV-2 Main Protease (M PRO ), an enzyme that plays a critical role in the replication of the novel SARS-CoV-2. Toward the design of covalent inhibitors, we built a covalent inhibitor dataset using deep learning models followed by high throughput virtual screening of these candidates against M PRO . Two top-ranking inhibitors were selected for mechanistic investigations—one with an activated ester warhead that has a piperazine core and the other with an acrylamide warhead. Specifically, we performed a detailed analysis of the free energetics of covalent inhibition by hybrid quantum mechanics/molecular mechanics simulations. Cleavage of a fragment of the non-structured protein (NSP) from the SARS-CoV-2 genome was also simulated for reference. Simulations show that both candidates form more stable enzyme-inhibitor (E-I) complexes than the chosen NSP. It was found that both the NSP fragment and the activated ester inhibitor react with CYS145 of M PRO in a concerted manner, whereas the acrylamide inhibitor follows a stepwise mechanism. Most importantly, the reversible reaction and the subsequent hydrolysis reaction from E-I complexes are less probable when compared to the reactions with an NSP fragment, showing promise for these candidates to be the base for efficient M PRO inhibitors.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2024

Saturation of Fishbone Instability by Self-Generated Zonal Flows in Tokamak Plasmas

Gyrokinetic simulations of the fishbone instability in DIII-D tokamak plasmas find that self-generated zonal flows can dominate the nonlinear saturation by preventing coherent structures from persisting or drifting in the energetic particle phase space when the mode frequency down-chirps. Results from the simulation with zonal flows agree quantitatively, for the first time, with experimental measurements of the fishbone saturation amplitude and energetic particle transport. Moreover, the fishbone-induced zonal flows are likely responsible for the formation of an internal transport barrier that was observed after fishbone bursts in this DIII-D experiment. Finally, gyrokinetic simulations of a related ITER baseline scenario show that the fishbone induces insignificant energetic particle redistribution and may enable high performance scenarios in ITER burning plasma experiments. Published by the American Physical Society 2024

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS1977

The record of solar and galactic radiations in the ancient lunar regolith and their implications for the early history of the sun and moon

The paper reviews research into the nature and history of the lunar environment, as recorded in rocks and core samples, performed by studying effects produced by the energetic nuclear particles constituting the solar wind, solar flares, and galactic cosmic rays. Results obtained with lunar rocks are discussed which suggest a remarkable constancy of the lunar environment at least over the last several million years. Analyses of lunar core samples are examined which indicate an apparent secular change in the N-15/N-14 ratio with time in solar-wind-related nitrogen, possibly due to greatly enhanced solar flare activity in the past. Lunar and meteoritic breccias are proposed as obvious candidates for extending the radiation record much further back in time, perhaps even close to the beginning of the solar system.

Grozaz, G.↗

NASA NTRS1978

Spontaneous synchrotron emission from a plasma with an energetic runaway electron tail

The emissivity of spontaneous synchrotron radiation is computed for a plasma consisting of a background thermal plasma in addition to an energetic runaway electron component. The analysis is performed for both the ordinary and extraordinary modes, for frequencies in the vicinity of the electron plasma frequency and the higher harmonics of the electron gyrofrequency, and for the case when the electron plasma frequency is approximately the same as or smaller than the cyclotron frequency. The relativistic gyroresonance with the runaway electrons is found to result in a level of spontaneous emission which, for frequencies in the neighborhood of the electron plasma frequency, is significantly enhanced over the thermal radiation.

Freund, H. P.↗

NASA NTRS1984

The energetics of hydrogen atom recombination - Analysis, experiments, and modeling

A theoretical investigation of the effect of the microscopic energetics of the recombination reaction on the performance of a microwave-plasma electrothermal propulsion system is described, and the results of the analysis are presented. A series of experiments to test the concept is described and analyzed by comparison with a computer model of the recombination reaction. It is concluded that internal energy considerations are not likely to significantly affect the design of a microwave-plasma electrothermal rocket. The experimental results indicate that the microwave power is far higher than the capacity of the gas to absorb it; the cooling needed to control the energy dominates the experimental results.

Filpus, J. W.↗

NASA NTRS2010

Helium vs. Proton Induced Displacement Damage in Electronic Materials

In this project, the specific effects of displacement damage due to the passage of protons and helium nuclei on some typical electronic materials will be evaluated and contrasted. As the electronic material absorbs the energetic proton and helium momentum, degradation of performance occurs, eventually leading to overall failure. Helium nuclei traveling at the same speed as protons are expected to impart more to the material displacement damage; due to the larger mass, and thus momentum, of helium nuclei compared to protons. Damage due to displacement of atoms in their crystalline structure can change the physical properties and hence performance of the electronic materials.

Ringo, Sawnese↗

DOE OSTI2022

Precise $\textit{Q}$-value measurements of 112,113 Ag and 115 Cd with the Canadian Penning trap for evaluation of potential ultralow $\textit{Q}$-value $\textit{β}$ decays

Background: An ultralow $\textit{Q}$-value $\textit{β}$ decay can occur from a parent nuclide to an excited nuclear state in the daughter such that $Q_{\text{UL}}$ 1 keV. These decay processes are of interest for nuclear $\textit{β}$-decay theory and as potential candidates in neutrino mass determination experiments. To date, only one ultralow $\textit{Q}$-value $\textit{β}$ decay has been observed—that of 115 In with $Q_β$ = 147(10) eV. A number of other potential candidates exist, but improved mass measurements are necessary to determine if these decay channels are energetically allowed and, in fact, ultralow. Purpose: To perform precise $\textit{β}$-decay $\textit{Q}$-value measurements of 112,113 Ag and 115 Cd and to use them in combination with nuclear energy level data for the daughter isotopes 112,113 Cd and 115 In to determine if the potential ultralow $\textit{Q}$-value $\textit{β}$-decay branches of 112,113 Ag and 115 Cd are energetically allowed and 1 keV. Method: The Canadian Penning Trap at Argonne National Laboratory was used to measure the cyclotron frequency ratios of singly charged 112,113 Ag and 115 Cd ions with respect to their daughters 112,113 Cd and 115 In. From these measurements, the ground-state to ground-state $\textit{β}$-decay $\textit{Q}$ values were obtained. Results: The 112 Ag → 112 Cd, 113 Ag → 113 Cd, and 115 Cd → 115 In $\textit{β}$-decay $\textit{Q}$ values were measured to be $Q_β$( 112 Ag) = 3990.16(22) keV, $Q_β$( 113 Ag) = 2085.7(4.6) keV, and $Q_β$( 115 Cd) = 1451.36(34) keV. These results were compared to energies of excited states in 112 Cd at 3997.75(14) keV, 113 Cd at 2015.6(2.5) and 2080(10) keV, and 115 In at 1448.787(9) keV, resulting in precise $Q_{\text{UL}}$ values for the potential decay channels of –7.59(26) keV, 6(11) keV, and 2.57(34) keV, respectively. Conclusion: The potential ultralow $\textit{Q}$-value decays of 112 Ag and 115 Cd have been ruled out. 113 Ag is still a possible candidate until a more precise measurement of the 2080(10) keV, 1/2+ state of 113 Cd is available. In the course of this work we have found the ground state mass of 113 Ag reported in the 2020 Atomic Mass Evaluation [Wang et al., Chin. Phys. C 45, 030003 (2021)] to be lower than our measurement by 69(17) keV (a 4σ discrepancy).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

3D modeling of the Staged Z-pinch with the FLASH code

The Staged Z-pinch (SZP) fusion concept is a magneto-inertial compression scheme developed by Magneto-Inertial Fusion Technologies, Inc. (MIFTI), in which small amounts of fusion fuel are brought to fusion-relevant conditions by passing multi-million amperes strong current through a cylindrical shell of high atomic number material. One- and two-dimensional modeling performed by MIFTI with the MACH2 code, suggests that net fusion energy gain can be achieved when currents in the 10 million amperes range compress a 50%-50% mixture of deuterium and tritium gas. In this project we enhance and use the FLASH code to execute high-fidelity, simulations of various SZP configurations, a collaboration between the Flash Center for Computational Science at the University of Rochester and the Laboratory for Laser Energetics, and MIFTI. FLASH is a high-performance computing, multi-physics, radiation magnetohydrodynamic (MHD) code with extended physics capabilities, which is developed at the Flash Center. The goal of this project is to assess the shell/fuel stability of the pinch to two- and three-dimensional MHD instabilities and to utilize FLASH’s extended physics capabilities to understand how extended-MHD effects impact implosion dynamics and plasma conditions at stagnation. The project is a natural extension of an ongoing collaborative effort between MIFTI and the Flash Center through the U.S. DOE Advanced Research Projects Agency-Energy (ARPA-E) BETHE program and can provide MIFTI with simulation capabilities that are currently beyond their reach with MACH2. Ultimately, MIFTI wants FLASH to become one of their simulation workhorses for reliable, high-fidelity SZP platform design. During the project, the Flash Center team developed a suite of in one- and two-dimensional FLASH simulations to model different variants of the SZP platform, performed code-to-code comparisons with MACH2, and used the FLASH code to design and model SZP experiments like the Double Eagle experiments that MIFTI recently performed. Also, the Flash Center team developed the capabilities of FLASH to be able to do three-dimensional simulations of pulsed-power experiments with the code for the first time. Two publications from this effort are currently under review and two more are in preparation. MIFTI has also committed to the use of FLASH for future SZP simulation efforts.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS2005

Energetic Metastable Oxygen and Nitrogen Atoms in the Terrestrial Atmosphere

This report summarizes our research performed under NASA Grant NAG5-11857. The three-year grant have been supported by the Geospace Sciences SR&T program. We have investigated the energetic metastable oxygen and nitrogen atoms in the terrestrial stratosphere, mesosphere and thermosphere. Hot atoms in the atmosphere are produced by solar radiation, the solar wind and various ionic reactions. Nascent hot atoms arise in ground and excited electronic states, and their translational energies are larger by two - three orders of magnitude than the thermal energies of the ambient gas. The relaxation kinetics of hot atoms determines the rate of atmospheric heating, the intensities of aeronomic reactions, and the rate of atom escape from the planet. Modeling of the non-Maxwellian energy distributions of metastable oxygen and nitrogen atoms have been focused on the determination of their impact on the energetics and chemistry of the terrestrial atmosphere between 25 and 250 km . At this altitudes, we have calculated the energy distribution functions of metastable O and N atoms and computed non-equilibrium rates of important aeronomic reactions, such as destruction of the water molecules by O(1D) atoms and production of highly excited nitric oxide molecules. In the upper atmosphere, the metastable O(lD) and N(2D) play important role in formation of the upward atomic fluxes. We have computed the upward fluxes of the metastable and ground state oxygen atoms in the upper atmosphere above 250 km. The accurate distributions of the metastable atoms have been evaluated for the day and night-time conditions.

Kharchenko, Vasili↗

DOE OSTI2025

Interfacial Properties of Gold and Cobalt Oxyhydroxide in Plasmon-Mediated Oxygen Evolution Reaction

Water electrolysis is one green approach of storing electrical energy within chemical bonds of the high-energy hydrogen gas (H2). The anodic reaction involved in the oxygen evolution reaction (OER) requires high kinetic overpotential on the overall rate of the process. Recently, plasmonic gold nanoparticles (Au NPs) have been added to enhance the charge transfer at the interface of the OER electrocatalysts and electrolyte under light illumination. However, mechanistic understanding of how Au NPs on the photo-assisted electrochemical process is still lacking. We applied a model system of plasmonic Au electrode and a cobalt (Co)-based OER electrocatalyst in alkaline electrolytes to investigate the plasmon-mediated OER process with (photo)electrochemical and spectroscopic studies. Our results demonstrated that the electrodeposited and surfactant-free plasmonic Au electrode could enhance the electrocatalytic performances of the Co-based electrocatalysts in the OER process with continuous visible and near infrared light illumination. Both the photothermal and energetic charge carriers were found to contribute to the enhanced OER performance based on the transient photocurrent studies, and the interfaces of Au and the Co-based electrocatalysts determined the enhancement mechanisms. The active phase of the cobalt based OER electrocatalyst at operating potentials was identified with electrochemical Raman measurements.

OER↗

NASA NTRS2017

Impact of Substorm Time O+ Outflow on Ring Current Enhancement

Energetic O+ ions (tens of keV) rapidly increase in the inner magnetosphere and contribute significantly to the ring current during substorms. Previously, two source regions of the energetic O+ ions have been proposed. The first one is the dayside polar region. Ions from the dayside polar region are transported to the lobe; then they are injected to the nightside plasma sheet during substorm expansion phase. The second one is the nightside aurora region. After the substorm onset, energetic O+ ions are extracted from the ionosphere with the auroral acceleration processes, and the O+ ions are directly supplied to the nightside plasma sheet. We investigated the relative importance of these two regions on supplying the energetic O+ ions in the inner magnetosphere. We performed a test particle simulation in global MHD electromagnetic fields. We obtained the following results. (1) During the substorm growth phase, O+ ions at tens of eV are extracted from the dayside polar region, resulting in the enhancement of the warm O+ ions (hundreds of eV) in the lobe. After the substorm onset, the warm O+ ions are nonadiabatically accelerated to tens of keV and injected to the inner magnetosphere. These O+ ions contribute to most of the O+ ring current. (2) O+ ions at less than a few keVs are supplied from the nightside aurora region to the plasma sheet. However, their contribution to the O+ ring current remains small. From the results, we concluded that the main source of the energetic O+ ions is the dayside polar region.

outflow↗

DOE OSTI2022

Towards performing high-resolution inelastic X-ray scattering measurements at hard X-ray free-electron lasers coupled with energetic laser drivers

High-resolution inelastic X-ray scattering is an established technique in the synchrotron community, used to investigate collective low-frequency responses of materials. When fielded at hard X-ray free-electron lasers (XFELs) and combined with high-intensity laser drivers, it becomes a promising technique for investigating matter at high temperatures and high pressures. This technique gives access to important thermodynamic properties of matter at extreme conditions, such as temperature, material sound speed, and viscosity. The successful realization of this method requires the acquisition of many identical laser-pump/X-ray-probe shots, allowing the collection of a sufficient number of photons necessary to perform quantitative analyses. Here, a 2.5-fold improvement in the energy resolution of the instrument relative to previous works at the Matter in Extreme Conditions (MEC) endstation, Linac Coherent Light Source (LCLS), and the High Energy Density (HED) instrument, European XFEL, is presented. Some aspects of the experimental design that are essential for improving the number of photons detected in each X-ray shot, making such measurements feasible, are discussed. A careful choice of the energy resolution, the X-ray beam mode provided by the XFEL, and the position of the analysers used in such experiments can provide a more than ten-fold improvement in the photometrics. The discussion is supported by experimental data on 10 µm-thick iron and 50 nm-thick gold samples collected at the MEC endstation at the LCLS, and by complementary ray-tracing simulations coupled with thermal diffuse scattering calculations.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Local Structural Coherence and Interfacial Charge Transfer in Cu 2 ⁢S/Mo⁢S 2 Heterostructure

Precise control over electronic coupling at nanoscale interfaces is critical for designing materials with tunable charge-transfer behavior and catalytic function. Heterostructures with locally coherent interfaces provide a platform for interrogating interfacial charge redistribution in coupled material systems. Here, we report Cu 2 ⁢S/Mo⁢S 2 heterostructures exhibiting nanoscale crystallographic alignment, which are synthesized through a rapid thermal transformation pathway. We employed electrochemical reduction reactions to probe interfacial charge transfer, revealing shifts in product distribution attributable to modified interfacial energetics, even in the absence of optimized catalytic performance. The observed formate Faradaic efficiency suggests that interfacial electronic modulation in the heterostructure shifts product selectivity towards formate, highlighting how interface-driven electronic modulation can direct reaction pathways and influence product selectivity. Optimizing catalyst loading, architecture, and reactor configuration will be critical for future improvement. Structural and compositional integrity were confirmed through powder x-ray diffraction, x-ray photoelectron spectroscopy, and high-resolution transmission electron microscopy. Electron transfer between Cu 2 ⁢S and Mo⁢S 2 domains was further evaluated by electrochemical impedance spectroscopy, while selected-area electron diffraction revealed local crystallographic alignment consistent with a local epitaxial relationship at the Cu 2 S/Mo⁢S 2 heterointerface. To illustrate the broader applicability of this approach, a Zn⁢S/Mo⁢S 2 heterostructure was also synthesized using the same microwave strategy, confirming the generalizability of interfacial engineering principles across metal sulfide-Mo⁢S 2 systems. Collectively, these findings demonstrate that controlled local epitaxial alignment serves as an effective design principle for tuning interfacial energetics and catalytic reactivity in complex heterostructure materials.

carbon capture & utilization↗

DOE OSTI2023

High-throughput calculations of charged point defect properties with semi-local density functional theory—performance benchmarks for materials screening applications

Abstract Calculations of point defect energetics with Density Functional Theory (DFT) can provide valuable insight into several optoelectronic, thermodynamic, and kinetic properties. These calculations commonly use methods ranging from semi-local functionals with a-posteriori corrections to more computationally intensive hybrid functional approaches. For applications of DFT-based high-throughput computation for data-driven materials discovery, point defect properties are of interest, yet are currently excluded from available materials databases. This work presents a benchmark analysis of automated, semi-local point defect calculations with a-posteriori corrections, compared to 245 “gold standard” hybrid calculations previously published. We consider three different a-posteriori correction sets implemented in an automated workflow, and evaluate the qualitative and quantitative differences among four different categories of defect information: thermodynamic transition levels, formation energies, Fermi levels, and dopability limits. We highlight qualitative information that can be extracted from high-throughput calculations based on semi-local DFT methods, while also demonstrating the limits of quantitative accuracy.

36 MATERIALS SCIENCE↗

NASA NTRS2013

Properties and Performance Attributes of Novel Co-extruded Polyolefin Battery Separator Materials: Electrical Properties - Part 2

As NASA prepares for its next era of manned spaceflight missions, advanced energy storage technologies are being developed and evaluated to address and enhance future mission needs and technical requirements. Cell-level components for advanced lithium-ion batteries possessing higher energy, more reliable performance and enhanced, inherent safety characteristics have been under development within the NASA infrastructure. A key component for safe and reliable cell performance is the cell separator, which separates the two energetic electrodes and functions to inhibit the occurrence of an internal short circuit but preserves an ionic current. Recently, a new generation of co-extruded separator films has been developed by ExxonMobil Chemical and introduced into their battery separator product portfolio. Several grades of this new separator material were evaluated with respect to dynamic mechanical properties and safety-related performance attributes, and the results of these evaluations were previously reported in "Part 1: Mechanical Properties" of this publication. This current paper presents safety-related performance results for these novel materials obtained by employing a complementary experimental methodology, which involved the analysis of separator impedance characteristics as a function of temperature. The experimental results from this study are discussed with respect to potential cell safety enhancement for future aerospace as well as for terrestrial energy storage needs, and they are compared with pertinent mechanical properties of these materials, as well as with current state-of-the practice separator materials.

Baldwin, Richard S.↗

NASA NTRS2011

Properties and Performance Attributes of Novel Co-Extruded Polyolefin Battery Separator Materials: Mechanical Properties - Part 1

As NASA prepares for its next era of manned spaceflight missions, advanced energy storage technologies are being developed and evaluated to address future mission needs and technical requirements and to provide new mission-enabling technologies. Cell-level components for advanced lithium-ion batteries possessing higher energy, more reliable performance and enhanced, inherent safety characteristics are actively under development within the NASA infrastructure. A key component for safe and reliable cell performance is the cell separator, which separates the two energetic electrodes and functions to prevent the occurrence of an internal short-circuit while enabling ionic transport. Recently, a new generation of co-extruded separator films has been developed by ExxonMobil Chemical and introduced into their battery separator product portfolio. Several grades of this new separator material have been evaluated with respect to dynamic mechanical properties and safety-related performance attributes. This paper presents the results of these evaluations in comparison to a current state-ofthe-practice separator material. The results are discussed with respect to potential opportunities to enhance the inherent safety characteristics and reliability of future, advanced lithium-ion cell chemistries.

Baldwin, Richard S.↗