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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 595 records · Page 33
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Activation of methane by U + studied by guided ion beam tandem mass spectrometry and quantum chemistry

Reaction pathways of all products formed in the U + + CH 4 (CD 4 ) reaction were explored as a function of kinetic energy using guided ion beam tandem mass spectrometry and quantum chemical calculations. UH + , UC + , UCH + , UCH 2 + , and UCH 3 + (and their perdeuterated analogues) are formed in endothermic reactions. In both systems, the UCH 2 + (UCD 2 + ) dehydrogenated product was the dominant product in the low-energy region, whereas the UH + (UD + ) hydride product became predominant at high energies. The kinetic energy behavior of the various products is consistent with a common intermediate of H–U + –CH 3 (D–U + –CD 3 ). Here, the kinetic energy dependence of all product cross sections was modeled to obtain experimental bond dissociation energies at 0 K (in eV): D 0 (U + –H) = 2.42 ± 0.10, D 0 (U + –C) = 3.95 ± 0.12, D 0 (U + –CH) = 4.91 ± 0.09, D 0 (U + –CH 2 ) = 4.11 ± 0.04, and D 0 (U + –CH 3 ) = 2.41 ± 0.09. Quantum chemical calculations using the UCCSD(T) and UB3LYP approaches with the cc-pwCVXZ-PP basis set with MDF-60 pseudopotential for U + and the aug-cc-pCVXZ and aug-cc-pVXZ (X = T, Q) basis set for carbon and hydrogen, respectively, validate the experimental bond dissociation energies and outline the potential energy surface for all reactions observed. In addition, spin–orbit corrections of the bond energies for all products were calculated at a CASSCF-CASPT2-RASSI level.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Localized Active Space Pair-Density Functional Theory

Accurate quantum chemical methods for the prediction of spin-state energy gaps for strongly correlated systems are computationally expensive and scale poorly with the size of the system. This makes calculations for many experimentally interesting molecules impractical even with abundant computational resources. Previous work has shown that the localized active space (LAS) self-consistent field (SCF) method can be an efficient way to obtain multiconfiguration SCF wave functions of comparable quality to the corresponding complete active space (CAS) ones. To obtain quantitative results, a post-SCF method is needed to estimate the complete correlation energy. One such method is multiconfiguration pair-density functional theory (PDFT), which calculates the energy based on the density and on-top pair density obtained from a multiconfiguration wave function. In this work, we introduce localized-active-space PDFT, which uses a LAS wave function for subsequent PDFT calculations. The method is tested by computing spin-state energies and gaps in conjugated organic molecules and a bimetallic compound and comparing to the corresponding CAS-PDFT values.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Consequences and Control of Multiscale Order/Disorder in Chiral Magnetic Textures

Transition metal intercalated transition metal dichalcogenides (TMDs) are promising platforms for next-generation spintronic devices based on their wide range of electronic and magnetic phases, which can be tuned by varying the host lattice or intercalant’s identity, stoichiometry, or spatial order. Some of these compounds host a chiral magnetic phase in which the helical winding of magnetic moments propagates along a high-symmetry crystalline axis. Previous studies have demonstrated that variation in intercalant concentrations can have a dramatic effect on the formation of chiral domains and ensemble magnetic properties. However, a systematic and comprehensive study of how atomic-scale order and disorder impact these chiral magnetic textures is so far lacking. Here, we leverage a combination of imaging modes in the (scanning) transmission electron microscope (S/TEM) to directly probe (dis)order across multiple length scales and show how subtle changes in the atomic lattice can tune the mesoscale spin textures and bulk magnetic response in Cr 1/3 NbS 2 , with direct implications for the fundamental understanding and technological implementation of such compounds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Ferromagnetism out of charge fluctuation of strongly correlated electrons in κ -(BEDT-TTF) 2 Hg(SCN) 2 Br

We perform magnetic susceptibility and magnetic torque measurements on the organic κ-(BEDT-TTF) 2 Hg(SCN) 2 Br, which is recently suggested to host an exotic quantum dipole-liquid in its low-temperature insulating phase. Below the metal-insulator (MI) transition temperature, the magnetic susceptibility follows a Curie–Weiss law with a positive Curie–Weiss temperature, and a particular M∝ $\sqrt{H}$ curve is observed. The emergent ferromagnetically interacting spins amount to about 1/6 of the full spin moment of localized charges. Taking account of the possible inhomogeneous quasi-charge-order that forms a dipole-liquid, we construct a model of antiferromagnetically interacting spin chains in two adjacent charge-ordered domains, which are coupled via fluctuating charges on a Mott-dimer at the boundary. We find that the charge fluctuations can draw a weak ferromagnetic moment out of the spin singlet domains.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Adsorption of a single Pt atom on graphene: spin crossing between physisorbed triplet and chemisorbed singlet states

Diffusion Monte Carlo (DMC) calculations have been performed to study the adsorption of a single Pt atom on pristine graphene. In this work, we obtain the adsorption energy curves of a single Pt atom adsorbed at three different adsorption sites (bridge, on-top, hollow) as functions of the vertical distance from a graphene surface for both spin singlet and triplet states. The bridge-site adsorption in a singlet spin state is found to be energetically most stable, which is consistent with previous theoretical predictions. As the Pt atom moves away from a graphene surface, spin triplet states are favored over spin singlet states for all three adsorption sites, reflecting that the ground state of an isolated Pt atom is in a spin triplet state. Furthermore, our DMC calculations reveal local-minimum features in the triplet region which is understood to be due to van der Waals interaction between the Pt atom and graphene. This provides a comprehensive understanding for a spin crossing from a physisorbed triplet state to a chemisorbed singlet state in the adsorption process of a single Pt atom on graphene.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Simulations of x-ray absorption spectra for CO desorbing from Ru(0001) with transition-potential and time-dependent density functional theory approaches

The desorption of a carbon monoxide molecule from a Ru(0001) surface was studied by means of X-ray Absorption Spectra (XAS) computed with Transition Potential (TP-DFT) and Time Dependent (TD-DFT) DFT methods. By unraveling the evolution of the CO electronic structure upon desorption, we observed that at 2.3 Å from the surface, the CO molecule has already predominantly gas-phase character. While C 1s XAS is quite insensitive to changes in the C–O bond length, the O 1s excitation is very sensitive with the π* coming down in energy upon CO bond stretching, which competes with the increase in orbital energy due to the repulsive interaction with the metallic surface. We show in a systematic way that the TP-DFT method can describe the XAS rather well at the endpoints (chemisorbed and gas phase) but is affected by artificial charge transfer and/or incorrect spin treatment in the transition region in cases like CO, where there are low-lying π* orbitals and large exchange interactions between the core 1s and valence-acceptor π* orbitals. As an alternative, we demonstrate by comparing with experimental data that a linear response approach using TD-DFT employing common exchange-correlation functionals and finite-size clusters can yield a good description of the spectral evolution of the 1s → π* transition with correct spin and gas-to-chemisorbed chemical shifts in good agreement with experiment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Electronic and Spintronic Open-Shell Macromolecules, Quo Vadis ?

Open-shell macromolecules (i.e., polymers containing radical sites either along their backbones or at the pendant sites of repeat units) have attracted significant attention owing to their intriguing chemical and physical (e.g., redox, optoelectronic, and magnetic) properties, and they have been proposed and/or implemented in a wide range of potential applications (e.g., energy storage devices, electronic systems, and spintronic modules). These successes span multiple disciplines that range from advanced macromolecular chemistry through nanoscale structural characterization and on to next-generation solid-state physics and the associated devices. In turn, this has allowed different scientific communities to expand the palette of radical-containing polymers relatively quickly. However, critical gaps remain on many fronts, especially regarding the elucidation of key structure–property–function relationships that govern the underlying electrochemical, optoelectronic, and spin phenomena in these materials systems. Here, we highlight vital developments in the history of open-shell macromolecules to explain the current state of the art in the field. Moreover, we provide a critical review of the successes and bring forward open opportunities that, if solved, could propel this class of materials in a meaningful manner. Finally, we provide an outlook to address where it seems most likely that open-shell macromolecules will go in the coming years. Furthermore, our considered view is that the future of radical-containing polymers is extremely bright and the addition of talented researchers with diverse skills to the field will allow these materials and their end-use devices to have a positive impact on the global science and technology enterprise in a relatively rapid manner.

36 MATERIALS SCIENCE↗
DOE OSTI2023

2022 American Conference on Neutron Scattering (ACNS 2022)

The 11th American Conference on Neutron Scattering (ACNS 2022) will be held on June 5-9, 2022, in Boulder, CO. The Conference will provide essential information on the breadth and depth of current neutron-related research worldwide. Hosted by the Neutron Scattering Society of America, this year’s Conference will feature a combination of invited and contributed talks, poster sessions, and tutorials. Topics of the conference are: Advances in Neutron Facilities, Instrumentation and Software: Developments in sources, instrumentation, sample environments and control software. Hard Condensed Matter: Magnetism, correlated metals, quantum/topological materials, superconductors, ferroelectrics, multiferroics, glasses, and disorder phenomena. Submissions outlining examples of neutron scattering in industrial and engineering applications involving hard condensed matter systems are also encouraged. Soft Matter: Neutron studies of soft materials and related fields including in situ and in operando studies. Polymers, surfactants, emulsions, gels, nanoparticles, colloidal suspensions and more. Submissions of computational studies or applications of machine learning beneficial to neutron scattering experiments, as well as examples of neutron scattering in industrial and engineering applications are strongly encouraged. Biology, Biophysics and Biotechnology: Neutron studies of biological and biologically relevant systems. Proteins, bio membranes, biological assemblies, natural materials, nucleic acids, drug-delivery platforms and biomedical systems. Submissions of computational studies or applications of machine learning beneficial to biological neutron scattering experiments, as well as examples of neutron scattering in applied research involving biological systems, are strongly encouraged. Materials Chemistry and Energy: Neutron-based studies of functional materials and materials for energy applications. Examples include porous materials such as metal organic frameworks (MOFs), zeolites; phosphors; novel pigments; electrolytes; catalysts; ionic conductors/cathode materials; photovoltaic materials (hybrid perovskites); thermoelectrics; magnetocalorics/electrocalorics. Structural Materials and Engineering: Neutron scattering studies of materials and engineering processes including structural materials, concrete and metals, as well as engineering processes including combustion, corrosion, additive manufacturing, and others. Neutron Physics: Fundamental physical studies of the neutron and related areas. Emerging Applications in Neutron Scattering: Machine Learning and Data Science: Advances in computing power have contributed to rapidly evolving machine learning and data science fields that can be leveraged to the benefit of the neutron scattering community. The purpose of this session is to highlight recent advances in machine learning and data science and to serve as the foundation of a parallel data and computation track highlighting computation advances and applications in neutron scattering throughout the conference.

36 MATERIALS SCIENCE↗
NASA NTRS1979

The impact of gas-surface reactions on mass spectrometric measurements of atomic nitrogen

The paper presents a simplified model of the ion source chemistry, explains several details of the data reduction method used in obtaining atomic-nitrogen (N) densities from OSS data, and discusses implications of gas-surface reactions for the design of future satellite-borne mass spectrometers. Because of various surface reactions, N appears in three different forms in the ion source, as N, NO, and NO2. Considering the rather small spin modulation of NO and NO2 in the semi-open ionization chamber used in the OSS instrument, it is not surprising that these reaction products have not been previously identified in closed source instruments as a measure of the presence of atomic nitrogen. Warmup and/or outgassing of the ion source are shown to drastically reduce the NO2 concentration, thereby making possible reliable measurement of ambient N densities.

Engebretson, M. J.↗
NASA NTRS2011

Messengers from the Early Solar System - Comets as Carriers of Cosmic Information

Viewed from a cosmic perspective, Earth is a dry planet yet its oceans are enriched in deuterium by a large factor relative to nebular hydrogen. Can comets have delivered Earth s water? The question of exogenous delivery of water and organics to Earth and other young planets is of critical importance for understanding the origin of Earth s water, and for assessing the possible existence of exo-planets similar to Earth. Strong gradients in temperature and chemistry in the proto-planetary disk, coupled with dynamical models, imply that comets from the Oort Cloud and Kuiper Disk reservoirs should have diverse composition. The primary volatiles in comets (ices native to the nucleus) provide the preferred metric, and taxonomies based on them are now beginning to emerge [1, 2, 3]. The measurement of cosmic parameters such as the nuclear spin temperatures for H2O, NH3, and CH4, and of enrichment factors for isotopologues (D/H in water and hydrogen cyanide, N-14/N-15 in CN and hydrogen cyanide) provide additional important tests for the origin of cometary material.

Mumma, Michael J.↗
NASA NTRS2012

Messengers from the Early Solar System - The Similarity and Diversity of Comets

Viewed from a cosmic perspective, Earth is a dry planet yet its oceans are enriched in deuterium by a large factor relative to nebular hydrogen. Can comets have delivered Earth's water? The question of exogenous delivery of water and organics to Earth and other young planets is of critical importance for understanding the origin of Earth's water, and for assessing the possible existence of exo-planets similar to Earth. Strong gradients in temperature and chemistry in the proto-planetary disk, coupled with dynamical models, imply that comets from the Oort Cloud and Kuiper Disk reservoirs should have diverse composition. The primary volatiles in comets (ices native to the nucleus) provide the preferred metric, and taxonomies based on them are now beginning to emerge [1,2,3]. The measurement of cosmic parameters such as the nuclear spin temperatures for H2O, NH3, and CH4, and of enrichment factors for isotopologues (D/H in water and hydrogen cyanide, N-14/N-15 in CN and hydrogen cyanide provide additional important tests for the origin of cometary material. I will provide an overview of these aspects, and their implications for the origin of Earth's water and prebiotic organics.

Mumma, Michael J.↗
NASA NTRSDate not supplied

Dragonfly Preparation for Powered Flight: Lander Separation State Control to Ensure Successful Landing

NASA’s Dragonfly mission, led by The Johns Hopkins University Applied Physics Laboratory, is a relocatable octocopter lander to study Saturn’s largest moon Titan. The scientific goals of the mission include studying Titan’s prebiotic chemistry, geology, and atmosphere. Upon Titan arrival, the lander will enter the atmosphere, descend on a parachute to a ground-relative altitude of about 1000 m before being released, and then fly on internal power down to the surface. To guarantee desirable initial conditions for the lander release, the lander must meet certain angular rate conditions. These conditions include reducing the spin rate about the vertical axis to 4.9 deg/sec, using the rotors as actuators; and releasing with a negative pitch rate (rotating nose down) to ensure a successful transition to powered flight. This is achieved using a release trigger. Achieving these desired rates for lander release is part of the mission phase known as ‘preparation for powered flight’ (PPF). This paper proposes controls and logic to achieve the desired conditions for releasing the lander from the parachute.

Flight Mechanics↗
NASA NTRSDate not supplied

Dragonfly Preparation for Powered Flight: Lander Separation State Control to Ensure Successful Landing

NASA’s Dragonfly mission, led by The Johns Hopkins University Applied Physics Laboratory, is a relocatable octocopter lander to study Saturn’s largest moon Titan. The scientific goals of the mission include studying Titan’s prebiotic chemistry, geology, and atmosphere. Upon Titan arrival, the lander will enter the atmosphere, descend on a parachute to a ground-relative altitude of about 1000 m before being released, and then fly on internal power down to the surface. To guarantee desirable initial conditions for the lander release, the lander must meet certain angular rate conditions. These conditions include reducing the spin rate about the vertical axis to 4.9 deg/sec, using the rotors as actuators; and releasing with a negative pitch rate (rotating nose down) to ensure a successful transition to powered flight. This is achieved using a release trigger. Achieving these desired rates for lander release is part of the mission phase known as ‘preparation for powered flight’ (PPF). This paper proposes controls and logic to achieve the desired conditions for releasing the lander from the parachute.

Flight Mechanics↗
DOE OSTI2022

Analysis of spin frustration in an Fe III 7 cluster using a combination of computational, experimental, and magnetostructural correlation methods

The synthesis, structure, and magnetic properties are reported for [Fe 7 O 3 (O 2 C t Bu) 9 (mda) 3 (H 2 O) 3 ] ( 1 ), where mdaH 2 is N -methyldiethanolamine. 1 was prepared from the reaction of [Fe 3 O(O 2 C t Bu) 6 (H 2 O) 3 ](NO 3 ) with mdaH 2 in a 1:~3 ratio in MeCN. The core of 1 consists of a central octahedral Fe III ion held within a non-planar Fe 6 loop by three μ 3 -O 2- and three μ 2 -RO - arms from the three mda 2- chelates. Variable-temperature dc and ac magnetic susceptibility studies revealed dominant antiferromagnetic coupling, leading to a ground state spin of S = 5 / 2 . The ground state was confirmed by a fit of magnetization data collected in the 0.1–7.0 T and 1.8–10.0 K ranges. The four Fe 2 pairwise exchange parameters ( J 1 - J 4 ) were estimated by independent methods: theoretical calculations using either broken symmetry energy differences (-46.3, -16.2, -3.9, and - 28.1 cm -1 , respectively) or Green’s function approximation methods (-41.4, -14.8, -13.2, and - 24.7 cm -1 ), and a magnetostructural correlation (MSC) previously developed for high nuclearity Fe III /O complexes (-39.5, -13.8, -6.7, and - 23.5 cm -1 ). Additionally, the J 1 - J 4 obtained from the MSC and theoretical methods were used with the program PHI to both simulate χ M T vs T as well as to serve as reasonable input values to fit the experimental data (-41.0, -11.4, -5.0, and - 27.3 cm -1 ). Analysis of the J ij led to identification of the spin frustration effects operative and the resultant spin vector alignments at each Fe III ion, thus allowing for the rationalization of the experimental ground state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Spin and Orbital Effects on Asymmetric Exchange Interaction in Polar Magnets: M(IO 3 ) 2 (M = Cu and Mn)

We report magnetic polar materials feature an astonishing range of physical properties, such as magnetoelectric coupling, chiral spin textures, and related new spin topology physics. This is primarily attributable to their lack of space inversion symmetry in conjunction with unpaired electrons, potentially facilitating an asymmetric Dzyaloshinskii–Moriya (DM) exchange interaction supported by spin–orbital and electron–lattice coupling. However, engineering the appropriate ensemble of coupled degrees of freedom necessary for enhanced DM exchange has remained elusive for polar magnets. Here, we study how spin and orbital components influence the capability of promoting the magnetic interaction by studying two magnetic polar materials, α-Cu(IO 3 ) 2 ( 2 D) and Mn(IO 3 ) 2 ( 6 S), and connecting their electronic and magnetic properties with their structures. The chemically controlled low-temperature synthesis of these complexes resulted in pure polycrystalline samples, providing a viable pathway to prepare bulk forms of transition-metal iodates. Rietveld refinements of the powder synchrotron X-ray diffraction data reveal that these materials exhibit different crystal structures but crystallize in the same polar and chiral P2 1 space group, giving rise to an electric polarization along the b-axis direction. The presence and absence of an evident phase transition to a possible topologically distinct state observed in α-Cu(IO 3 ) 2 and Mn(IO 3 ) 2 , respectively, imply the important role of spin–orbit coupling. Neutron diffraction experiments reveal helpful insights into the magnetic ground state of these materials. While the long-wavelength incommensurability of α-Cu(IO 3 ) 2 is in harmony with sizable asymmetric DM interaction and low dimensionality of the electronic structure, the commensurate stripe AFM ground state of Mn(IO 3 ) 2 is attributed to negligible DM exchange and isotropic orbital overlapping. The work demonstrates connections between combined spin and orbital effects, magnetic coupling dimensionality, and DM exchange, providing a worthwhile approach for tuning asymmetric interaction, which promotes evolution of topologically distinct spin phases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

“Magic” Orientation Angles to Suppress Spin-Driven Hall Currents in Anisotropic 2D Materials with an Ideal Skyrmion Gas

The Hall effect depending on conduction electron spin projection becomes very different for anisotropic 2D crystals. In this case the spin-dependent electron current strongly determined by the orientation angle, θ, of the sample with respect to an applied electric eld. The spin-up and -down components of the direct and Hall charge currents oscillate with the angle 2θ. The direct and Hall components of the current have the structure where there are the angle-independent part, oscillation amplitude, and phase shift. All three quantitates strongly depend on the electron spin projection, electron mass ratio, and skyrmion size. We nd that there are "magic" orientation angles where the spin-up, spin-down, and total Hall currents vanish. There is a great interest in computations based on 2D materials with skyrmions. Such properties can be useful for computer logic operations based on skyrmions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗