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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 415 records · Page 23
All sourcesNASA NTRSDOE OSTI
NASA NTRS1973

Measured catalycities of various candidate space shuttle thermal protection system coatings at low temperatures

Atom recombination catalytic rates for surface coatings of various candidate thermal protection system materials for the space shuttle vehicle were obtained from measurements in arc jet, air flow. The coatings, chrome oxides, siliconized carbon/carbon, hafnium/tantalum carbide on carbon/carbon, and niobium silicide, were bonded to the sensitive surface of transient slug calorimeters that measured the heat transfer rates to the coatings. The catalytic rates were inferred from these heat transfer rates Surface temperatures of the calorimeters varied from approximately 300 to 410 K.

Scott, C. D.↗
NASA NTRS1976

Energy storage possibilities of atomic hydrogen

Several recent experiments designed to produce and store macroscopic quantities of atomic hydrogen are discussed. The bulk, ground state properties of atomic hydrogen, deuterium, and tritium systems are calculated assuming that all pair interactions occur via the atomic triplet potential. The conditions required to obtain this system, including inhibition of recombination through the energetically favorable singlet interaction, are discussed. The internal energy, pressure, and compressibility are calculated applying the Monte Carlo technique with a quantum mechanical variational wavefunction. The system studied consisted of 32 atoms in a box with periodic boundary conditions. Results show that atomic triplet hydrogen and deuterium remain gaseous at 0 K; i.e., the internal energy is positive at all molar volumes considered.

Etters, R. D.↗
DOE OSTI2021

Three-state harmonic models for photoinduced charge transfer

A widely used strategy for simulating the charge transfer between donor and acceptor electronic states in an all-atom anharmonic condensedphase system is based on invoking linear response theory to describe the system in terms of an effective spin-boson model Hamiltonian. Extending this strategy to photoinduced charge transfer processes requires also taking into consideration the ground electronic state in addition to the excited donor and acceptor electronic states. In this paper, we revisit the problem of describing such nonequilibrium processes in terms of an effective three-state harmonic model. We do so within the framework of nonequilibrium Fermi’s golden rule (NE-FGR) in the context of photoinduced charge transfer in the carotenoid–porphyrin–C 60 (CPC 60 ) molecular triad dissolved in explicit tetrahydrofuran (THF). To this end, we consider different ways for obtaining a three-state harmonic model from the equilibrium autocorrelation functions of the donor–acceptor, donor–ground, and acceptor–ground energy gaps, as obtained from all-atom molecular dynamics simulations of the CPC 60 /THF system. The quantum-mechanically exact time-dependent NE-FGR rate coefficients for two different charge transfer processes in two different triad conformations are then calculated using the effective three-state model Hamiltonians as well as a hierarchy of more approximate expressions that lead to the instantaneous Marcus theory limit. Our results show that the photoinduced charge transfer in CPC 60 /THF can be described accurately by the effective harmonic three-state models and that nuclear quantum effects are small in this system.

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

Towards Quantum-Chemical Level Calculations of SARS-CoV-2 Spike Protein Variants of Concern by First Principles Density Functional Theory

The spike protein (S-protein) is a crucial part of the severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), with its many domains responsible for binding, fusion, and host cell entry. In this review we use the density functional theory (DFT) calculations to analyze the atomic-scale interactions and investigate the consequences of mutations in S-protein domains. We specifically describe the key amino acids and functions of each domain, which are essential for structural stability as well as recognition and fusion processes with the host cell; in addition, we speculate on how mutations affect these properties. Such unprecedented large-scale ab initio calculations, with up to 5000 atoms in the system, are based on the novel concept of amino acid–amino acid-bond pair unit (AABPU) that allows for an alternative description of proteins, providing valuable information on partial charge, interatomic bonding and hydrogen bond (HB) formation. In general, our results show that the S-protein mutations for different variants foster an increased positive partial charge, alter the interatomic interactions, and disrupt the HB networks. We conclude by outlining a roadmap for future computational research of biomolecular virus-related systems.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2024

Molecular NMR shieldings, J -couplings, and magnetizabilities from numeric atom-centered orbital based density-functional calculations

This paper reports and benchmarks a new implementation of nuclear magnetic resonance shieldings, magnetizabilities, and J-couplings for molecules within semilocal density functional theory, based on numeric atom-centered orbital (NAO) basis sets. NAO basis sets are attractive for the calculation of these nuclear magnetic resonance (NMR) parameters because NAOs provide accurate atomic orbital representations especially near the nucleus, enabling high-quality results at modest computational cost. Moreover, NAOs are readily adaptable for linear scaling methods, enabling efficient calculations of large systems. Here, the paper has five main parts: (1) It reviews the formalism of density functional calculations of NMR parameters in one comprehensive text to make the mathematical background available in a self-contained way. (2) The paper quantifies the attainable precision of NAO basis sets for shieldings in comparison to specialized Gaussian basis sets, showing similar performance for similar basis set size. (3) The paper quantifies the precision of calculated magnetizabilities, where the NAO basis sets appear to outperform several established Gaussian basis sets of similar size. (4) The paper quantifies the precision of computed J-couplings, for which a group of customized NAO basis sets achieves precision of ~Hz for smaller basis set sizes than some established Gaussian basis sets. (5) The paper demonstrates that the implementation is applicable to systems beyond 1000 atoms in size.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS1987

Neutral atomic oxygen beam produced by ion charge exchange for Low Earth Orbital (LEO) simulation

A low energy neutral atomic oxygen beam system was designed and is currently being assembled at the Lewis Research Center. The system utilizes a 15 cm diameter Kaufman ion source to produce positive oxygen ions which are charge exchange neutralized to produce low energy (variable from 5 to 150 eV) oxygen atoms at a flux simulating real time low Earth orbital conditions. An electromagnet is used to direct only the singly charged oxygen ions from the ion source into the charge exchange cell. A retarding potential grid is used to slow down the oxygen ions to desired energies prior to their charge exchange. Cryogenically cooled diatomic oxygen gas in the charge exchange cell is then used to transfer charge to the oxygen ions to produce a neutral atomic oxygen beam. Remaining non-charge exchanged oxygen ions are then swept from the beam by electromagnetic or electrostatic deflection depending upon the desired experiment configuration. The resulting neutral oxygen beam of 5 to 10 cm in diameter impinges upon target materials within a sample holder fixture that can also provide for simultaneous heating and UV exposure during the atomic oxygen bombardment.

Banks, Bruce↗
DOE OSTI2023

Revealing the strength of three-nucleon interactions with the proposed Einstein Telescope

Nuclear systems, ranging from atomic nuclei to dense matter probed in neutron stars, are governed by strong interactions. Three-nucleon forces have been found to be a crucial ingredient for the reliable description of these systems. Here, in this work, we explore how astrophysical data on neutron stars and their mergers from current and next-generation observatories will enable us to distinguish nuclear Hamiltonians. In particular, we investigate two different nuclear Hamiltonians that have been adjusted to reproduce two-nucleon scattering data and properties of light nuclei, but differ in the three-nucleon interactions among neutrons. We find that no significant constraints can be obtained from current data, but that the proposed Einstein Telescope could provide strong evidence to distinguish among these Hamiltonians.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Hybrid Basis and Multi-Center Grid Method for Strong-Field Processes

We present a time-dependent framework that combines a hybrid basis, consisting of Gaussian-type orbitals (GTOs) and finite-element discrete-variable representation (FEDVR) functions, with a multicenter grid to simulate strong-field and attosecond dynamics in atoms and molecules. The method incorporates the construction of the orthonormal hybrid basis, the evaluation of electronic integrals, a unitary time-propagation scheme, and the extraction of optical and photoelectron observables. Its accuracy and robustness are benchmarked on one-electron systems such as atomic hydrogen and the dihydrogen cation (H$^+_2$) through comparisons with essentially-exact reference results for bound-state energies, high-harmonic generation spectra, photoionization cross sections, and photoelectron momentum distributions. This work establishes the groundwork for its integration with quantum-chemistry methods, which is already operational but will be detailed in future work, thereby enabling ab initio simulations of correlated polyatomic systems in intense ultrafast laser fields.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Effective optimization of atomic decoration in giant and superstructurally ordered crystals with machine learning

Crystals with complicated geometry are often observed with mixed chemical occupancy among Wyckoff sites, presenting a unique challenge for accurate atomic modeling. Similar systems possessing exact occupancy on all the sites can exhibit superstructural ordering, dramatically inflating the unit cell size. In this work, a crystal graph convolutional neural network (CGCNN) is used to predict optimal atomic decorations on fixed crystalline geometries. This is achieved with a site permutation search (SPS) optimization algorithm based on Monte Carlo moves combined with simulated annealing and basin-hopping techniques. Our approach relies on the evidence that, for a given chemical composition, a CGCNN estimates the correct energetic ordering of different atomic decorations, as predicted by electronic structure calculations. This provides a suitable energy landscape that can be optimized according to site occupation, allowing the prediction of chemical decoration in crystals exhibiting mixed or disordered occupancy, or superstructural ordering. Verification of the procedure is carried out on several known compounds, including the superstructurally ordered clathrate compound Rb8Ga27Sb16 and vacancy-ordered perovskite Cs2SnI6, neither of which was previously seen during the neural network training. In addition, the critical temperature of an order–disorder phase transition in solid solution CuZn is probed with our SPS routines by sampling site configuration trajectories in the canonical ensemble. This strategy provides an accurate method for determining favorable decoration in complex crystals and analyzing site occupation at unprecedented speed and scale.

Chemistry↗
DOE OSTI2022

Finite-Size Scaling on a Digital Quantum Simulator Using Quantum Restricted Boltzmann Machine

The critical point and the critical exponents for a phase transition can be determined using the Finite-Size Scaling (FSS) analysis. This method assumes that the phase transition occurs only in the infinite size limit. However, there has been a lot of interest recently in quantum phase transitions occurring in finite size systems such as a single two-level system interacting with a single bosonic mode e.g., in the Quantum Rabi Model (QRM). Since these phase transitions occur at a finite system size, the traditional FSS method is rendered inapplicable for these cases. For cases like this, we propose an alternative FSS method in which the truncation of the system is done in the Hilbert space instead of the physical space. This approach has previously been used to calculate the critical parameters for stability and symmetry breaking of electronic structure configurations of atomic and molecular systems. We calculate the critical point for the quantum phase transition of the QRM using this approach. We also provide a protocol to implement this method on a digital quantum simulator using the Quantum Restricted Boltzmann Machine algorithm. Our work opens up a new direction in the study of quantum phase transitions on quantum devices.

Khalid, Bilal↗
DOE OSTI2022

Nonadiabatic dissociation of molecular Bose-Einstein condensates: Competition between chemical reactions

Here, we provide a framework to solve generic models describing the dissociation of multiple molecular Bose Einstein condensates in a nonadiabatic regime. The competition between individual chemical reactions can lead to non-trivial dependence on critical components such as path interference and symmetries, thus, affecting the final distribution of atomic population. We find an analytical solution for an illustrative example model involving four atomic modes. When the system parameters satisfy CPT symmetry, where C is charge conjugation, P is parity, and T is time-reversal symmetry, our solution predicts a population imbalance between atomic modes that is exponentially sensitive to system parameters. However, a weakly broken symmetry alters the population in each atomic mode and can reverse the population imbalance. Our solution also demonstrates a strong quantum correlation between atomic modes that leads to the spontaneous production of atoms in a multi-mode squeezed state. Moreover, in our framework, a time-dependent non-Hermitian quantum mechanics naturally manifests which can alternatively be realized experimentally in photonic systems.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Intrinsic Defect-Induced Local Semiconducting-to-Metallic Regions Within Monolayer 1T-TiS2 Displayed by First-Principles Calculations and Scanning Tunneling Microscopy

Using density functional theory (DFT) and scanning tunneling microscopy (STM), the intrinsic point defects, formation energy, and electronic structure of 1T-TiS2 were investigated. Defect systems include single-atom vacancies, interstitial and adatom additions, and direct atomic substitution. Using a collective approach for analyzing realistic systems for point defect investigation, we provide a more straightforward comparison to the experimental measurements, reproducing more realistic environmental conditions related to thin film growth. STM images are compared to computationally simulated electron density images to identify specific geometries that result from favorable point defects. DFT suggests that titanium interstitials are the most energetically favorable intrinsic defect, and sulfur vacancies are more likely to form than titanium vacancies within this realistic analysis, which is in agreement with STM data. A pristine, stoichiometric monolayer system is calculated to have a direct band gap of 0.422 eV, which varies based on local point defects. Local semiconducting-to-metallic electronic transitions are predicted to occur based on the presence of Ti interstitials.

Keeney, P. J.↗
DOE OSTI2024

Ultrafast high-harmonic spectroscopy of solids

High-harmonic spectroscopy, an ultrafast all-optical technique initially conceptualized in atomic and molecular systems, has now emerged as a powerful platform for studying the structure and dynamics of condensed matter. Unlike that in the gas phase, solid-state high-harmonic generation relies on the fundamental response from high atomic density and periodicity, leading to interband transitions and coherent driving of electrons and holes in their respective bands. These mechanisms make high-harmonic spectroscopy particularly sensitive to the electronic band structure, topological properties and many-body correlations in condensed media. An advantage of high-harmonic spectroscopy over other spectroscopic methods is its ability to probe ultrafast phenomena, capturing femto- to attosecond dynamics of multi-band and strongly correlated electron interactions in solids. Furthermore, in this Review, we discuss the latest experimental and theoretical advances in ultrafast high-harmonic spectroscopy of solids and provide perspectives for future research in this field.

High-harmonic generation↗
DOE OSTI2023

Student Travel Support for the Inaugural Gordon Research Seminar on Multiphoton Processes (Final Technical Report)

This project provided financial support for early-career participants of the 2022 Gordon Research Seminar (GRS) on Multiphoton Processes, which was held on June 11 & 12, 2022 in Smithfield, Rhode Island, in conjunction with the Gordon Research Conference (GRC) on the same topic, held on June 12-17, 2022 in the same location. The GRC on Multiphoton Processes is an established conference series in the field of Atomic, Molecular and Optical (AMO) Physics with intense lasers. It regularly attracts around one hundred fifty researchers from around the world to present and discuss their forefront research featuring light-matter interaction in a variety of systems, ranging from atoms and molecules to nanosystems. In order to increase the attendance of early-career researchers at the GRC, in particular graduate students, post-docs, and other scientists with comparable levels of experience and education, the general assembly of the GRC on Multiphoton Processes decided during their last session in 2018 to organize a Gordon Research Seminar in conjunction with the next conference and organized and attended by early-career researchers. The GRS's primary intent is to provide a forum to graduate students and post-docs working in the field of intense and ultrafast AMO physics to present and exchange new data and cutting-edge ideas and to network with their peers at other research institutions around the U.S. and the world.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

COLUMBUS─An Efficient and General Program Package for Ground and Excited State Computations Including Spin–Orbit Couplings and Dynamics

The COLUMBUS program system provides the tools for performing high-level multireference (MR) computations, including the multireference configuration interaction (MRCI) method and its multireference averaged quadratic coupled cluster (MR-AQCC) extension, allowing computations on a wide range of fascinating atomic and molecular systems, including the treatment of open-shells and complicated excited state phenomena. The inclusion of spin−orbit coupling (SOC) directly within the MRCI step enables the description of systems containing heavy elements, such as lanthanides and actinides, whose properties are strongly influenced by SOC. Analytic energy gradients and nonadiabatic couplings at the correlated MRCI level provide the foundation for a variety of dynamics studies, giving insight into ultrafast photochemistry. New and ongoing method developments in COLUMBUS include the computation of spin densities, improved descriptions of ionic states, enhancements to the AQCC method, and the porting of COLUMBUS to graphical processing units (GPUs). New external interfaces enable an enhanced description of electronic resonances and molecules in strong laser fields. This work highlights these new developments while providing a detailed account of the diverse applications of COLUMBUS in recent years.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗