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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 NTRS2006

Modeling Ellipsometry Measurements of Molecular Thin-Film Contamination on Genesis Array Samples

The discovery of a molecular thin-film contamination on Genesis flown array samples changed the course of preliminary assessment strategies. Analytical techniques developed to measure solar wind elemental abundances must now compensate for a thin-film contamination. Currently, this is done either by experimental cleaning before analyses or by depth-profiling techniques that bypass the surface contamination. Inside Johnson Space Center s Genesis dedicated ISO Class 4 (Class 10) cleanroom laboratory, the selection of collector array fragments allocated for solar wind analyses are based on the documentation of overall surface quality, visible surface particle contamination greater than 1 m, and the amount of thin film contamination measured by spectroscopic ellipsometry. Documenting the exact thickness, surface topography, and chemical composition of these contaminates is also critical for developing accurate cleaning methods. However, the first step in characterization of the molecular film is to develop accurate ellipsometry models that will determine an accurate thickness measurement of the contamination film.

Calaway, Michael J.↗
DOE OSTI2020

The impact of the atmospheric turbulence-development tendency on new particle formation: a common finding on three continents

Abstract A new mechanism of new particle formation (NPF) is investigated using comprehensive measurements of aerosol physicochemical quantities and meteorological variables made in three continents, including Beijing, China; the Southern Great Plains site in the USA; and SMEAR II Station in Hyytiälä, Finland. Despite the considerably different emissions of chemical species among the sites, a common relationship was found between the characteristics of NPF and the stability intensity. The stability parameter (ζ = Z/L, where Z is the height above ground and L is the Monin–Obukhov length) is found to play an important role; it drops significantly before NPF as the atmosphere becomes more unstable, which may serve as an indicator of nucleation bursts. As the atmosphere becomes unstable, the NPF duration is closely related to the tendency for turbulence development, which influences the evolution of the condensation sink. Presumably, the unstable atmosphere may dilute pre-existing particles, effectively reducing the condensation sink, especially at coarse mode to foster nucleation. This new mechanism is confirmed by model simulations using a molecular dynamic model that mimics the impact of turbulence development on nucleation by inducing and intensifying homogeneous nucleation events.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Atomic-Level Features for Kinetic Monte Carlo Models of Complex Chemistry from Molecular Dynamics Simulations

The high computational cost of evaluating atomic interactions recently motivated the development of computationally inexpensive kinetic models, which can be parametrized from MD simulations of complex chemistry of thousands of species or other processes and accelerate the prediction of the chemical evolution by up to four order of magnitude. Such models go beyond the commonly employed potential energy surface fitting methods in that they are aimed purely at describing kinetic effects. So far, such kinetic models utilize molecular descriptions of reactions and have been constrained to only reproduce molecules previously observed in MD simulations. Therefore, these descriptions fail to predict the reactivity of unobserved molecules, for example in the case of large molecules or solids. In this work, we propose a new approach for the extraction of reaction mechanisms and reaction rates from MD simulations, namely the use of atomic-level features. Using the complex chemical network of hydrocarbon pyrolysis as example, it is demonstrated that kinetic models built using atomic features are able to explore chemical reaction pathways never observed in the MD simulations used to parametrize them, a critical feature to describe rare events. Atomic-level features are shown to construct reaction mechanisms and estimate reaction rates of unknown molecular species from elementary atomic events. Through comparisons of the model ability to extrapolate to longer simulation timescales and different chemical compositions than the ones used for parameterization, it is demonstrated that kinetic models employing atomic features retain the same level of accuracy and transferability as the use of features based on molecular species, while being more compact and parametrized with less data. We also find that atomic features can better describe the formation of large molecules enabling the simultaneous description of small molecules and condensed phases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Advancing quantitative models of soil microbiology, ecology, and biochemistry

Rapid advances in soil biology are increasingly reflected in mathematical models. From molecular to global scales, models contribute to fundamental understanding and prediction of critical soil processes, such as carbon sequestration. Recent models explicitly incorporate microbial control over soil carbon and nutrient cycling, an approach that offers greater biological realism but raises new challenges in model parameterization and stability. Although they have proliferated at community and ecosystem scales, microbial-explicit models have yet to be incorporated into most Earth system models. Applying soil models across scales requires integration with data to support parameterization and validation using approaches such as Bayesian data assimilation. In conclusion, to catalyze future progress, we recommend breaking down barriers between modeling and empirical disciplines while broadening access to the computational infrastructure that supports soil biological modeling.

Xie, Wally↗
DOE OSTI2024

Multinucleon transfer in 48 Ti + 48 Ti collisions at 11.5 MeV/nucleon

In this work, experimental data of projectile fragment distributions from a preliminary experimental study of the reaction of 11.5 MeV/nucleon 48 Ti on 48 Ti analyzed with the MARS recoil separator at the Cyclotron Institute of Texas A&M University are presented. Production cross sections, momentum distributions and excitation-energy distributions are extracted and compared with calculations with the Deep Inelastic Transfer (DIT) model and the Constrained Molecular Dynamics model (CoMD). Despite the limited extent of the present dataset, an overall agreement of the models with the data is found pointing at the prevailing nucleon-exchange character of the collisions at this energy.

Souliotis, Georgios↗
NASA NTRS1992

A source model for the L134N molecular cloud

The dark molecular cloud L134N is observed at millimeter wavelengths in the CS (J = 3-2), OCS (J = 7-6), and HDO (1 sub 11-1 sub 10) transitions. The CS (J = 3-2) transition was observed at four positions within the cloud, while the other two transitions were observed at one position each. Fractional abundances in the LTE approximation are calculated for each emission line detected. L134N appears to have a high-density core characterized by NH3, C3H2, and H(C-13)O(+) emission maps. A lower density envelope characterized by C(0-18), CS (J = 2-1), and SO emission surrounds the core. There appears to be a gas-phase oxygen abundance gradient in L134N with atomic oxygen depleted in the high-density core. Observed molecular distributions within L134N can be explained by a model in which chemical and physical processes in icy-dust-grain mantles influence the gas-phase molecular abundances.

Swade, Daryl A.↗
NASA NTRS2006

Isotope Effects in Collisional VT Relaxation of Molecular Hydrogen

A simple exponential-potential model of molecular collisions leads to a two-parameter analytic expression for rates of collisionally induced vibrational-translation (VT) energy exchange that has been shown to be accurate over variations of orders of magnitude as a function of temperature in a variety of systems. This includes excellent agreement with reported experimental and theoretical results for the fundamental self-relaxation rate of molecular hydrogen H2(v = 1) + H2 yields H2(v = 0) + H2. The analytic rate successfully follows the five-orders-of-magnitude change in experimental values for the temperature range 50-2000 K. This approach is now applied to isotope effects in the vibrational relaxation rates of excited HD and D2 in collision with H2: HD(v = 1)+H2 yields HD(v = 0)+H2 and D2(v = 1)+H2 yields D2(v = 0)+H2. The simplicity of the analytic expression for the thermal rate lends itself to convenient application in modeling the evolving vibrational populations of molecular hydrogen in shocked astrophysical environments.

Bieniek, R. J.↗
NASA NTRS1985

Spectral identification/elimination of molecular species in spacecraft glow

Computer models of molecular electronic and vibrational emission intensities were developed. Known radiative emission rates (Einstein coefficients) permit the determination of relative excited state densities from spectral intensities. These codes were applied to the published spectra of glow above shuttle surface and to the Spacelab 1 results of Torr and Torr. The theoretical high-resolution spectra were convolved with the appropriate instrumental slit functions to allow accurate comparison with data. The published spacelab spectrum is complex but N2+ Meinel emission can be clearly identified in the ram spectrum. M2 First Positive emission does not correlate well with observed features, nor does the CN Red System. Spectral overlay comparisons are presented. The spectrum of glow above shuttle surfaces, in contrast to the ISO data, is not highly structured. Diatomic molecular emission was matched to the observed spectral shape. Source excitation mechanisms such as (oxygen atom)-(surface species) reaction product chemiluminescence, surface recombination, or resonance fluorescent re-emission will be discussed for each tentative assignment. These assignments are the necessary first analytical step toward mechanism identification. Different glow mechanisms will occur above surfaces under different orbital conditions.

Green, B. D.↗
DOE OSTI2024

KCl-UCl 3 molten salts investigated by Ab Initio Molecular Dynamics (AIMD) simulations: A comparative study with three dispersion models

Ab Initio Molecular Dynamics (AIMD) simulations are performed on molten KCl-UCl 3 salt mixtures to determine energies, heat capacities, and densities. The density-dependent energy correction (DFT-dDsC), Grimme et al.’s DFT-D3, and Langreth & Lundqvist (vdW-cx) models are used for dispersion forces and combined with the Perdew-Burke-Ernzerhof (PBE) exchange-correlation potential with a Hubbard U param eter for the 5$f$ electrons of uranium. After validating predictions for the end-member systems to literature data, KCl-UCl 3 mixtures are studied at select temperatures. Densities and energies both deviate from ideal solution behavior, with the maximum deviation occurring around 36% UCl 3 for mixing energies and slightly lower (29% UCl 3 ) for densities. Compared to the NaCl-UCl 3 system, which was previously investigated using the same simulation methodologies, the KCl-UCl 3 density and mixing energy deviations from ideal solution behavior are larger by almost a factor of two. No deviation from ideal solution behavior for heat capacity was observed. The AIMD predictions for mixing energies and densities agree qualitatively with experimental data, though the spread in data obtained from the various dispersion force models utilized, measurements, and empirical estimates makes strong conclusions difficult. The dependence of thermodynamic and thermophysical properties on composition is correlated with the local chemistry of the solution phase, in particular, the tendency of UCl 3 to form network structures.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Geometry-complete diffusion for 3D molecule generation and optimization

Abstract Generative deep learning methods have recently been proposed for generating 3D molecules using equivariant graph neural networks (GNNs) within a denoising diffusion framework. However, such methods are unable to learn important geometric properties of 3D molecules, as they adopt molecule-agnostic and non-geometric GNNs as their 3D graph denoising networks, which notably hinders their ability to generate valid large 3D molecules. In this work, we address these gaps by introducing the Geometry-Complete Diffusion Model (GCDM) for 3D molecule generation, which outperforms existing 3D molecular diffusion models by significant margins across conditional and unconditional settings for the QM9 dataset and the larger GEOM-Drugs dataset, respectively. Importantly, we demonstrate that GCDM’s generative denoising process enables the model to generate a significant proportion of valid and energetically-stable large molecules at the scale of GEOM-Drugs, whereas previous methods fail to do so with the features they learn. Additionally, we show that extensions of GCDM can not only effectively design 3D molecules for specific protein pockets but can be repurposed to consistently optimize the geometry and chemical composition of existing 3D molecules for molecular stability and property specificity, demonstrating new versatility of molecular diffusion models. Code and data are freely available on GitHub .

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

Shadow Molecular Dynamics and Atomic Cluster Expansions for Flexible Charge Models

Here, a shadow molecular dynamics scheme for flexible charge models is presented where the shadow Born–Oppenheimer potential is derived from a coarse-grained approximation of range-separated density functional theory. The interatomic potential, including the atomic electronegativities and the charge-independent short-range part of the potential and force terms, is modeled by the linear atomic cluster expansion (ACE), which provides a computationally efficient alternative to many machine learning methods. The shadow molecular dynamics scheme is based on extended Lagrangian (XL) Born–Oppenheimer molecular dynamics (BOMD). XL-BOMD provides stable dynamics while avoiding the costly computational overhead associated with solving an all-to-all system of equations, which normally is required to determine the relaxed electronic ground state prior to each force evaluation. To demonstrate the proposed shadow molecular dynamics scheme for flexible charge models using atomic cluster expansion, we emulate the dynamics generated from self-consistent charge density functional tight-binding (SCC-DFTB) theory using a second-order charge equilibration (QEq) model. The charge-independent potentials and electronegativities of the QEq model are trained for a supercell of uranium oxide (UO 2 ) and a molecular system of liquid water. The combined ACE+XL-QEq molecular dynamics simulations are stable over a wide range of temperatures both for the oxide and for the molecular systems and provide a precise sampling of the Born–Oppenheimer potential energy surfaces. Accurate ground Coulomb energies are produced by the ACE-based electronegativity model during an NVE simulation of UO 2 , predicted to be within 1 meV of those from SCC-DFTB on average during comparable simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Stochastic symplectic reduced-order modeling for model-form uncertainty quantification in molecular dynamics simulations in various statistical ensembles

Here, this work focuses on the representation of model-form uncertainties in molecular dynamics simulations in various statistical ensembles. In prior contributions, the modeling of such uncertainties was formalized and applied to quantify the impact of, and the error generated by, pair-potential selection in the microcanonical ensemble (NVE). In this work, we extend this formulation and present a linear-subspace reduced-order model for the canonical (NVT) and isobaric (NPT) ensembles. The symplectic reduced-order basis is randomized on the tangent space of the Stiefel manifold to provide topological relationships and capture model-form uncertainty. Using the Large-scale Atomic/Molecular Massively Parallel Simulator (LAMMPS), we assess the relevance of these stochastic reduced-order atomistic models on canonical problems involving a Lennard-Jones fluid and an argon crystal melt.

42 ENGINEERING↗
NASA NTRS2026

Gateway Element and Payload Materials Outgassing Analyses: HALO, HERMES, and ERSA

Gateway was intended to be humanity’s first space station around the Moon, but its development has been paused as the National Aeronautics and Space Administration (NASA) shifts focus to achieving the United States’ National Space Policy goals. Instead of an orbiting lunar outpost, NASA will now pursue the development of a lunar surface base to support a sustained human presence on the Moon. Before the program’s pause, Gateway’s Induced Environments team worked to ensure payloads and elements (i.e., modules) complied with induced environment requirements. Methods developed and insights gained from this work will have applicability to NASA’s Moon Base and the potential repurposing of Gateway elements and payloads, as well as to induced environments modeling for future space stations. The Gateway program’s induced environment included molecular contamination, electric thruster plume sputter and redeposition, and lunar dust transfer from the Human Landing System (HLS). Primary sources of external molecular contamination included materials outgassing, chemical thruster plume contamination, and vacuum venting. The focus of this paper will be on element- and payload-level materials outgassing analyses performed for Gateway Configuration 1, extending the previously-developed framework for Gateway system-level external molecular contamination modeling. Gateway Configuration 1 consisted of the Power and Propulsion Element (PPE) and the Habitation and Logistics Outpost (HALO). It also included payloads like the European Radiation Sensor Array (ERSA) attached to PPE and the Heliophysics Environmental and Radiation Measurement Experiment Suite (HERMES) attached to HALO. The element- and payload-level analyses to be introduced in this paper for HALO, HERMES, and ERSA enabled high-fidelity descriptions of Gateway’s external molecular contamination environment. Approaches to geometric modeling, meshing, outgassing rate assignment, molecular transport modeling, and analysis methodology will be presented. Element and payload contaminant deposition onto sensitive Gateway receiver surfaces will be summarized and results compared to induced environment requirements. While these results incorporate refinements made over the course of the program, they were not intended to be final. Therefore, modeling assumptions and inputs, potential improvements, and lessons-learned will be documented to inform future work on Moon Base, repurposed elements and payloads, and other space stations.

Gateway↗
NASA NTRS1980

Laboratory and modeling studies of chemistry in dense molecular clouds

A chemical evolutionary model with a large number of species and a large chemical library is used to examine the principal chemical processes in interstellar clouds. Simple chemical equilibrium arguments show the potential for synthesis of very complex organic species by ion-molecule radiative association reactions.

Huntress, W. T., Jr.↗
NASA NTRS1988

A molecular dynamics study of chloride binding by the cryptand SC24

The capture of chloride from water by the tetraprotonated form of the spherical macrotricyclic molecule SC24 was studied using molecular dynamics simulation methods. This model ionophore represents a broad class of molecules which remove ions from water. Two binding sites for the chloride were found, one inside and one outside the ligand. These sites are separated by a potential energy barrier of approximately 20 kcal mol-1. The major contribution to this barrier comes from dehydration of the chloride. The large, unfavorable dehydration effect is compensated for by an increase in electrostatic attraction between the oppositely charged chloride and cryptand, and by energetically favorable rearrangements of water structure. Additional assistance in crossing the barrier and completing the dehydration of the ion is provided by the shift of three positively charged hydrogen atoms of the cryptand towards the chloride. This structural rigidity is partially responsible for its selectivity.

NASA Discipline Exobiology↗
NASA NTRS1994

Modeling radiative transfer in molecular clouds. 1: HCO(+) in the star-forming region W49A North

A new general multilevel, non-Local Thermodynamic Equilibrium (LTE) radiative transfer code, valid for any velocity field, is applied to HCO(+) observations of W49A North. Three classes of collapse models are considered: free-fall collapse (v proportional to 1/sq. root of r), rho proportional to r(exp -3/2) throughout the molecular cloud, successfully reproduces the features of the observations and gives the best fit to the J = 1-0 and J = 3-2 profiles both toward the prominent H II component G of W49A North and off the center. In addition to a slow radial fall-off of density, the theoretical modeling implies the following for the molecular cloud: the large line widths result from motions occurring within the inner 1 pc, and there are probably one or more fragments with peculiar velocities within this same region.

Dickel, Helene R.↗
NASA NTRS1980

Clumpy molecular clouds - A dynamic model self-consistently regulated by T Tauri star formation

A model is proposed which can account for the longevity, energetics, and dynamical structure of dark molecular clouds. Recent observations of a high space density of T Tauri stars in some dark clouds provide the basis for the assertion that high-velocity winds from these low mass pre-main-sequence stars provide a continuous dynamic input into molecular clouds. It is postulated that as clumps are driven above the Jeans mass, both by coalescence and the enhancement of ram pressure through continuing acceleration by protostellar winds, collapse is followed by the formation of low-mass stars that generate additional protostellar winds. Finally, it is found that star formation occurs on a relatively slow time scale, comparable to the cloud lifetime

Norman, C.↗
DOE OSTI2021

Attention-based generative models for de novo molecular design

An implementation of attention within the variational autoencoder framework for continuous representation of molecules. The addition of attention significantly increases model performance for complex tasks such as exploration of novel chemistries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗