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At least 235 records · Page 13

Theory of inelastic ion-atom scattering at low and intermediate energies

Ab initio calculations are presented of inelastic energy loss and ionization phenomena associated with Ar(+)-Ar collisions at small distances of closest approach and for laboratory collision energies ranging from several keV to several hundred keV. Outer-shell excitations are handled statistically; inner-shell excitations are calculated from the viewpoint of quasidiabatic molecular orbital promotion. Auger electron yield, average state of ionization, and average inelastic energy loss are calculated per collision as a function of distance of closest approach of the collision partners for several laboratory collision energies. Average charge-state probabilities per collision partner are calculated as a function of the average inelastic energy loss per atom. It is shown that the structure in the data is due to the underlying structure in the inner-shell independent-electron quasimolecular promotion probabilities.

Schmid, G. B.↗

Structure-activity correlations for organophosphorus ester anticholinesterases. Part 2: CNDO/2 calculations applied to ester hydrolysis rates

Quantitative structure-activity relationships are presented for the hydrolysis of organophosphorus esters, RR'P(O)X, where R and R' are alkyl and/or alkoxy groups and X is fluorine, chlorine or a phenoxy group. CNDO/2 calculations provide values for molecular parameters that correlate with alkaline hydrolysis rates. For each subset of esters with the same leaving group, X, the CNDO-derived net atomic charge at the central phosphorus atom correlates well with the alkaline hydrolysis rate constants. For the whole set of esters with different leaving groups, equations are derived that relate charge, orbital energy and bond order to the hydrolysis rate constants.

Johnson, H.↗

Molecular dynamics investigation of radiation damage in semiconductors

Results of a molecular dynamics investigation of the effects of radiation damage on the crystallographic structure of semiconductors are reported. Particular cosiderastion is given to the formation of point defects and small defect complexes in silicon at the end of a radiation-damage cascade. The calculations described make use of the equivalent crystal theory of Smith and Banerjea (1988). Results on the existence of an atomic displacement threshold, the defect formation energy, and some crystallographic information on the defects observed are reported.

Good, Brian S.↗

High-Performance Computing Optimization for Aladyn – Adaptive Neural Network Molecular Dynamics Mini-Application

This report provides a description and performance evaluation of the optimization techniques for high performance computing (HPC) implementation of the open source Computational Materials mini-application Aladyn (https://github.com/nasa/aladyn). Aladyn is a basic molecular dynamics code written in FORTRAN 2003, which is designed to demonstrate the use of adaptive neural networks (ANNs) in atomistic simulations. The role of ANNs is to efficiently reproduce the very complex energy landscape resulting from the atomic interactions in materials with the accuracy of the more expensive quantum mechanics-based calculations. The ANN is trained on a large set of atomic structures calculated using the density functional theory (DFT) method. While achieving orders of magnitude faster computational performance than DFT, the ANN-based approach was still very computationally demanding compared to the conventional approach of using empirically fitted energy functions. After its initial development, Aladyn was evaluated and optimized by experts at the NASA Advanced Supercomputing (NAS) division to exploit modern supercomputer architectures. The code has been optimized for execution on multicore central processing units (CPUs), including Intel® Skylake microarchitecture, and on graphic accelerators, such as Nvidia® V100 graphic processing units (GPUs), using Open Multi-Processing (OpenMP) and Open Accelerators (OpenACC) programming interfaces. The optimization achieved a speedup of 4.7 times the baseline version on CPU performance and an additional 2.4 times on CPU+GPU performance. Atomistic computer simulations are a fundamental tool in materials research to model material properties form physics-based first principles. Atomic interaction, governed by Quantum Mechanics (QM) require sophisticated and highly computationally demanding mathematical models to calculate [1]. Classical methods use approximate functional forms, empirically fitted through a set of variable parameters to emulate atomic energies as direct functions of atomic coordinates [2]. While empirical potentials are computationally much simpler, allowing simulations of large-scale systems of up to a trillion (1012) atoms [3], they are substantially less accurate compared to quantum calculations and applicable only to very specific atomic configurations or predefined crystallographic phases. A recently suggested approach is to use heuristic machine learning methods [4], such as those based on Adaptive Neural Networks (ANNs) to predict atomic energies, after being trained on a sufficiently large database of QM-calculated structures [5,6]. This approach reduces significantly the computational complexity, allowing for simulations of orders of magnitude larger systems compared to QM-based methods without compromising accuracy. Still, compared to classical methods using empirical energy functions, ANN methods remain two- to three orders of magnitude more computationally demanding. Hence, the computational cost of simulations, together with the need for extensive training of ANNs, still makes the practical implementation of ANN-based methods quite challenging. The purpose of the Aladyn mini-application software [7], available as open source at https://github.com/nasa/aladyn, is to be a testbed for exploring possible optimization strategies to develop highly scalable parallel algorithms for ANN-based atomistic simulations. Aladyn is aimed at utilizing the architecture of the high-end modern highperformance computing (HPC) hardware based on multicore central processing units (CPUs) equipped with graphic processing unit (GPU) accelerators. Specifically, the goal is to optimize the performance on a single HPC compute node, before implementing scaling to multi-node parallelization using message passing interface (MPI). At the same time, the open source code of Aladyn can serve as a training model for students and professors in academia.

Yamakov, Vesselin I.↗

AladynPi – Adaptive Neural Network Molecular Dynamics Simulation Code with Physically Informed Potential: Computational Materials Mini-Application

This report provides an overview and description of commands used in the Computational Materials mini-application, AladynPi. AladynPi is an extension of a previously released mini-application, Aladyn (https://github.com/nasa/aladyn; Yamakov, V.I., and Glaessgen, E.H., NASA/TM-2018-220104). Aladyn and AladynPi are basic molecular dynamics codes written in FORTRAN 2003, which are designed to demonstrate the use of adaptive neural networks (ANNs) in atomistic simulations. The role of ANNs is to efficiently reproduce the very complex energy landscape resulting from the atomic interactions in materials with the accuracy of the more expensive quantum mechanics-based calculations. The ANN is trained on a large set of atomic structures calculated using the density functional theory method. An input for the ANN is a set of structure coefficients, characterizing the local atomic environment of each atom, for which the atomic energy is obtained in the ANN inference process. In Aladyn, the ANN gives directly the energy of interatomic interactions. In AladynPi, the ANN gives optimized parameters for a predefined empirical function, known as bond-order-potential (BOP). The parameterized BOP function is then used to calculate the energy. AladynPi code is being released to serve as a training testbed for students and professors in academia to explore possible optimization algorithms for parallel computing on multicore central processing unit (CPU) computers or computers utilizing manycore architectures based on graphic processing units (GPUs). The effort is supported by the High Performance Computing incubator (HPCi) project at NASA Langley Research Center.

Yamakov, Vesselin I.↗

Discovery of optical molecular emission from the bipolar nebula surrounding HD 44179

Spectrophotometry and spectropolarimetry with HD 44179 are presented. These measurements reveal that the very broad bump evident in previous low-resolution spectra possesses a large amount of structure, including groups of narrow emission lines and several diffuse features. A reduction in polarization, but constant position angle, through the bump indicates that this emission originates within the nebula itself and merely dilutes the polarized scattered starlight. A few very weak atomic emission lines are detected, but the overall feature, which strongly resembles the emission spectra of some molecules, remains unidentified. Constraints on the excitation mechanism are discussed.

Schmidt, G. D.↗

Better PFAE's From Direct Fluorination

New low-molecular-weight perfluoroalkylethers (PFAE's) synthesized by direct fluorination in experimental study. Correlated viscosity and oxidation characteristics of PFAE's with structures to evaluate suitability as high-temperature lubricants and hydraulic fluids. Direct fluorination process attractive because it often involves single-step reaction and uses cheap starting materials. Versatile: produces highly branched ethers as well as polyethers containing more than two sequential carbon atoms in polymer chains. Such molecules cannot be made by conventional techniques.

Jones, W. R., Jr.↗

Analysis of plume backflow around a nozzle lip in a nuclear rocket

The structure of the flow around a nuclear thermal rocket nozzle lip has been investigated using the direct simulation Monte Carlo method. Special attention has been paid to the behavior of a small amount of harmful particles that may be present in the rocket exhaust gas. The harmful fission product particles are modeled by four inert gases whose molecular weights are in a range of 4 131. Atomic hydrogen, which exists in the flow due to the extremely high nuclear fuel temperature in the reactor, is also included. It is shown that the plume backflow is primarily determined by the thin subsonic fluid layer adjacent to the surface of the nozzle lip, and that the inflow boundary in the plume region has negligible effect on the backflow. It is also shown that a relatively large amount of the lighter species is scattered into the backflow region while the amount of the heavier species becomes negligible in this region due to extreme separation between the species. Results indicate that the backscattered molecules are very energetic and are fast-moving along the surface in the backflow region near the nozzle lip.

Chung, Chan H.↗

The calculation of theoretical chromospheric models and the interpretation of solar spectra from rockets and spacecraft

Since the early 1970s we have been developing the extensive computer programs needed to construct models of the solar atmosphere and to calculate detailed spectra for use in the interpretation of solar observations. This research involves two major related efforts: work by Avrett and Loeser on the Pandora computer program for non-LTE modeling of the solar atmosphere including a wide range of physical processes, and work by Kurucz on the detailed synthesis of the solar spectrum based on opacity data for over 58 million atomic and molecular lines. Our goals are to determine models of the various features observed on the Sun (sunspots, different components of quiet and active regions, and flares) by means of physically realistic models, and to calculate detailed spectra at all wavelengths that match observations of those features. These two goals are interrelated: discrepancies between calculated and observed spectra are used to determine improvements in the structure of the models, and in the detailed physical processes used in both the model calculations and the spectrum calculations. The atmospheric models obtained in this way provide not only the depth variation of various atmospheric parameters, but also a description of the internal physical processes that are responsible for non-radiative heating, and for solar activity in general.

Avrett, Eugene H.↗

The calculation of theoretical chromospheric models and the interpretation of the solar spectrum

Since the early 1970s we have been developing the extensive computer programs needed to construct models of the solar atmosphere and to calculate detailed spectra for use in the interpretation of solar observations. This research involves two major related efforts: work by Avrett and Loeser on the Pandora computer program for non-LTE modeling of the solar atmosphere including a wide range of physical processes, and work by Kurucz on the detailed synthesis of the solar spectrum based on opacity data for over 58 million atomic and molecular lines. Our goals are to determine models of the various features observed on the sun (sunspots, different components of quiet and active regions, and flares) by means of physically realistic models, and to calculate detailed spectra at all wavelengths that match observations of those features. These two goals are interrelated: discrepancies between calculated and observed spectra are used to determine improvements in the structure of the models, and in the detailed physical processes used in both the model calculations and the spectrum calculations. The atmospheric models obtained in this way provide not only the depth variation of various atmospheric parameters, but also a description of the internal physical processes that are responsible for nonradiative heating, and for solar activity in general.

Avrett, Eugene H.↗

Why Are Buckyonions Round?

Multi-layered round carbon particles (onions) containing tens to hundreds of thousands of atoms form during electron irradiation of graphite carbon. However, theoretical models of large icosahedral fullerenes predict highly faceted shapes for molecules with more than a few hundred atoms. This discrepancy in shape may be explained by the presence of defects during the formation of carbon onions. Here, we use the semi-empirical tight-binding method for carbon to simulate the incorporation of pentagon-heptagon defects on to the surface of large icosahedral fullerenes. We show a simple mechanism that results in energetically competitive derivative structures and a global change in molecular shape from faceted to round. Our results provide a plausible explanation of the apparent discrepancy between experimental observations of round buckyonions and theoretical predictions of faceted icosahedral fullerenes.

Bates, Kevin R.↗

The Calculation of Theoretical Chromospheric Models and the Interpretation of the Solar Spectrum

Since the early 1970s we have been developing the extensive computer programs needed to construct models of the solar atmosphere and to calculate detailed spectra for use in the interpretation of solar observations. This research involves two major related efforts: work by Avrett and Loeser on the Pandora computer program for non-LTE modeling of the solar atmosphere including a wide range of physical processes, and work by Rurucz on the detailed synthesis of the solar spectrum based on opacity data or over 58 million atomic and molecular lines. our goals are: to determine models of the various features observed on the Sun (sunspots, different components of quiet and active regions, and flares) by means of physically realistic models, and to calculate detailed spectra at all wavelengths that match observations of those features. These two goals are interrelated: discrepancies between calculated and observed spectra are used to determine improvements in the structure of the models, and in the detailed physical processes used in both the model calculations and the spectrum calculations. The atmospheric models obtained in this way provide not only the depth variation of various atmospheric parameters, but also a description of the internal physical processes that are responsible for non-radiative heating, and for solar activity in general.

Avrett, Eugene H.↗

Why are Buckyonions Round?

Multi-layered round carbon particles (onions) containing tens to hundreds of thousands of atoms form during electron irradiation of graphite. However. theoretical models or large icosahedral fullerenes predict highly faceted shapes for molecules with more than a few hundred atoms. This discrepancy in shape may be explained by the presence of defects during the formation of carbon onions. Here, we use the semi-empirical tight-binding method for carbon to simulate the incorporation of pentagon-heptagon defects on to the surface of large icosahedral fullerenes. We show a simple mechanism that results in energetically competitive derivative structures and a global change in molecular shape from faceted to round. Our results provide a plausible explanation of the apparent discrepancy between experimental observations or round buckyonions and theoretical predictions of faceted icosahedral fullerenes.

Bates, Kevin R.↗

Laboratory Astrophysics: The Universe in the Palm of Your Hand

Polycyclic aromatic compounds (PACs), a class of organic molecules whose structures are characterized by the presence of two or more fused aromatic rings, have been the subject of astrophysical interest for nearly two decades. Large by interstellar standards (from as few as 20 to perhaps as many as several hundred atoms), it has been suggested that these species are among the most abundant interstellar molecules impacting a wide range of astrophysical phenomena including: (1) the ubiquitous family of infrared emission bands observed in an ever-increasing assortment of astronomical objects; (2) the subtle but rich array of discrete visible/near-infrared interstellar molecular absorption features known as the diffuse interstellar bands (DIBs); (3) the broad near-infrared quasi-continuum observed in a number of nebulae known as excess red emission (ERE); (4) the interstellar ultraviolet extinction curve and broad '2200 Angstrom bump'; and (5) the heating/cooling mechanisms of interstellar clouds. Nevertheless, until recently a lack of good-quality laboratory spectroscopic data on PACs under astrophysically relevant conditions (i.e. isolated, ionized molecules, ionized molecular clusters, etc.) has hindered critical evaluation and extension of this model. Fortunately, the last decade has seen an explosion of experimental and theoretical techniques aimed specifically at addressing these issues. Indeed, many of these techniques will be explored in the series of talks which constitute this forum. This talk will provide an overview of the studies of the spectroscopic properties of isolated, neutral, and ionized PACs that have been conducted in the Astrochemistry Laboratory at NASA Ames, together with a consideration of their implications for astrophysics. Particular attention will be paid to models of the interstellar infrared emission spectra generated using the available database of laboratory PAC infrared spectra and the natural ability of this database to accommodate the variations observed in the astronomical spectra. Such models provide insight into the structure, abundance, and ionization state of the interstellar PAC population and, in turn, provide direct insight into the processes of carbon nucleation, growth and evolution as matter is processed through the interstellar medium. These models will be followed by a more in depth look at some specific aspects of the interstellar infrared emission spectrum, considering both what we can learn about them and what we can learn from them. Finally, some of the limitations of the current model and the available spectroscopic dataset will be 'dered along with future experimental directions designed to address these shortcomings. Further information about this and the related areas of research currently ongoing in the Astrochemistry Laboratory can be found at our world wide web site. http://www-space.arc.nasa.gov/(tilda)astrochem

Hudgins, Douglas M.↗

The formation of molecules in interstellar clouds from singly and multiply ionized atoms

The suggestion is considered that multiply ionized atoms produced by K- and L-shell X-ray ionization and cosmic-ray ionization can undergo ion-molecule reactions and also initiate molecule production. The role of X-rays in molecule production in general is discussed, and the contribution to molecule production of the C(+) radiative association with hydrogen is examined. Such gas-phase reactions of singly and multiply ionized atoms are used to calculate molecular abundances of carbon-, nitrogen-, and oxygen-bearing species. The column densities of the molecules are evaluated on the basis of a modified version of previously developed isobaric cloud models. It is found that reactions of multiply ionized carbon with H2 can contribute a significant fraction of the observed CH in diffuse interstellar clouds in the presence of diffuse X-ray structures or discrete X-ray sources and that substantial amounts of CH(+) can be produced under certain conditions.

Langer, W. D.↗

Computer simulation of protein systems

Ligand binding to dihydrofolate reductase (DHFR) is discussed. This is an extremely important enzyme, as it is the target of several drugs (inhibitors) which are used clinically as antibacterials, antiprotozoals and in cancer chemotherapy. DHFR catalyzes the NADPH (reduced nicotinamide adenine dinucleotide phosphate) dependent reduction of dihydrofolate to tetrahydrofolate, which is used in several pathways of purine and pyrimidine iosynthesis, including that of thymidylate. Since DNA synthesis is dependent on a continuing supply of thymidylate, a blockade of DHFR resulting in a depletion of thymidylate can lead to the cessation of growth of a rapidly proliferating cell line. DHFR exhibits a significant species to species variability in its sensitivity to various inhibitors. For example, trimethoprim, an inhibitor of DHFR, binds to bacterial DHFR's 5 orders of magnitude greater than to vertebrate DHFR's. The structural mechanics, dynamics and energetics of a family of dihydrofolate reductases are studied to rationalize the basis for the inhibitor of these enyzmes and to understand the molecular basis of the difference in the binding constants between the species. This involves investigating the conformational changes induced in the protein on binding the ligand, the internal strain imposed by the enzyme on the ligand, the restriction of fluctuations in atom positions due to binding and the consequent change in entropy.

Osguthorpe, D. J.↗

Interaction of a Model Peptide with a Water--Bilayer System

We discuss a molecular dynamics study of the alanine dipeptide at the interface between water and a glycerol-1-monooleate (GMO) bilayer. The dipeptide is interfacially active and incorporates into the bilayer without disrupting its structure. The interfacial region that is readily penetrated by the dipeptide spans the entire head group portion of the bilayer. The polar groups of the alanine dipeptide mostly remain well solvated by water and the oxygen atoms of GMO, and conformations of the dipeptide are characterized by (phi, psi) angles typical of alpha-helix and beta-sheet structures. When the molecule is deeper in the bilayer, the C(sub 7eq) state also becomes stable. The barrier to the isomerization reaction at the interface is lower than in bulk phases. After 7 ns of trajectories, the system is not fully equilibrated, due to slow collective motions involving GMO head groups. These result in decreased mobility and lower rates of isomerization of the dipeptide at the interface.

Pohorille, A.↗

Models for aurora and airglow emissions from other planetary atmospheres

Models for aurora and airglow emissions from planetary atmospheres other than the earth are surveyed, with emphasis on accomplishments of the last seven years. The goals of modeling the terrestrial planets and modeling the outer planets are very different. Because less is known about the atmospheres of the outer planets, models of their luminosity seek to provide information about the basic structure of the atmospheres and to identify the major production mechanisms. Models of the terrestrial planets have recently begun to address more complex questions about the abundances of trace and minor constituents, about transport phenomena, and about spatial and temporal variations in the atmosphere and in the processes that produce the emissions. In addition, there are a few instances in which models have been used to elucidate atomic and molecular processes that are difficult to study either in the terrestrial atmosphere or in the laboratory.

Fox, J. L.↗