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At least 199 records · Page 11

Calculations on the competition between association and reaction for C3H(+) + H2

The ab initio results presently obtained for the potential energy surface of competing associative and reactive ion-molecule processes of the reactants H2 and C3H(+) show that the linear ion is able to directly access the deep potential well of the propargyl ion H2CCCH(+). Using the minimum energy potential pathway and properties of the stationary point structures determined via the ab initio methods, calculation results are obtained for both the association-rate coefficient for C3H3(+) production as a function of density, and the branching ratio between the propargyl and cyclic structures of the ion.

Maluendes, Sergio A.↗

Investigation of matter-antimatter interaction for possible propulsion applications

Matter-antimatter annihilation is discussed as a means of rocket propulsion. The feasibility of different means of antimatter storage is shown to depend on how annihilation rates are affected by various circumstances. The annihilation processes are described, with emphasis on important features of atom-antiatom interatomic potential energies. A model is developed that allows approximate calculation of upper and lower bounds to the interatomic potential energy for any atom-antiatom pair. Formulae for the upper and lower bounds for atom-antiatom annihilation cross-sections are obtained and applied to the annihilation rates for each means of antimatter storage under consideration. Recommendations for further studies are presented.

Morgan, D. L., Jr.↗

Theoretical electronic transition moments for the Ballik-Ramsay, Fox-Herzberg, and Swan systems of C2

Electronic transition moments and their variation with internuclear separation are calculated for the Ballik-Ramsay (b 3 Sigma g - a 3 Pi u), Fox-Herzberg (e 3 Pi g-a 3 Pi u) and Swan (d 3 Pi g-a 3 Pi u) band systems of C2, which appear in a variety of terrestrial and astrophysical sources. Electronic wave functions of the a 3 Pi u, b 2 Sigma g -, d 3 Pi g and e 3 Pi g states of C2 are obtained by means of a self-consistent field plus configuration interaction calculation using an atomic basis of 46 Slater-type orbitals, and theoretical potential energy curves and spectroscopic constants for the four electronic states were computed. The results obtained for both the potential energy curves and electronic transition moments are found to be in good agreement with experimental data.

Cooper, D. M.↗

The structures and energetics of fully nonlinear symmetric baroclinic waves

Rotating baroclinic flow for Richardson number lower than about 1 is studied by means of a finite difference Navier-Stokes model assuming no variations except in the vertical plane that completely contains the density gradient vector. The horizontally infinite channel to which attention is given further assumes periodic boundary conditions at the vertical computational boundaries and no-slip conducting horizontal boundaries. Two configurations are considered. Symmetric baroclinic waves developed in the flows in a manner consistent with linear theory, and it is noted that the structures and energetics of the fully developed waves were dependent on the Prandtl number Pr. For Pr greater than 1, the conversion from potential energy to wave kinetic energy was direct, via temperature and vertical motion correlation, while for Pr of less than 1, conversion proceeded from potential energy to average kinetic energy by means of an induced meridional flow, and then to wave kinetic energy.

Miller, T. L.↗

Influence of magnetic pressure on stellar structure: A Mechanism for solar variability

A physical mechanism is proposed that couples the Sun's dynamo magnetic field to its gravitational potential energy. The mechanism involves the isotropic field pressure resulting in a lifting force on the convective envelope, thereby raising its potential energy. Decay of the field due to solar activity allows the envelop to subside and releases this energy, which can augment the otherwise steady solar luminosity. Equations are developed and applied to the Sun for several field configurations. The best estimate model suggests that uniform luminosity variations as large as 0.02% for half a sunspot cycle may occur. Brief temporal variations or the rotation of spatial structures could allow larger excursions in the energy released.

Schatten, K. H.↗

Molecular dynamics and quasidynamics simulations of the annealing of bulk and near-surface interstitials formed in molecular-beam epitaxial Si due to low-energy particle bombardment during deposition

The relaxation, diffusion, and annihilation of split and hexagonal interstitials resulting from 10 eV Si irradiation of (2x1)-terminated Si(100) are investigated. Molecular dynamics and quasidynamics simulations, utilizing the Tersoff many-body potential are used in the investigation. The interstitials are created in layers two through six, and stable atomic configurations and total potential energies are derived as a function of site symmetry and layer depth. The interstitial Si atoms are allowed to diffuse, and the total potential energy changes are calculated. Lattice configurations along each path, as well as the starting configurations, are relaxed, and minimum energy diffusion paths are derived. The results show that the minimum energy paths are toward the surface and generally involved tetrahedral sites. The calculated interstitial migration activation energies are always less than 1.4 eV and are much lower in the near-surface region than in the bulk.

Kitabatake, M.↗

The dissociation energy of He2(+)

Ab initio potential energy curves for He2(+) are computed using full CI wavefunctions in conjuction with large Gaussian and Slater basis sets. The computed curves yield rotational-vibrational transitions with errors of less than 1/cm. They also yield quasi-bound levels with energies and lifetimes in reasonable agreement with translational spectroscopy measurements. The best D(e) is estimated to be 2.470 eV. Green's function Monte Carlo calculations yield a very similar value, 2.466 + or - 0.005.

Bauschlicher, Charles W., Jr.↗

The Role of Conical Intersections in Electronic Quenching of a State OH by H2 and N2

Lester and coworkers have experimentally characterized complexes of OH in the X and A states with H2 and N2. Recently, we have carried out ab initio calculations of relevant portions of the ground state and excited state potential energy surfaces for these systems, including the conical intersection regions, which are responsible for electronic quenching of the A state of OH by H2 and N2. Both of these systems have weakly bound complexes in the X state and strongly bound complexes in the A state. The OH-H2 complex is T-shaped, while the OH-N2 complex is collinear. In both cases the H end of OH is oriented toward the H2 or N2 molecule, respectively. Rotation of the OH about its center of mass involves only a small barrier and rotation by 1800 so that the 0 end of OH is oriented toward the H2 or N2 molecule leads to conical intersections with the ground state surface. Since there is about 95 kcal/mol of available energy after crossing to the ground state surface, chemical reactions on the ground state surface are possible, in addition to electronic quenching. In the case of OH-H2, the conical intersection is much lower in energy than the OH (A state) + H2 asymptotic energy and the A state complex can be characterized as a hanging well on the upper cone of the conical intersection. Passage through the conical intersection places the system on the ground state potential energy surface with the possibility of going to OH (X state) + H2 (i.e. electronic quenching) or to H2O + H (reaction). For OH-N2, the A state complex is also a hanging well on the upper cone of the conical intersection, but the conical intersection is only slightly below the OH (A state) + H2 asymptotic energy. Passage through the conical intersection can lead to OH (X state) + N2 (i.e. electronic quenching), but so far reactive pathways have not been found.

Walch, Stephen P.↗

Accurate Energetics for the Unimolecular Decomposition of HN2

We report internally contracted configuration interaction (ICCI) calculations along the constrained energy minimum (CEM) path for the addition of H to N2 with both CC-pVQZ and augmented CC-pVQZ basis sets. The results agree to within 0.5 kcal/mol with the larger basis set results of Walch, which were used to calibrate the HN2 potential energy surface used by Koizumi, Schatz, and Walch in coupled channel calculations to determine the lifetimes for unimolecular decay of the lowest vibrational levels of HN2. These small changes in the potential energy surface should have no significant effect on the computed lifetimes.

Walch, Stephen P.↗

Transport properties of ground state oxygen atoms

The transport properties of dilute monatomic gases depend on the two-body interactions between like atoms. When two ground-state oxygen atoms interact, they can follow any of 18 potential energy curves corresponding to O2, all of which contribute to the transport properties of the ground-state atoms. Transport collision integrals have been calculated for those interactions with an attractive minimum in the potential, and repulsive ab initio potential-energy curves have been accurately represented. Results are given for viscosity, thermal conductivity, and diffusion and they are compared with previous theoretical calculations.

Holland, Paul M.↗

A model of the Schumann-Runge continuum of O2

Ab initio calculations of the B3Sigma sub u(-) potential energy curve of O2 are reported together with the transition moment connecting the B3Sigma sub u(-) and the ground electronic states. Photodissociation cross sections are presented over the wavelength region 127-152 nm. Small adjustments to the potential energy curve and the transition moment lead to a model of the absorption which agrees well with the experimental cross sections and which reproduces the structural features observed on the high-energy edge. The shoulder at 135.6 nm is attributed to the lowest 3Pi sub u state and the auxiliary maxima to transitions into the B3Sigma sub u(-) state.

Allison, A. C.↗

Ab Initio Calculation of Accurate Vibrational Frequencies for Molecules of Interest in Atmospheric Chemistry

Due to advances in quantum mechanical methods over the last few years, it is now possible to determine ab initio potential energy surfaces in which fundamental vibrational frequencies are accurate to within +/- 8 cm(sup -1) on average, and molecular bond distances are accurate to within +/- 0.001-0.003 A, depending on the nature of the bond. That is, the potential energy surfaces have not been scaled or empirically adjusted in any way, showing that theoretical methods have progressed to the point of being useful in analyzing spectra that are not from a tightly controlled laboratory environment, such as rovibrational spectra from the interstellar medium. Some recent examples demonstrating this accuracy win be presented and discussed. These include the HNO, CH4, C2H4, and ClCN molecules. The HNO molecule is interesting due to the very large H-N anharmonicity, while ClCN has a very large Fermi resonance. The ab initio studies for the CH4 and C2H4 molecules present the first accurate full quartic force fields of any kind (i.e., whether theoretical or empirical) for a five-atom and six-atom system, respectively.

Lee, Timothy J.↗

Raindrop oscillations

A model of the change in shape of a raindrop is presented. Raindrops measured by two orthogonal cameras were classified by shape and orientation to determine the nature of the oscillation. A physical model based on potential energy was then developed to study the amplitude variation of oscillating drops. The model results show that oscillations occur about the equilibrium axis ratio, but the time average axis ratio if significantly more spherical for large amplitudes because of asymmetry in the surface potential energy. A generalization of the model to oscillations produced by turbulence yields average axis ratios that are consistent with the camera measurements. The model results for average axis ratios were applied to rainfall studies with a dual polarized radar.

Beard, K. V.↗

Extension during continental convergence, with application to the Tibetan Plateau

An explanation in terms of the thermal evolution of thickened continental lithosphere is offered to explain the transition, in the late Tertiary to Quaternary, from north-south compression to east-west extension in the strain rate field of the Tibetan Plateau. The lower part of the lithosphere consists of a thermal boundary layer which, when thickened by horizontal shortening, is colder and denser than its surroundings. Convective instability of the thickened thermal boundary layer and its replacement by hot asthenosphere would rapidly raise the surface elevation and gravitational potential energy of the overlying part of the lithosphere. The convective instability would happen in a time brief compared with the collision time scale but would only occur after there had already been substantial thickening of the lithosphere. The increase in surface height and of potential energy are sufficient for east-west extension to replace north-south compression as the dominant feature of the stress field.

England, Philip↗

Helium-3 inventory of lunar samples: A potential future energy resource for mankind?

Recent public concern over the safety, cost, and environmental impact of the worldwide fission reactors has focused the attention of scientists and engineers towards perfecting fusion technology because it promises a much more environmentally acceptable 'clean' energy supply. The fusion reaction D-2 + He-3 yields p(14.7 MeV) + He-4(3.6 MeV) has long been recognized as an ideal candidate for producing commercially 'safer and cleaner' fusion power. Naturally occurring He-3 is scarce on earth; however, lunar regolith is a potential ore for He-3 because the high He-3 in solar wind has been implanted in the lunar regolith for more than 4 x 10(exp 9) years, along with other volatile species. The helium abundance in lunar soils is dependent not only on the maturity of soils (I(sub S)/FeO) but also on their mineralogy. The titanium-rich (ilmenite) lunar soils are important repositories for volatiles, which may be released by heating these soils up to approximately 700 C.

Murali, A. V.↗

A VTOL Small Unmanned Aircraft System to Expand Payload Capabilities

One of the goals of Unmanned Aerial Systems (UAS) is to increase the capabilities of flight vehicles while maintaining small airframes that are also lightweight. Private package delivery companies and government agencies have an interest in vehicles that have large payload to weight ratios; thus allowing to deliver heavy payloads. Currently, UAS configurations suffer from propulsive and aerodynamic limitations that decrease the payload weight and/or mission range. In order to decrease these limitations, the Kinetic and Potential Energy Alternation for Greater Lift Enhancement (KP EAGLE) concept provides a novel way to transport payloads that may be too heavy for vehicles in a similar weight class. The concept vehicle takes off vertically without the payload. It then performs a dive maneuver that transfers the gained potential energy into kinetic energy to pick up the payload. This concept does not require special equipment during takeoff or landing and provides a better payload to weight ratio than other conventional vehicles in the same weight class.

Geuther, Steven↗

A comparison of the general circulations of the Northern and Southern Hemispheres based on satellite, multi-channel radiance data

Certain aspects of the general circulations of the Northern and Southern Hemispheres are compared using atmospheric structure obtained from Nimbus 3 Satellite Infrared Spectrometer (SIRS) data. Comparisons between the hemispheres of zonal and eddy available potential energy (AZ and AE) and zonal and eddy kinetic energy (KZ and KE) indicate that the ratios of AZ to AE and KZ to KE are larger in the Southern Hemisphere. The relative importance of standing and transient eddies in both hemispheres is investigated. The results show that standing eddies in the Southern Hemisphere contribute less to eddy available potential energy (AE) and eddy kinetic energy (KE) than in the Northern Hemisphere. The same type of inter-hemispheric distinction is true for the mid-latitude eddy heat flux. The distribution with latitude of the relative importance of standing and transient eddies is also studied. Horizontal eddy heat fluxes in the upper troposphere of both hemispheres are examined and in midlatitudes found to be approximately equal in magnitude when averaged over the summer and winter month. The Southern Hemisphere mid-latitude eddy heat flux is also shown to have significant longitudinal variations, apparently associated with the location of the southern continents.

Adler, R. F.↗

Quantum Hardware-Enabled Molecular Dynamics via Transfer Learning

The ability to perform ab initio molecular dynamics simulations using potential energy surfaces provided by quantum computers would open the door to virtually exact dynamics for a variety of chemical and biochemical systems, with impacts on catalysis and biophysics. Nonetheless, performing molecular dynamics on surfaces produced by quantum hardware has been hampered by the noisy energies typically produced by quantum computers and challenges associated with computing gradients and scaling to large systems interest. A recent set of advances in machine learning, known as transfer learning, provides a new path forward for molecular dynamics simulations on quantum hardware. Transfer learning offers a workaround, where one first trains models on larger, less accurate classical datasets and then refines them on smaller, more accurate quantum datasets. We explore this approach by training machine learning models to predict a molecule's potential energy based on its geometric structure using Behler-Parrinello neural networks. When successfully trained, the model enables energy gradient predictions necessary for dynamic simulations. To reduce the quantum resources needed, the model is initially trained with data derived from classical density functional theory and subsequently refined with a smaller dataset obtained from a variational quantum eigensolver optimization of the unitary coupled cluster ansatz. We show that this approach significantly reduces the size of the needed quantum training dataset while capturing the high accuracies needed within quantum chemistry simulations. The success of this two-step training method opens more opportunities to apply machine learning models on quantum data, a significant stride towards efficient quantum-classical hybrid computational models.

quantum computing↗