Physics Commons^™

Does N-2(-) Exist? A Coupled-Cluster Study, Gennady L. Gutsev, Piotr B. Rozyczko, Rodney J. Bartlett, Charles A. Weatherford

Physics Publications

Potential energy curves of the ground-state N2 molecule and its doublet N−2 anion are calculated at the coupled-cluster level with single and double excitations and with noniterative triples [CCSD(T)] as well as with the multireference averaged-quadratic coupled-cluster (MR-AQCC) method. The N−2 anion is shown to be temporary and decays to its neutral parent plus a free electron at bond lengths shorter than ≈1.4 and larger than ≈2.5 Å. Thus, the N−2 anion exists within the 1.4⩽R(N–N)⩽2.5 Å range at the Born–Oppenheimer approximation.

Thermodynamical Stability Of Ch3ono And Ch3ono-: A Coupled-Cluster And Hartree-Fock-Density-Functional-Theory Study, Gennady L. Gutsev, Puru Jena, Rodney J. Bartlett

Physics Publications

The structure and thermodynamic stability of methylnitrite and its anion are studied by the infinite-order coupled-cluster method with all singles and doubles and noniterative inclusion of triple excitations [CCSD(T)] and Hartree–Fock-density-functional theory (HFDFT). We have optimized the geometries and computed the harmonic vibrational frequencies of major fragments, H2, CH, NH, OH, CN, N2, CO, NO, O2, CH2, NH2, H2O, HCN, HNC, HCO, HNO, O2H, CO2, NO2, CH3, NH3, CNH2, HCO2, HNO2, CH3N, CH3O, CH3NO, CH3ON, CH2NO2, and their anions, when the latter exist. Fragmentation energies obtained at both levels of theory are rather close to each other, except for channels …

Evolution Of The Electronic Structure And Properties Of Neutral And Charged Aluminum Clusters: A Comprehensive Analysis, B. K. Rao, P. Jena

Physics Publications

Density-functional theory with generalized gradient approximation for the exchange-correlation potential has been used to calculate the global equilibrium geometries and electronic structure of neutral, cationic, and anionic aluminumclusters containing up to 15 atoms. The total energies of these clusters are then used to study the evolution of their binding energy, relative stability, fragmentation channels, ionization potential, and vertical and adiabatic electron affinities as a function of size. The geometries are found to undergo a structural change from two dimensional to three dimensional when the cluster contains 6 atoms. An interior atom emerges only when clusters contain 11 or more atoms. …

Structure And Stability Of The Alx And Alx- Species, Gennady L. Gutsev, Puru Jena, Rodney J. Bartlett

Physics Publications

The electronic and geometrical structures of the ground and low-lying excited states of the diatomic AlX and AlX− series (X=H, Li, Be, B, C, N, O, and F) are calculated by the coupled-cluster method with all singles and doubles and noniterative inclusion of triples using a large atomic natural orbital basis. All the ground-state AlX molecules except for AlF can attach an additional electron and form ground-state AlX− anions. The ground-state AlBe−, AlB−, AlC−, AlN−, and AlO− anions possess excited states that are stable toward autodetachment of an extra electron; AlBe− also has a second excited state. Low-lying excited states …

Search For “Quadrupole-Bound” Anions. I, Gennady L. Gutsev, Puru Jena, Rodney J. Bartlett

Physics Publications

In a classical model, some anions exist due to the attraction between an electron and a molecule’s dipole moment. When the dipole moment is sufficiently large (μcrit>2.5 D), an electron can be trapped. Can a sufficiently large quadrupole moment produce the same effect? To help answer this question, we can search for molecules with a large quadrupole moment and use predictive, ab initio, correlated quantum chemistry methods to assess whether an anion forms and, if it does, to discover its nature. For this purpose, coupled-cluster calculations are reported for the structure and properties of KnClm and KnCl−m (n,m=0–2). …

Dynamics And Instabilities Near The Glass Transition: From Clusters To Crystals, Saroj K. Nayak, Puru Jena, Keith D. Ball, R. Stephen Berry

Physics Publications

Molecular dynamics simulation has been used to explore the evolution, kinetics, and dynamics of a liquid–glass transition in clusters and bulk matter. We demonstrate a dynamical indicator that characterizes the onset of the glass transition in clusters and is consistent with other indicators of glass transitions in bulk systems. This criterion, based on changes in chaotic behavior as measured by the largest Liapunov exponent, reveals aspects of the microscopic processes associated with the phase change from liquid to glass, and provides a connection between the thermodynamic and dynamical behavior of systems and their multidimensional potential surfaces.

Atomic And Electronic Structure Of Neutral And Charged Sinom Clusters, Saroj K. Nayak, B. K. Rao, S. N. Khanna, P. Jena

Physics Publications

Using molecular orbital approach and the generalized gradient approximation in the density functional theory, we have calculated the equilibrium geometries, binding energies, ionization potentials, and vertical and adiabatic electron affinities of SinOm clusters (n⩽6,m⩽12). The calculations were carried out using both Gaussian and numerical form for the atomic basis functions. Both procedures yield very similar results. The bonding in SinOm clusters is characterized by a significant charge transfer between the Si and O atoms and is stronger than in conventional semiconductor clusters. The bond distances are much less sensitive to cluster size than seen for metallic clusters. Similarly, calculated energy …

A Lattice Model For Computing The Transmissivity Of The Cornea And Sclera, David B. Ameen, Marilyn F. Bishop, Tom Mcmullen

Physics Publications

Abstract

The method of photonic band structure is used to calculate the frequencies of light that propagate in lattice models of the cornea and sclera of the mammalian eye, providing an explanation for transparency in the cornea that first properly accounts for multiple scattering of light. Each eye tissue is modeled as an ordered array of collagen rods, and photonic band structure methods are used to solve Maxwell's equations exactly for these models, a procedure that automatically effectively includes all orders of multiple scattering. These calculations show that the dispersion relation for the cornea is linear in the visible range, …

Atomic And Electronic Structures Of Neutral And Charged Boron And Boron-Rich Clusters, J. Niu, B. K. Rao, P. Jena

Physics Publications

Ab initio molecular orbital theory based on both density functional formalism and quantum chemical methods has been used to calculate the equilibrium geometries, binding energies, ionization potentials, fragmentation patterns, and electronic structures of neutral and charged boron clusters containing up to six atoms. Calculations have also been performed on restricted geometries for BnX (n=1,5,12; X=Be, B, C) and B20 clusters to see if clusters can be designed so as to increase their stability. Energetics of doubly chargedB++n clusters have also been studied to find the critical size for Coulomb explosion. The results are compared with existing experimental and theoretical data.

Structure And Magnetism Of Multiphase Sm0.080co0.645fe0.276 Powders, V. G. Harris, M. Liou, B. N. Das, V. M. Browning, J. E. Snyder, M. Rubinstein, S. H. Lawrence, R. Littleton Iii, D. P. Pappas

Physics Publications

A Sm-poor mixture of Fe-substituted Sm₂Co₁₇, having the nominal stoichiometry of Sm_0.080Co_0.645Fe_0.276, was ball-milled to explore the possibility of enhancing its remanence through direct microstructural refinement. With milling, the Sm₂(Co_0.7Fe_0.3)₁₇ compound disassociates to a body-centered-cubic supersaturated SmCoFe solid solution and a residual SmCoFe amorphous phase. Correspondingly, the coercive field values first increase, peaking at 0.83 kOe after 180 min of milling, then decrease with continued milling to

Equilibrium Structure And Bonding Of Small Iron-Carbon Clusters, Beth K. Nash, B. K. Rao, Puru Jena

Physics Publications

The equilibrium geometries, binding energies, and electronic structure of neutral FeC _n (n≤3) clusters have been calculated self‐consistently using ab initio molecular orbital theory. The exchange and correlation contributions to the total energy were computed using both the density functional method (with and without nonlocal correction) as well as the Hartree–Fock–Möller–Plesset theory. All levels of theory predict the equilibrium geometries to be cyclic. The binding energies, bond lengths, and the Mulliken charges obtained from both methods of calculations are also in agreement. The results are compared with recent mobility and photoelectron spectroscopy experiments.

A Fast Serial Algorithm For The Finite Temperature Quenched Potts Model, Gregory N. Hassold, Elizabeth A. Holm

Physics Publications

An efficient serial algorithm for finite temperature, quenched Potts model simulations of domain evolution has been developed. This ''n‐fold way'' algorithm eliminates unsuccessful spin flip attempts a priori by flipping sites with a frequency proportional to their site activity, defined as the sum of the probability of success for every possible spin flip at that site. Finite temperature efficiency for high‐spin degeneracy systems is achieved by utilizing a new, analytical expression for the portion of the site activity due to flips to non-neighbor spin values. Hence, to determine the activity of a site, only flips to the …

Phenomenological Theory Of Cuprate Superconductivity, Mario Rabinowitz, T. Mcmullen

Physics Publications

Reasonably good agreement with the superconducting transitiontemperatures of the cuprate high‐T _c superconductors can be obtained on the basis of an approximate phenomenological theory. In this theory, two criteria are used to calculate the superconducting transitiontemperature. One is that the quantum wavelength is of the order of the electron‐pair spacing. The other is that a fraction of the normal carriers exist as Cooper pairs at T _c . The resulting simple equation for T _c contains only two parameters: the normal carrier density and effective mass. We calculate specific transition temperatures for 12 cuprate superconductors.

Molecular View Of The Interfacial Adhesion In Aluminum‐Silicon Carbide Metal‐Matrix Composites, B. K. Rao, Puru Jena

Physics Publications

The binding energies, electron charge transfer,bond lengths, and core level shifts of Al‐Al, Al‐Si, Al‐C, and Si‐C dimers have been calculated self‐consistently using the linear combination of atomic orbitals‐molecular orbital theory. The exchange interactions are treated using the unrestricted Hartree–Fock theory and correlation corrections are included through the Möller–Plesset perturbation scheme up to fourth order. The results are used to understand the nature and strength of bonding at the interface of Al and SiC crystals. The strong bonding of Al‐C dimers compared to Al‐Al and Al‐Si is shown to be responsible for the aluminumcarbide formation at the interface. The charge …

Effect Of Size And Dimensionality On The Magnetic Moment Of Transition Metals, Feng Liu, S. N. Khanna, P. Jena

Physics Publications

The effect of size and dimensionality on the magnetic moments of Fe, Co, and Ni have been studied theoretically by confining the atoms to various structural forms such as chains, surfaces, and thin films. The size of these systems is controlled by limiting the number of atoms. A new first‐principles theory is developed that enables us to study the electron spin density of states and moments of atoms in clusters containing two to a few thousand atoms. The theory is based upon the elementary principles governing the tight binding and linear combination of atomic orbitals formulations. It contains no adjustable …

Calculations Of Scattered Light From Rigid Polymers By Shifrin And Rayleigh-Debye Approximations, M. F. Bishop

Physics Publications

ABSTRACT

We show that the commonly used Rayleigh-Debye method for calculating light scattering can lead to significant errors when used for describing scattering from dilute solutions of long rigid polymers, errors that can be overcome by use of the easily applied Shifrin approximation. In order to show the extent of the discrepancies between the two methods, we have performed calculations at normal incidence both for polarized and unpolarized incident light with the scattering intensity determined as a function of polarization angle and of scattering angle, assuming that the incident light is in a spectral region where the absorption of hemoglobin …

Optical And Electrochemical Studies Of Passive Film Formation In Amorphous Ni‐Cr‐P‐C Alloys, D. B. Hagan, B. W. Sloope, V. A. Niculescu

Physics Publications

The investigation of passivation of an amorphous Ni‐l4Cr‐17P‐0.5C alloy in lN H₂ SO₄ through anodic polarization and near‐normal optical reflectance is reported. It was found that the alloy passivates with a current density of 10^{− 1} A/m² extending to 1.0 V with current density dependent upon surface morphology. In the transpassive region under constant current density conditions the reflectance of the film exhibits strong interference phenomena and overall exponential decay in intensity. The behavior of the system in this region is described with a single thin‐film optical model consistent with the formation of a chromium …

Gravity‐Induced Density And Concentration Profiles In Binary Mixtures Near Gas–Liquid Critical Lines, R. F. Chang, J. M. H. Levelt Sengers, T. Doiron, J. Jones

Physics Publications

We have calculated gravity‐induced density and concentration gradients using scaled equations of state fashioned after that of Leung and Griffiths for binary mixtures near gas–liquid critical lines. The mixtures considered here are those of helium‐3 and helium‐4 and of carbon dioxide and ethane. Our calculations show that the density profiles for both mixtures in any proportion of the components are similar to those of pure fluids. The concentration gradients in the helium mixture have the same appearance as the density gradients. In the carbon dioxide–ethane system, however, the form of the concentration profile varies greatly, depending on the overall composition. …

Effective Field Model For Ising Ferromagnets: Influence Of Triplet Correlations, G. B. Taggart

Physics Publications

We use an effective field model which explicitly incorporates correlations to determine the critical temperatures for Ising ferromagnets on the common lattices. We specifically retain only the first nontrivial odd correlation function, i.e., the triplet correlation function, while neglecting higher order correlations. Within this approximation, assuming the equivalence of triplet correlations involving both central and noncentral sites in the nearest neighbor cluster yields values for the critical temperature below the Bethe approximations for z⩾4. Likewise, assuming the inequivalence of triplet correlations involving the central and noncentral sites yields values of the critical temperature only slightly higher than the Bethe approximation …

Laf3 Insulators For Mis Structures, A. Sher, W. E. Miller, Y. H. Tsuo, John A. Moriarty, R. K. Crouch, B. A. Seiber

Physics Publications

Thin films of Laf₃ deposited on Si or GaAs substrates have been observed to form blocking contacts with very high capacitances. This results in comparatively‐hysteresis‐free and sharpC‐V (capacitance‐voltage) characteristics for MIS structures. Such structures have been used to study the interface states of GaAs with increased resolution and to construct improved photocapacitive infrared detectors.