The limitations of Slater's element-dependent exchange functional from analytic density functional theory

Our recent formulation of the analytic and variational Slater-Roothaan (SR) method, which uses Gaussian basis sets to variationally express the molecular orbitals, electron density and the one body effective potential of density functional theory, is reviewed. Variational fitting can be extended to the resolution of identity method,where variationality then refers to the error in each two electron integral and not to the total energy. It is proposed that the appropriate fitting functions be charge neutral and that all ab initio energies be evaluated using two-center fits of the two-electron integrals. The SR method has its root in the Slater's Xalpha method and permits an arbitrary scaling of the Slater-Gaspar-Kohn-Sham exchange-correlation potential around each atom in the system. Of several ways of choosing the scaling factors (Slater's exchange parameters), two most obvious are the Hartree-Fock (HF), alpha_HF, values and the exact atomic, alpha_EA, values. The performance of this simple analytic model with both sets for atomization energies of G2 set of 148 molecules is better than the local density approximation or the HF theory, although the errors in atomization energy are larger than the target chemical accuracy. To improve peformance for atomization energies, the SR method is reparametrized to give atomization energies of 148 molecules to be comparbale to those obtained by one of the most widely used generalized gradient approximations. The mean absolute error in ionization potentials of 49 atoms and molecules is about 0.5 eV and that in bond distances of 27 molecules is about 0.02 Angstrom. The overall good performance of the computationally efficient SR method using any reasonable set of alpha values makes it a promising method for study of large systems.Comment: 33 pages, Uses RevTex, to appear in The Journal of Chemical Physic

Accurate molecular energies by extrapolation of atomic energies using an analytic quantum mechanical model

Using a new analytic quantum mechanical method based on Slater's Xalpha method, we show that a fairly accurate estimate of the total energy of a molecule can be obtained from the exact energies of its constituent atoms. The mean absolute error in the total energies thus determined for the G2 set of 56 molecules is about 16 kcal/mol, comparable to or better than some popular pure and hybrid density functional models.Comment: 5 pages, REVTE

Static dielectric response of icosahedral fullerenes from C60 to C2160 by an all electron density functional theory

The static dielectric response of C60, C180, C240, C540, C720, C960, C1500, and C2160 fullerenes is characterized by an all-electron density-functional method. First, the screened polarizabilities of C60, C180, C240, and C540, are determined by the finite-field method using Gaussian basis set containing 35 basis functions per atom. In the second set of calculations, the unscreened polarizabilities are calculated for fullerenes C60 through C2160 from the self-consistent Kohn-Sham orbitals and eigen-values using the sum-over-states method. The approximate screened polarizabilities, obtained by applying a correction determined within linear response theory show excellent agreement with the finite-field polarizabilities. The static dipole polarizability per atom in C2160 is (4 Angstrom^3) three times larger than that in C60 (1.344 Angstrom^3). Our results reduce the uncertainty in various theoretical models used previously to describe the dielectric response of fullerenes and show that quantum size effects in polarizability are significantly smaller than previously thought.Comment: RevTex, 3 figure

High Frequency (4th order) Sequence Stratigraphy of Early Miocene Deltaic Shorelines, Offshore Texas and Louisiana

DOE-NETL Award Numbers DE-FE0026083 and DEFE0029487Bureau of Economic Geolog

Effect of nonlinearity on the dynamics of a particle in dc field-induced systems

Dynamics of a particle in a perfect chain with one nonlinear impurity and in a perfect nonlinear chain under the action of dc field is studied numerically. The nonlinearity appears due to the coupling of the electronic motion to optical oscillators which are treated in adiabatic approximation. We study for both the low and high values of field strength. Three different range of nonlinearity is obtained where the dynamics is different. In low and intermediate range of nonlinearity, it reduces the localization. In fact in the intermediate range subdiffusive behavior in the perfect nonlinear chain is obtained for a long time. In all the cases a critical value of nonlinear strength exists where self-trapping transition takes place. This critical value depends on the system and the field strength. Beyond the self-trapping transition nonlinearity enhances the localization.Comment: 9 pages, Revtex, 6 ps figures include

Scaling Properties of 1D Anderson Model with Correlated Diagonal Disorder

Statistical and scaling properties of the Lyapunov exponent for a tight-binding model with the diagonal disorder described by a dichotomic process are considered near the band edge. The effect of correlations on scaling properties is discussed. It is shown that correlations lead to an additional parameter governing the validity of single parameter scaling.Comment: 5 pages, 3 figures, RevTe

Stationary Localized States Due to a Nonlinear Dimeric Impurity Embedded in a Perfect 1-D Chain

The formation of Stationary Localized states due to a nonlinear dimeric impurity embedded in a perfect 1-d chain is studied here using the appropriate Discrete Nonlinear Schr$\ddot{o}$dinger Equation. Furthermore, the nonlinearity has the form, $\chi |C|^\sigma$ where $C$ is the complex amplitude. A proper ansatz for the Localized state is introduced in the appropriate Hamiltonian of the system to obtain the reduced effective Hamiltonian. The Hamiltonian contains a parameter, $\beta = \phi_1/\phi_0$ which is the ratio of stationary amplitudes at impurity sites. Relevant equations for Localized states are obtained from the fixed point of the reduced dynamical system. $|\beta|$ = 1 is always a permissible solution. We also find solutions for which $|\beta| \ne 1$. Complete phase diagram in the $(\chi, \sigma)$ plane comprising of both cases is discussed. Several critical lines separating various regions are found. Maximum number of Localized states is found to be six. Furthermore, the phase diagram continuously extrapolates from one region to the other. The importance of our results in relation to solitonic solutions in a fully nonlinear system is discussed.Comment: Seven figures are available on reques

Topological Phases in Graphitic Cones

The electronic structure of graphitic cones exhibits distinctive topological features associated with the apical disclinations. Aharonov-Bohm magnetoconductance oscillations (period Phi_0) are completely absent in rings fabricated from cones with a single pentagonal disclination. Close to the apex, the local density of states changes qualitatively, either developing a cusp which drops to zero at the Fermi energy, or forming a region of nonzero density across the Fermi energy, a local metalization of graphene.Comment: 4 pages, RevTeX 4, 3 PostScript figure

Solution of the relativistic Dirac-Hulthen problem

The one-particle three-dimensional Dirac equation with spherical symmetry is solved for the Hulthen potential. The s-wave relativistic energy spectrum and two-component spinor wavefunctions are obtained analytically. Conforming to the standard feature of the relativistic problem, the solution space splits into two distinct subspaces depending on the sign of a fundamental parameter in the problem. Unique and interesting properties of the energy spectrum are pointed out and illustrated graphically for several values of the physical parameters. The square integrable two-component wavefunctions are written in terms of the Jacobi polynomials. The nonrelativistic limit reproduces the well-known nonrelativistic energy spectrum and results in Schrodinger equation with a "generalized" three-parameter Hulthen potential, which is the sum of the original Hulthen potential and its square.Comment: 13 pages, 3 color figure

Coil Formation in Multishell Carbon Nanotubes: Competition between Curvature Elasticity and Interlayer Adhesion

To study the shape formation process of carbon nanotubes, a string equation describing the possible existing shapes of the axis-curve of multishell carbon tubes (MCTs) is obtained in the continuum limit by minimizing the shape energy, that is the difference between the MCT energy and the energy of the carbonaceous mesophase (CM). It is shown that there exists a threshold relation of the outmost and inmost radii, that gives a parameter regime in which a straight MCT will be bent or twisted. Among the deformed shapes, the regular coiled MCTs are shown being one of the solutions of the string equation. In particular,the optimal ratio of pitch $p$ and radius $r_0$ for such a coil is found to be equal to $2\pi$, which is in good agreement with recent observation of coil formation in MCTs by Zhang et al.Comment: RevTeX, no figure, 12 pages, to appear in Phys. Rev. Let