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

Distribution of averages in a correlated Gaussian medium as a tool for the estimation of the cluster distribution on size

Calculation of the distribution of the average value of a Gaussian random field in a finite domain is carried out for different cases. The results of the calculation demonstrate a strong dependence of the width of the distribution on the spatial correlations of the field. Comparison with the simulation results for the distribution of the size of the cluster indicates that the distribution of an average field could serve as a useful tool for the estimation of the asymptotic behavior of the distribution of the size of the clusters for "deep" clusters where value of the field on each site is much greater than the rms disorder.Comment: 15 pages, 6 figures, RevTe

Electronic and magnetic properties of some rare-earth dihydrides and dideuterides

Mössbauer spectroscopy has been used to study the electronic and magnetic properties of a number of rare-earth dihydrides and dideuterides. In stoichiometric ErH2 and DyH2, magnetic transitions and crystal field ground states have been established. In non-stoichiometric compounds DyH2+x and (Er)HoH2+x changes of the rare-earth point symmetry due to distributions in hydrogen site occupations are seen. This results in increases in the magnetic transition temperatures and distributions in the magnetic moments

Evidence from K2 for rapid rotation in the descendant of an intermediate-mass star

Using patterns in the oscillation frequencies of a white dwarf observed by K2, we have measured the fastest rotation rate, 1.13(02) hr, of any isolated pulsating white dwarf known to date. Balmer-line fits to follow-up spectroscopy from the SOAR telescope show that the star (SDSSJ0837+1856, EPIC 211914185) is a 13,590(340) K, 0.87(03) solar-mass white dwarf. This is the highest mass measured for any pulsating white dwarf with known rotation, suggesting a possible link between high mass and fast rotation. If it is the product of single-star evolution, its progenitor was a roughly 4.0 solar-mass main-sequence B star; we know very little about the angular momentum evolution of such intermediate-mass stars. We explore the possibility that this rapidly rotating white dwarf is the byproduct of a binary merger, which we conclude is unlikely given the pulsation periods observed.Comment: 5 pages, 4 figure, 1 table; accepted for publication in The Astrophysical Journal Letter

Magnetic relaxation in highly anisotropic systems

Using the Mori formalism, a general theory is developed for the calculation of paramagnetic relaxation effects in a general crystal field doublet. For systems with extreme magnetic anisotropy, the relaxation rates show a strong angular dependence, being severely peaked in a direction perpendicular to the magnetic easy axis. Application to the RRh/sub 4/B/sub 4/ (R = rare-earth) compounds is discussed. 5 refs

Localization Properties of Electronic States in Polaron Model of poly(dG)-poly(dC) and poly(dA)-poly(dT) DNA polymers

We numerically investigate localization properties of electronic states in a static model of poly(dG)-poly(dC) and poly(dA)-poly(dT) DNA polymers with realistic parameters obtained by quantum-chemical calculation. The randomness in the on-site energies caused by the electron-phonon coupling are completely correlated to the off-diagonal parts. In the single electron model, the effect of the hydrogen-bond stretchings, the twist angles between the base pairs and the finite system size effects on the energy dependence of the localization length and on the Lyapunov exponent are given. The localization length is reduced by the influence of the fluctuations in the hydrogen bond stretchings. It is also shown that the helical twist angle affects the localization length in the poly(dG)-poly(dC) DNA polymer more strongly than in the poly(dA)-poly(dT) one. Furthermore, we show resonance structures in the energy dependence of the localization length when the system size is relatively small.Comment: 6 pages, 6 figure

Quantitative analysis of regulatory flexibility under changing environmental conditions

The circadian clock controls 24-h rhythms in many biological processes, allowing appropriate timing of biological rhythms relative to dawn and dusk. Known clock circuits include multiple, interlocked feedback loops. Theory suggested that multiple loops contribute the flexibility for molecular rhythms to track multiple phases of the external cycle. Clear dawn- and dusk-tracking rhythms illustrate the flexibility of timing in Ipomoea nil. Molecular clock components in Arabidopsis thaliana showed complex, photoperiod-dependent regulation, which was analysed by comparison with three contrasting models. A simple, quantitative measure, Dusk Sensitivity, was introduced to compare the behaviour of clock models with varying loop complexity. Evening-expressed clock genes showed photoperiod-dependent dusk sensitivity, as predicted by the three-loop model, whereas the one- and two-loop models tracked dawn and dusk, respectively. Output genes for starch degradation achieved dusk-tracking expression through light regulation, rather than a dusk-tracking rhythm. Model analysis predicted which biochemical processes could be manipulated to extend dusk tracking. Our results reveal how an operating principle of biological regulators applies specifically to the plant circadian clock

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

Time evolution of models described by one-dimensional discrete nonlinear Schr\"odinger equation

The dynamics of models described by a one-dimensional discrete nonlinear Schr\"odinger equation is studied. The nonlinearity in these models appears due to the coupling of the electronic motion to optical oscillators which are treated in adiabatic approximation. First, various sizes of nonlinear cluster embedded in an infinite linear chain are considered. The initial excitation is applied either at the end-site or at the middle-site of the cluster. In both the cases we obtain two kinds of transition: (i) a cluster-trapping transition and (ii) a self-trapping transition. The dynamics of the quasiparticle with the end-site initial excitation are found to exhibit, (i) a sharp self-trapping transition, (ii) an amplitude-transition in the site-probabilities and (iii) propagating soliton-like waves in large clusters. Ballistic propagation is observed in random nonlinear systems. The effect of nonlinear impurities on the superdiffusive behavior of random-dimer model is also studied.Comment: 16 pages, REVTEX, 9 figures available upon request, To appear in Physical Review