Spatially dependent correlation functions in the Anderson model

We report results from a first principles calculation of spatially dependent correlation functions around a magnetic impurity in metals described by the nondegenerate Anderson model. Our computations are based on a combination of perturbative scaling theory and numerical renormalization group methods. Results for the conduction election charge density around the impurity and correlation functions involving the conduction electron and impurity charge and spin densities will be presented. The behavior in various regimes including the mixed valent regime will be explored.

A Comprehensive Theory of Erosive Burning in Solid Rocket Propeilants

The theory of erosive burning has been constructed front first principles using turbulent boundary layer concepts. It is shown that the problem constitutes one of solution of flame propagation equation for turbulent flow. The final approximate solution for the case of single step overall kinetics reveals the combined effects of fluid mechanics and chemical kinetics. The results obtained from this theory are compared with earlier experimental results. The dependence of erosive burning characteristics on various parameters has been elucidated.

A Microscopic Theory of the f.c.c.-b.c.c. Interface .

We present a first-principles theory of the equilibrium b.c.c.-f.c.c. interface at coexistence using the density functional method. We assume that the interfacial region has local body-centred tetragonal (b.c.t.) symmetry and predict typical interfacial widths to be of order 2 to 3 lattice spacings with typical energies close to 0.05 J/m2. These quantities are in good agreement with laboratory measurements on coherent interfaces.

A simplified kinetic model for oxidative dehydrogenation of ethylbenzene over Pd-NaBr/Al2O3 catalyst

The oxidative dehydrogenation of ethylbenzene is gaining considerable importance in recent years as a promising alternative for styrene production. This vapour phase reaction has been studied over Pd-NaBr/Al2O3 catalyst in the temperature range 623-793 K in a fixed bed reactor. Kinetic analysis of this reaction has been done using a recursion procedure developed in this work from first principles. The advantage of this method is the absence of any restriction on the conversion level as it uses an integrated rate equation. The rate of styrene formation was found to follow a linear relationship with concentration of ethylbenzene and shows a Langmuir type dependence on the concentration of oxygen.

Origin of magnetism and trend in T-c in Cr-based double perovskites: Interplay of two driving mechanisms

Hamiltonian constructed in a first principles manner, we explored the origin of magnetism and the T-c trend in Cr-based double perovskite series, Sr2CrB'O-6 (B' = W/Re/Os). Our study shows that the apparently puzzling T-c trend in Sr2CrB'O-6 (B' = W/Re/Os) series can be understood in terms of the interplay of the hybridization driven mechanism and the superexchange mechanism.

Molecular interpretation of the linear relationship between the entropy and the enthalpy of activation of charge transfer reactions in polar liquids

The well-known linear relationship (T?S# =??H# +?, where 1 >? > 0,? > 0) between the entropy (?S#) and the enthalpy (?H#) of activation for reactions in polar liquids is investigated by using a molecular theory. An explicit derivation of this linear relation from first principles is presented for an outersphere charge transfer reaction. The derivation offers microscopic interpretation for the quantities? and?. It has also been possible to make connection with and justify the arguments of Bell put forward many years ago.

Muon-spin rotation spectra in the mixed phase of high-T-c superconductors: Thermal fluctuations and disorder effects

We study muon-spin rotation (mu SR) spectra in the mixed phase of highly anisotropic layered superconductors, specifically Bi2+xSr2-xCaCu2O8+delta (BSCCO), by modeling the fluid and solid phases of pancake Vortices using liquid-state and density functional methods. The role of thermal fluctuations in causing motional narrowing of mu SR line shapes is quantified in terms of a first-principles theory of the flux-lattice melting transition. The effects of random point pinning are investigated using a replica treatment of liquid-state correlations and a replicated density functional theory. Our results indicate that motional narrowing in the pure system, although substantial, cannot account for the remarkably small linewidths obtained experimentally at relatively high fields and low temperatures. We find that satisfactory agreement with the mu SR data for BSCCO in this regime can be obtained through the ansatz that this ''phase'' is characterized by frozen short-range positional correlations reflecting the structure of the liquid just above the melting transition. This proposal is consistent with recent suggestions of a ''pinned liquid'' or ''glassy'' state of pancake Vortices in the presence of pinning disorder. Our results for the high-temperature liquid phase indicate that measurable linewidths may be obtained in this phase as a consequence of density inhomogeneities induced by the pinning disorder. The results presented here comprise a unified, first-principles theoretical treatment of mu SR spectra in highly anisotropic layered superconductors in terms of a controlled set of approximations. [S0163-1829(99)08033-9].

CO adsorption on ionic Pt, Pd and Cu sites in Ce(1-x)M(x)O(2-delta) (M = Pt(2+), Pd(2+), Cu(2+))

Noble metal ion substituted CeO(2) in the form of Ce(0.98)M(0.02)O(2-delta) solid solution (where M = Pt, Pd, Cu) are the new generation catalysts with applications in three-way exhaust catalysis. While adsorption of CO on noble metals ions is well-known, adsorption of CO on noble metal ions has not been studied because creating exclusive ionic sites has been difficult. Using first-principles density functional theory (DFT) we have shown that CO gets adsorbed on the noble metal Pt(2+), Pd(2+), Cu(2+) ionic sites in the respective compounds, and the net energy of the overall system decreases. Adsorption of CO on metal ions is also confirmed by Fourier transform infrared spectroscopy (FTIR).

Magnetoelectric Effect in L1(0)-CoPd Thin Films

The effect of an applied electric field on the magnetic properties of L1(0)-ordered CoPd thin films is investigated by first-principle calculations. Both the magnetic moment and the magnetocrystalline anisotropy of the surface atoms are changed by the electric field, but the net effect depends on the surface termination. The magnetocrystalline anisotropy switches from in-plane to perpendicular in the presence of external electric field. Typical magnetic-moment changes are 0.1 mu(B) per eV/angstrom The main mechanism is the shift of the Fermi level, but the anisotropy change also reflects a crystal-field change due to incomplete screening.

LOCAL TWO-DIMENSIONAL PARTICLE-IN-CELL SIMULATIONS OF THE COLLISIONLESS MAGNETOROTATIONAL INSTABILITY

The magnetorotational instability (MRI) is a crucial mechanism of angular momentum transport in a variety of astrophysical accretion disks. In systems accreting at well below the Eddington rate, such as the central black hole in the Milky Way (Sgr A*), the plasma in the disk is essentially collisionless. We present a nonlinear study of the collisionless MRI using first-principles particle-in-cell plasma simulations. We focus on local two-dimensional (axisymmetric) simulations, deferring more realistic three-dimensional simulations to future work. For simulations with net vertical magnetic flux, the MRI continuously amplifies the magnetic field, B, until the Alfven velocity, v(A), is comparable to the speed of light, c (independent of the initial value of v(A)/c). This is consistent with the lack of saturation of MRI channel modes in analogous axisymmetric MHD simulations. The amplification of the magnetic field by the MRI generates a significant pressure anisotropy in the plasma (with the pressure perpendicular to B being larger than the parallel pressure). We find that this pressure anisotropy in turn excites mirror modes and that the volume-averaged pressure anisotropy remains near the threshold for mirror mode excitation. Particle energization is due to both reconnection and viscous heating associated with the pressure anisotropy. Reconnection produces a distinctive power-law component in the energy distribution function of the particles, indicating the likelihood of non-thermal ion and electron acceleration in collisionless accretion disks. This has important implications for interpreting the observed emission-from the radio to the gamma-rays-of systems such as Sgr A*.

Gap renormalization of molecular crystals from density-functional theory

Fundamental gap renormalization due to electronic polarization is a basic phenomenon in molecular crystals. Despite its ubiquity and importance, all conventional approaches within density-functional theory completely fail to capture it, even qualitatively. Here, we present a new screened range-separated hybrid functional, which, through judicious introduction of the scalar dielectric constant, quantitatively captures polarization-induced gap renormalization, as demonstrated on the prototypical organic molecular crystals of benzene, pentacene, and C-60. This functional is predictive, as it contains system-specific adjustable parameters that are determined from first principles, rather than from empirical considerations.

Li diffusion through doped and defected graphene

We investigate the effect of nitrogen and boron doping on Li diffusion through defected graphene using first principles based density functional theory. While a high energy barrier rules out the possibility of Li-diffusion through the pristine graphene, the barrier reduces with the incorporation of defects. Among the most common defects in pristine graphene, Li diffusion through the divacancy encounters the lowest energy barrier of 1.34 eV. The effect of nitrogen and boron doping on the Li diffusion through doped defected-graphene sheets has been studied. N-doping in graphene with a monovacancy reduces the energy barrier significantly. The barrier reduces with the increasing number of N atoms. On the other hand, for N doped graphene with a divacancy, Li binds in the plane of the sheet, with an enhanced binding energy. The B doping in graphene with a monovacancy leads to the enhancement of the barrier. However, in the case of B-doped graphene with a divacancy, the barrier reduces to 1.54 eV, which could lead to good kinetics. The barriers do not change significantly with B concentration. Therefore, divacancy, B and N doped defected graphene has emerged as a better alternative to pristine graphene as an anode material for Li ion battery.

Effect of high-temperature shock-wave compression on few-layer MoS2, WS2 and MoSe2

Exposure of few-layer MoS2, WS2 and MoSe2 to high-temperature shock waves causes morphological changes and a significant decrease in the interlayer separation between the (002) planes, the decrease being greatest in MoSe2. Raman spectra show softening of both the A(1g) and the E-2g(1) modes initially, followed by a slightly stiffening. Using first-principles density functional theoretical analysis of the response of few-layer MoS2 to shock waves, we propose that a combination of shear and uniaxial compressive deformation leads to flattening of MoS2 sheets which is responsible for the changes in the vibrational spectra. (C) 2013 Elsevier B.V. All rights reserved.

Entanglement entropy in higher derivative holography

We consider holographic entanglement entropy in higher derivative gravity theories. Recently Lewkowycz and Maldacena 1] have provided a method to derive the equations for the entangling surface from first principles. We use this method to compute the entangling surface in four derivative gravity. Certain interesting differences compared to the two derivative case are pointed out. For Gauss-Bonnet gravity, we show that in the regime where this method is applicable, the resulting equations coincide with proposals in the literature as well as with what follows from considerations of the stress tensor on the entangling surface. Finally we demonstrate that the area functional in Gauss-Bonnet holography arises as a counterterm needed to make the Euclidean action free of power law divergences.

Local structural disorder and its influence on the average global structure and polar properties in Na0.5Bi0.5TiO3

Na0.5Bi0.5TiO3 (NBT) and its derivatives have prompted a great surge in interest owing to their potential as lead-free piezoelectrics. In spite of five decades since its discovery, there is still a lack of clarity on crucial issues such as the origin of significant dielectric relaxation at room temperature, structural factors influencing its depoling, and the status of the recently proposed monoclinic (Cc) structure vis-a-vis the nanosized structural heterogeneities. In this work, these issues are resolved by comparative analysis of local and global structures on poled and unpoled NBT specimens using electron, x-ray, and neutron diffraction in conjunction with first-principles calculation, dielectric, ferroelectric, and piezoelectric measurements. The reported global monoclinic (Cc) distortion is shown not to correspond to the thermodynamic equilibrium state at room temperature. The global monocliniclike appearance rather owes its origin to the presence of local structural and strain heterogeneities. Poling removes the structural inhomogeneities and establishes a long-range rhombohedral distortion. In the process the system gets irreversibly transformed from a nonergodic relaxor to a normal ferroelectric state. The thermal depoling is shown to be associated with the onset of incompatible in-phase tilted octahedral regions in the field-stabilized long range rhombohedral distortion.