1,953 research outputs found
First-principles theory of ferroelectric phase transitions for perovskites: The case of BaTiO3
We carry out a completely first-principles study of the ferroelectric phase
transitions in BaTiO. Our approach takes advantage of two features of these
transitions: the structural changes are small, and only low-energy distortions
are important. Based on these observations, we make systematically improvable
approximations which enable the parameterization of the complicated energy
surface. The parameters are determined from first-principles total-energy
calculations using ultra-soft pseudopotentials and a preconditioned
conjugate-gradient scheme. The resulting effective Hamiltonian is then solved
by Monte Carlo simulation. The calculated phase sequence, transition
temperatures, latent heats, and spontaneous polarizations are all in good
agreement with experiment. We find the transitions to be intermediate between
order-disorder and displacive character. We find all three phase transitions to
be of first order. The roles of different interactions are discussed.Comment: 33 pages latex file, 9 figure
Structure and apparent topography of TiO2 (110) surfaces
We present self-consistent ab-initio total-energy and electronic-structure
calculations on stoichiometric and non-stoichiometric TiO2 (110) surfaces.
Scanning tunneling microscopy (STM) topographs are simulated by calculating the
local electronic density of states over an energy window appropriate for the
experimental positive-bias conditions. We find that under these conditions the
STM tends to image the undercoordinated Ti atoms, in spite of the physical
protrusion of the O atoms, giving an apparent reversal of topographic contrast
on the stoichiometric 1x1 or missing-row 2x1 surface. We also show that both
the interpretation of STM images and the direct comparison of surface energies
favor an added-row structure over the missing-row structure for the
oxygen-deficient 2x1 surface.Comment: 6 pages, two-column style with 5 postscript figures embedded. Uses
REVTEX and epsf macros. Also available at
http://www.physics.rutgers.edu/~dhv/preprints/index.html#ng_tio
Electronic structure of periodic curved surfaces -- continuous surface versus graphitic sponge
We investigate the band structure of electrons bound on periodic curved
surfaces. We have formulated Schr\"{o}dinger's equation with the Weierstrass
representation when the surface is minimal, which is numerically solved. Bands
and the Bloch wavefunctions are basically determined by the way in which the
``pipes'' are connected into a network, where the Bonnet(conformal)-transformed
surfaces have related electronic strucutres. We then examine, as a realisation
of periodic surfaces, the tight-binding model for atomic networks
(``sponges''), where the low-energy spectrum coincides with those for
continuous curved surfaces.Comment: 4 page
Accurate calculation of polarization-related quantities in semiconductors
We demonstrate that polarization-related quantities in semiconductors can be
predicted accurately from first-principles calculations using the appropriate
approach to the problem, the Berry-phase polarization theory. For III-V
nitrides, our test case, we find polarizations, polarization differences
between nitride pairs, and piezoelectric constants quite close to their
previously established values. Refined data are nevertheless provided for all
the relevant quantities.Comment: RevTeX 4 pages, no figure
First-principles study of (BiScO3){1-x}-(PbTiO3){x} piezoelectric alloys
We report a first-principles study of a class of (BiScO3)_{1-x}-(PbTiO3)_x
(BS-PT) alloys recently proposed by Eitel et al. as promising materials for
piezoelectric actuator applications. We show that (i) BS-PT displays very large
structural distortions and polarizations at the morphotropic phase boundary
(MPB) (we obtain a c/a of ~1.05-1.08 and P_tet of ~1.1 C/m^2); (ii) the
ferroelectric and piezoelectric properties of BS-PT are dominated by the onset
of hybridization between Bi/Pb-6p and O-2p orbitals, a mechanism that is
enhanced upon substitution of Pb by Bi; and (iii) the piezoelectric responses
of BS-PT and Pb(Zr_{1-x}Ti_x)O3 (PZT) at the MPB are comparable, at least as
far as the computed values of the piezoelectric coefficient d_15 are concerned.
While our results are generally consistent with experiment, they also suggest
that certain intrinsic properties of BS-PT may be even better than has been
indicated by experiments to date. We also discuss results for PZT that
demonstrate the prominent role played by Pb displacements in its piezoelectric
properties.Comment: 6 pages, with 3 postscript figures embedded. Uses REVTEX and epsf
macros. Also available at
http://www.physics.rutgers.edu/~dhv/preprints/ji_bi/index.htm
Modeling the momentum distributions of annihilating electron-positron pairs in solids
Measuring the Doppler broadening of the positron annihilation radiation or
the angular correlation between the two annihilation gamma quanta reflects the
momentum distribution of electrons seen by positrons in the
material.Vacancy-type defects in solids localize positrons and the measured
spectra are sensitive to the detailed chemical and geometric environments of
the defects. However, the measured information is indirect and when using it in
defect identification comparisons with theoretically predicted spectra is
indispensable. In this article we present a computational scheme for
calculating momentum distributions of electron-positron pairs annihilating in
solids. Valence electron states and their interaction with ion cores are
described using the all-electron projector augmented-wave method, and atomic
orbitals are used to describe the core states. We apply our numerical scheme to
selected systems and compare three different enhancement (electron-positron
correlation) schemes previously used in the calculation of momentum
distributions of annihilating electron-positron pairs within the
density-functional theory. We show that the use of a state-dependent
enhancement scheme leads to better results than a position-dependent
enhancement factor in the case of ratios of Doppler spectra between different
systems. Further, we demonstrate the applicability of our scheme for studying
vacancy-type defects in metals and semiconductors. Especially we study the
effect of forces due to a positron localized at a vacancy-type defect on the
ionic relaxations.Comment: Submitted to Physical Review B on September 1 2005. Revised
manuscript submitted on November 14 200
A real-space grid implementation of the Projector Augmented Wave method
A grid-based real-space implementation of the Projector Augmented Wave (PAW)
method of P. E. Blochl [Phys. Rev. B 50, 17953 (1994)] for Density Functional
Theory (DFT) calculations is presented. The use of uniform 3D real-space grids
for representing wave functions, densities and potentials allows for flexible
boundary conditions, efficient multigrid algorithms for solving Poisson and
Kohn-Sham equations, and efficient parallelization using simple real-space
domain-decomposition. We use the PAW method to perform all-electron
calculations in the frozen core approximation, with smooth valence wave
functions that can be represented on relatively coarse grids. We demonstrate
the accuracy of the method by calculating the atomization energies of twenty
small molecules, and the bulk modulus and lattice constants of bulk aluminum.
We show that the approach in terms of computational efficiency is comparable to
standard plane-wave methods, but the memory requirements are higher.Comment: 13 pages, 3 figures, accepted for publication in Physical Review
Spontaneous polarization and piezoelectric constants of III-V nitrides
The spontaneous polarization, dynamical Born charges, and piezoelectric
constants of the III-V nitrides AlN, GaN, and InN are studied ab initio using
the Berry phase approach to polarization in solids. The piezoelectric constants
are found to be up 10 times larger than in conventional III-V's and II-VI's,
and comparable to those of ZnO. Further properties at variance with those of
conventional III-V compounds are the sign of the piezoelectric constants
(positive as in II-VI's) and the very large spontaneous polarization.Comment: RevTeX 4 pages, improved upon revie
Dynamics of Phononic Dissipation at the Atomic Scale: Dependence on Internal Degrees of Freedom
Dynamics of dissipation of a local phonon distribution to the substrate is a
key issue in friction between sliding surfaces as well as in boundary
lubrication. We consider a model system consisting of an excited nano-particle
which is weakly coupled with a substrate. Using three different methods we
solve the dynamics of energy dissipation for different types of coupling
between the nano-particle and the substrate, where different types of
dimensionality and phonon densities of states were also considered for the
substrate. In this paper, we present our analysis of transient properties of
energy dissipation via phonon discharge in the microscopic level towards the
substrate. Our theoretical analysis can be extended to treat realistic
lubricant molecules or asperities, and also substrates with more complex
densities of states. We found that the decay rate of the nano-particle phonons
increases as the square of the interaction constant in the harmonic
approximation.Comment: 10 pages, 6 figures, submitted to Phys. Rev.
Fermi level alignment in molecular nanojunctions and its relation to charge transfer
The alignment of the Fermi level of a metal electrode within the gap of the
hi ghest occupied (HOMO) and lowest unoccupied orbital (LUMO) of a molecule is
a key quantity in molecular electronics, which can vary the electron
transparency of a single molecule junction by orders of magnitude. We present a
quantitative analysis of the relation between this level alignment (which can
be estimated from charging free molecules) and charge transfer for bipyridine
and biphenyl dithiolate (BPDT) molecules attached to gold leads based on
density functional theory calculations. For both systems the charge
distribution is defined by a balance between Pauli repulsion with subsequent
electrostatic screening and the filling of the LUMO, where bipyridine loses
electrons to the leads and BPDT gains electrons. As a direct consequence the
Fermi level of the metal is found close to the LUMO for bipyridine and close to
the HOMO for BPDT
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