24 research outputs found
First-principles extrapolation method for accurate CO adsorption energies on metal surfaces
We show that a simple first-principles correction based on the difference
between the singlet-triplet CO excitation energy values obtained by DFT and
high-level quantum chemistry methods yields accurate CO adsorption properties
on a variety of metal surfaces.
We demonstrate a linear relationship between the CO adsorption energy and the
CO singlet-triplet splitting, similar to the linear dependence of CO adsorption
energy on the energy of the CO 2* orbital found recently {[Kresse {\em et
al.}, Physical Review B {\bf 68}, 073401 (2003)]}. Converged DFT calculations
underestimate the CO singlet-triplet excitation energy ,
whereas coupled-cluster and CI calculations reproduce the experimental . The dependence of on is used
to extrapolate for the top, bridge and hollow sites for the
(100) and (111) surfaces of Pt, Rh, Pd and Cu to the values that correspond to
the coupled-cluster and CI value. The correction
reproduces experimental adsorption site preference for all cases and obtains
in excellent agreement with experimental results.Comment: Table sent as table1.eps. 3 figure
Influence of uniaxial tensile stress on the mechanical and piezoelectric properties of short-period ferroelectric superlattice
Tetragonal ferroelectric/ferroelectric BaTiO3/PbTiO3 superlattice under
uniaxial tensile stress along the c axis is investigated from first principles.
We show that the calculated ideal tensile strength is 6.85 GPa and that the
superlattice under the loading of uniaxial tensile stress becomes soft along
the nonpolar axes. We also find that the appropriately applied uniaxial tensile
stress can significantly enhance the piezoelectricity for the superlattice,
with piezoelectric coefficient d33 increasing from the ground state value by a
factor of about 8, reaching 678.42 pC/N. The underlying mechanism for the
enhancement of piezoelectricity is discussed
First-principles study of the structural energetics of PdTi and PtTi
The structural energetics of PdTi and PtTi have been studied using
first-principles density-functional theory with pseudopotentials and a
plane-wave basis. We predict that in both materials, the experimentally
reported orthorhombic phase will undergo a low-temperature phase
transition to a monoclinic ground state. Within a soft-mode framework,
we relate the structure to the cubic structure, observed at high
temperature, and the structure to via phonon modes strongly
coupled to strain. In contrast to NiTi, the structure is extremely close
to hcp. We draw on the analogy to the bcc-hcp transition to suggest likely
transition mechanisms in the present case.Comment: 8 pages 5 figure
Real-space local polynomial basis for solid-state electronic-structure calculations: A finite-element approach
We present an approach to solid-state electronic-structure calculations based
on the finite-element method. In this method, the basis functions are strictly
local, piecewise polynomials. Because the basis is composed of polynomials, the
method is completely general and its convergence can be controlled
systematically. Because the basis functions are strictly local in real space,
the method allows for variable resolution in real space; produces sparse,
structured matrices, enabling the effective use of iterative solution methods;
and is well suited to parallel implementation. The method thus combines the
significant advantages of both real-space-grid and basis-oriented approaches
and so promises to be particularly well suited for large, accurate ab initio
calculations. We develop the theory of our approach in detail, discuss
advantages and disadvantages, and report initial results, including the first
fully three-dimensional electronic band structures calculated by the method.Comment: replacement: single spaced, included figures, added journal referenc
First-principles thermodynamics of transition metals and alloys: W, NiAl, PdTi
We apply the pseudopotential density functional perturbation theory approach
along with the quasiharmonic approximation to calculate the thermal expansion
of tungsten and two important metallic alloys, NiAl and PdTi. We derive the
theory for anisotropic crystal structures and test the approximation that the
anisotropic effects of thermal expansion are equivalent to negative pressure -
this simplifies the calculation enormously for complex structures. Throughout,
we find excellent agreement with experimental results.Comment: 11 pages 9 fig
Construction and solution of a Wannier-functions based Hamiltonian in the pseudopotential plane-wave framework for strongly correlated materials
Ab initio determination of model Hamiltonian parameters for strongly
correlated materials is a key issue in applying many-particle theoretical tools
to real narrow-band materials. We propose a self-contained calculation scheme
to construct, with an ab initio approach, and solve such a Hamiltonian. The
scheme uses a Wannier-function-basis set, with the Coulomb interaction
parameter U obtained specifically for these Wannier functions via constrained
Density functional theory (DFT) calculations. The Hamiltonian is solved by
Dynamical Mean-Field Theory (DMFT) with the effective impurity problem treated
by the Quantum Monte Carlo (QMC) method. Our scheme is based on the
pseudopotential plane-wave method, which makes it suitable for developments
addressing the challenging problem of crystal structural relaxations and
transformations due to correlation effects. We have applied our scheme to the
"charge transfer insulator" material nickel oxide and demonstrate a good
agreement with the experimental photoemission spectra
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Correlated Wavefunction Monte Carlo Studies of Excitations in the Quantum Hall Liquids
Enhancing ferroelectric photovoltaic effect by polar order engineering
10.1126/sciadv.aat3438Science Advances47eaat343