186 research outputs found
Ferroelectric Phase Transitions from First Principles
An effective Hamiltonian for the ferroelectric transition in is
constructed from first-principles density-functional-theory total-energy and
linear-response calculations through the use of a localized, symmetrized basis
set of ``lattice Wannier functions.'' Preliminary results of Monte Carlo
simulations for this system show a first-order cubic-tetragonal transition at
660 K. The involvement of the Pb atom in the lattice instability and the
coupling of local distortions to strain are found to be particularly important
in producing the behavior characteristic of the transition. A
tentative explanation for the presence of local distortions experimentally
observed above is suggested. Further applications of this method to a
variety of systems and structures are proposed for first-principles study of
finite-temperature structural properties in individual materials.Comment: 14 pages, harvmac, 4 uuencoded figure
Chemical control of polar behavior in bicomponent short-period superlattices
Using first-principles density functional calculations, we study the
interplay of ferroelectricity and polar discontinuities in a range of 1-1 oxide
superlattices, built out of ferroelectric and paraelectric components. Studies
have been carried out for a varied choice of chemical composition of the
components. We find that, when polar interfaces are present, the polar
discontinuities induce off- centric movements in the ferroelectric layers, even
though the ferroelectric is only one unit cell thick. The distortions yield
non-switchable polarizations, with magnitudes comparable to those of the
corresponding bulk ferroelectrics. In contrast, in superlattices with no polar
discontinuity at the interfaces, the off-centric movements in the ferroelectric
layer are usually suppressed. The details of the behavior and functional
properties are, however, found to be sensitive to epitaxial strain, rotational
instabilities and second-order Jahn-Teller activity, and are therefore strongly
in uenced by the chemical composition of the paraelectric layer.Comment: 7 pages, 2 figure
Diffusive phase transitions in ferroelectrics and antiferroelectrics
In this paper, we present a microscopic model for heterogeneous ferroelectric
and an order parameter for relaxor phase. We write a Landau theory based on
this model and its application to ferroelectric PbFeTaO
(PFT) and antiferroelectric NaNbO:Gd. We later discuss the coupling between
soft mode and domain walls, soft mode and quasi-local vibration and resulting
susceptibility function.Comment: 6 pages, Fundamental physics of ferroelectrics 200
Lattice dynamics of BaTiO3, PbTiO3 and PbZrO3: a comparative first-principles study
The full phonon dispersion relations of lead titanate and lead zirconate in
the cubic perovskite structure are computed using first-principles variational
density-functional perturbation theory, with ab initio pseudopotentials and a
plane-wave basis set. Comparison with the results previously obtained for
barium titanate shows that the change of a single constituent (Ba to Pb, Ti to
Zr) has profound effects on the character and dispersion of unstable modes,
with significant implications for the nature of the phase transitions and the
dielectric and piezoelectric responses of the compounds. Examination of the
interatomic force constants in real space, obtained by a transformation which
correctly treats the long-range dipolar contribution, shows that most are
strikingly similar, while it is the differences in a few key interactions which
produce the observed changes in the phonon dispersions. These trends suggest
the possibility of the transferability of force constants to predict the
lattice dynamics of perovskite solid solutions.Comment: 9 pages, 2 figures (one in colors), revised version (small changes
essentially in Sec. III
Magnetic-induced phonon anisotropy in ZnCrO from first principles
We have studied the influence of magnetic order on the optical phonons of the
geometrically frustrated spinel ZnCrO from first-principles. By mapping
the first-principles phonon calculations onto a Heisenberg-like model, we
developed a method to calculate exchange derivatives and subsequently the
spin-phonon couping parameter from first-principles. All calculations were
performed within LSDA+U
Ab initio statistical mechanics of the ferroelectric phase transition in PbTiO<SUB>3</SUB>
An effective Hamiltonian for the ferroelectric transition in PbTiO3 is constructed from ab initio pseudopotential local-density-functional total-energy and linear-response calculations through the use of a localized, symmetrized basis set of "lattice Wannier functions''. Explicit parametrization of the polar lattice Wannier functions is used for subspace projection, addressing the issues of LO-TO splitting and coupling to the complementary subspace. In contrast with ferroelectric BaTiO3 and KNbO3, we find significant involvement of the Pb atom in the lattice instability. Monte Carlo simulations for this Hamiltonian show a first-order cubic-tetragonal transition at 660 K. The resulting temperature dependence of spontaneous polarization, c/a ratio, and unit-cell volume near the transition are in good agreement with experiment. Comparison of Monte Carlo results with mean-field theory analysis shows that both strain and fluctuations are necessary to produce the first-order character of this transition
Interaction of small gold clusters with carbon nanotube bundles: formation of gold atomic chains
We use first-principles density functional theory to simulate the interaction of bundles of semiconducting (10, 0) and metallic (6, 6) carbon nanotubes (CNTs) with small gold clusters (Aun, n = 3, 5) inserted in their interstitial spaces. We find that gold clusters spontaneously evolve to form atomic chains along the axis of nanotubes and induce weak metallicity in the semiconducting nanotubes through charge transfer. We further show that a similar structural evolution of Pt3 clusters occurs in the interstitial spaces of a (10, 0) CNT bundle. Our calculations show that these structural changes, along with interesting changes in the electronic structure, occur at moderate pressures that are readily achievable in a laboratory, and should be relevant to devices that make use of gold-nanotube contacts
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