149 research outputs found
Ab initio phonon dispersion curves and interatomic force constants of barium titanate
The phonon dispersion curves of cubic BaTiO_3 have been computed within a
first-principles approach and the results compared to the experimental data.
The curves obtained are very similar to those reported for KNbO_3 by Yu and
Krakauer [Phys. Rev. Lett. 74, 4067 (1995)]. They reveal that correlated atomic
displacements along chains are at the origin of the ferroelectric
instability. A simplified model illustrates that spontaneous collective
displacements will occur when a dozen of aligned atoms are coupled. The
longitudinal interatomic force constant between nearest neighbour Ti and O
atoms is relatively weak in comparison to that between Ti atoms in adjacent
cells. The small coupling between Ti and O displacements seems however
necessary to reproduce a ferroelectric instability.Comment: 12 pages, 4 figure
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First-principles reinvestigation of bulk WO
Using first-principles calculations, we analyze the structural properties of tungsten trioxide WO. Our calculations rely on density functional theory and the use of the B1-WC hybrid functional, which provides very good agreement with experimental data. We show that the hypothetical high-symmetry cubic reference structure combines several ferroelectric and antiferrodistortive (antipolar cation motions, rotations, and tilts of oxygen octahedra) structural instabilities. Although the ferroelectric instability is the largest, the instability related to antipolar W motions combines with those associated to oxygen rotations and tilts to produce the biggest energy reduction, yielding a 2/ ground state. This nonpolar 2/ phase is only different from the experimentally reported ground state by the absence of a very tiny additional ferroelectric distortion. The calculations performed on a stoichiometric compound so suggest that the low-temperature phase of WO is not intrinsically ferroelectric and that the experimentally observed ferroelectric character might arise from extrinsic defects such as oxygen vacancies. Independently, we also identify never observed and ferroelectric metastable phases with large polarizations and low energies close to the 2/ ground state, which makes WO potential antiferroelectric material. The relative stability of various phases is discussed in terms of the anharmonic couplings between different structural distortions, highlighting a very complex interplay.The work was supported by the ARC project AIMED and the F.R.S-FNRS PDR projects HiT4FiT and MaRePeThe. Calculations have been performed within the PRACE project TheDeNoMo and relied on the Céci facilities funded by F.R.S-FNRS (Grant No. 2.5020.1) and Tier-1 supercomputer of the Fédération Wallonie-Bruxelles funded by the Walloon Region (Grant No. 1117545). E.K.H.S. is grateful for support to EPSRC and the Leverhulme trust. H.H. thanks the AVERROES-ERASMUS Mundus project
Band alignment at metal/ferroelectric interfaces: insights and artifacts from first principles
Based on recent advances in first-principles theory, we develop a general
model of the band offset at metal/ferroelectric interfaces. We show that,
depending on the polarization of the film, a pathological regime might occur
where the metallic carriers populate the energy bands of the insulator, making
it metallic. As the most common approximations of density functional theory are
affected by a systematic underestimation of the fundamental band gap of
insulators, this scenario is likely to be an artifact of the simulation. We
provide a number of rigorous criteria, together with extensive practical
examples, to systematically identify this problematic situation in the
calculated electronic and structural properties of ferroelectric systems. We
discuss our findings in the context of earlier literature studies, where the
issues described in this work have often been overlooked. We also discuss
formal analogies to the physics of polarity compensation at LaAlO3/SrTiO3
interfaces, and suggest promising avenues for future research.Comment: 29 pages, 23 figure
Electroresistance effects in ferroelectric tunnel barriers
Electron transport through fully depleted ferroelectric tunnel barriers
sandwiched between two metal electrodes and its dependence on ferroelectric
polarization direction are investigated. The model assumes a polarization
direction dependent ferroelectric barrier. The transport mechanisms, including
direct tunneling, Fowler-Nordheim tunneling and thermionic injection, are
considered in the calculation of the electroresistance as a function of
ferroelectric barrier properties, given by the properties of the ferroelectric,
the barrier thickness, and the metal properties, and in turn of the
polarization direction. Large electroresistance is favored in thicker films for
all three transport mechanisms but on the expense of current density. However,
switching between two transport mechanisms, i.e., direct tunneling and
Fowler-Nordheim tunneling, by polarization switching yields a large
electroresistance. Furthermore, the most versatile playground in optimizing the
device performance was found to be the electrode properties, especially
screening length and band offset with the ferroelectric.Comment: 24pages, 7 figures, revised, one figure adde
Born Effective Charges of Barium Titanate: band by band decomposition and sensitivity to structural features
The Born effective charge tensors of Barium Titanate have been calculated for
each of its 4 phases. Large effective charges of Ti and O, also predicted by
shell model calculations and made plausible by a simplified model, reflect the
partial covalent character of the chemical bond. A band by band decomposition
confirms that orbital hybridization is not restricted to Ti and O atoms but
also involves Ba which appears more covalent than generally assumed. Our
calculations reveal a strong dependence of the effective charges on the atomic
positions contrasting with a relative insensitivity on isotropic volume
changes.Comment: 13 page
Efficient total energy calculations from self-energy models
We propose a new method for calculating total energies of systems of interacting electrons, which requires little more computational resources than standard density-functional theories. The total energy is calculated within the framework of many-body perturbation theory by using an efficient model of the self-energy, that nevertheless retains the main features of the exact operator. The method shows promising performance when tested against quantum Monte Carlo results for the linear response of the homogeneous electron gas and structural properties of bulk silicon
First-principles approach to lattice-mediated magnetoelectric effects
We present a first-principles scheme for the computation of the
magnetoelectric response of magnetic insulators. The method focuses on the
lattice-mediated part of the magnetic response to an electric field, which we
argue can be expected to be the dominant contribution in materials displaying a
strong magnetoelectric coupling. We apply our method to Cr2O3, a relatively
simple and experimentally well studied magnetoelectric compound.Comment: 4 pages with 1 figure embedded. More information at
http://www.icmab.es/dmmis/leem/jorg
The physics of dynamical atomic charges: the case of ABO3 compounds
Based on recent first-principles computations in perovskite compounds,
especially BaTiO3, we examine the significance of the Born effective charge
concept and contrast it with other atomic charge definitions, either static
(Mulliken, Bader...) or dynamical (Callen, Szigeti...). It is shown that static
and dynamical charges are not driven by the same underlying parameters. A
unified treatment of dynamical charges in periodic solids and large clusters is
proposed. The origin of the difference between static and dynamical charges is
discussed in terms of local polarizability and delocalized transfers of charge:
local models succeed in reproducing anomalous effective charges thanks to large
atomic polarizabilities but, in ABO3 compounds, ab initio calculations favor
the physical picture based upon transfer of charges. Various results concerning
barium and strontium titanates are presented. The origin of anomalous Born
effective charges is discussed thanks to a band-by-band decomposition which
allows to identify the displacement of the Wannier center of separated bands
induced by an atomic displacement. The sensitivity of the Born effective
charges to microscopic and macroscopic strains is examined. Finally, we
estimate the spontaneous polarization in the four phases of barium titanate.Comment: 25 pages, 6 Figures, 10 Tables, LaTe
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