A First-Principles Study of the Electronic Reconstructions of LaAlO3/SrTiO3 Heterointerfaces and Their Variants

We present a first-principles study of the electronic structures and properties of ideal (atomically sharp) LaAlO3/SrTiO3 (001) heterointerfaces and their variants such as a new class of quantum well systems. We demonstrate the insulating-to-metallic transition as a function of the LaAlO3 film thickness in these systems. After the phase transition, we find that conduction electrons are bound to the n-type interface while holes diffuse away from the p-type interface, and we explain this asymmetry in terms of a large hopping matrix element that is unique to the n-type interface. We build a tight-binding model based on these hopping matrix elements to illustrate how the conduction electron gas is bound to the n-type interface. Based on the `polar catastrophe' mechanism, we propose a new class of quantum wells at which we can manually control the spatial extent of the conduction electron gas. In addition, we develop a continuous model to unify the LaAlO3/SrTiO3 interfaces and quantum wells and predict the thickness dependence of sheet carrier densities of these systems. Finally, we study the external field effect on both LaAlO3/SrTiO3 interfaces and quantum well systems. Our systematic study of the electronic reconstruction of LaAlO3/SrTiO3 interfaces may serve as a guide to engineering transition metal oxide heterointerfaces.Comment: 50 pages, 18 figures and 4 table

Phenomenological theory of phase transitions in highly piezoelectric perovskites

Recently discovered fine structure of the morphotropic phase boundaries in highly piezoelectric mixture compounds PZT, PMN-PT, and PZN-PT demonstrates the importance of highly non-linear interactions in these systems. We show that an adequate Landau-type description of the ferroelectric phase transitions in these compounds is achieved by the use of a twelfth-order expansion of the Landau potential in terms of the phenomenological order parameter. Group-theoretical and catastrophe-theory methods are used in constructing the appropriate Landau potential. A complete phase diagram is calculated in phenomenological parameter space. The theory describes both PZT and PZN-PT types of phase diagrams, including the newly found monoclinic and orthorhombic phases. Anomalously large piezoelectric coefficients are predicted in the vicinity of the phase transition lines.Comment: RevTex4, 8 pages, 2 figures. Dramatically changed after referees' Comments, to appear in Phys. Rev. B, 1 April 200

Tunability of the dielectric response of epitaxially strained SrTiO3 from first principles

The effect of in-plane strain on the nonlinear dielectric properties of SrTiO3 epitaxial thin films is calculated using density-functional theory within the local-density approximation. Motivated by recent experiments, the structure, zone-center phonons, and dielectric properties with and without an external electric field are evaluated for several misfit strains within +-3% of the calculated cubic lattice parameter. In these calculations, the in-plane lattice parameters are fixed, and all remaining structural parameters are permitted to relax. The presence of an external bias is treated approximately by applying a force to each ion proportional to the electric field. After obtaining zero-field ground state structures for various strains, the zone-center phonon frequencies and Born effective charges are computed, yielding the zero-field dielectric response. The dielectric response at finite electric field bias is obtained by computing the field dependence of the structure and polarization using an approximate technique. The results are compared with recent experiments and a previous phenomenological theory. The tunability is found to be strongly dependent on the in-plane lattice parameter, showing markedly different behavior for tensile and compressive strains. Our results are expected to be of use for isolating the role of strain in the tunability of real ultrathin epitaxial films.Comment: 11 pages, with postscript figures embedded. Uses REVTEX and epsf macros. Also available at http://www.physics.rutgers.edu/~dhv/preprints/ant_srti/index.htm

High frequency polarization switching of a thin ferroelectric film

We consider both experimentally and analytically the transient oscillatory process that arises when a rapid change in voltage is applied to a $Ba_xSr_{1-x}TiO_3$ ferroelectric thin film deposited on an $Mg0$ substrate. High frequency ($\approx 10^{8} rad/s$) polarization oscillations are observed in the ferroelectric sample. These can be understood using a simple field-polarization model. In particular we obtain analytic expressions for the oscillation frequency and the decay time of the polarization fluctuation in terms of the material parameters. These estimations agree well with the experimental results

Ab-initio design of perovskite alloys with predetermined properties: The case of Pb(Sc_{0.5} Nb_{0.5})O_{3}

A first-principles derived approach is combined with the inverse Monte Carlo technique to determine the atomic orderings leading to prefixed properties in Pb(Sc_{0.5}Nb_{0.5})O_{3} perovskite alloy. We find that some arrangements between Sc and Nb atoms result in drastic changes with respect to the disordered material, including ground states of new symmetries, large enhancement of electromechanical responses, and considerable shift of the Curie temperature. We discuss the microscopic mechanisms responsible for these unusual effects.Comment: 5 pages with 2 postscript figures embedde

Monte Carlo Study of Relaxor Systems: A Minimum Model for Pb(In1/2_{1/2}Nb1/2_{1/2})O3_3}

We examine a simple model for Pb(In$_{1/2}$Nb$_{1/2}$)O$_3$ (PIN), which includes both long-range dipole-dipole interaction and random local anisotropy. A improved algorithm optimized for long-range interaction has been applied for efficient large-scale Monte Carlo simulation. We demonstrate that the phase diagram of PIN is qualitatively reproduced by this minimum model. Some properties characteristic of relaxors such as nano-scale domain formation, slow dynamics and dispersive dielectric responses are also examined.Comment: 5 pages, 4 figure

Second harmonic generation and X-ray diffraction studies of pretransitional region in relaxor K(1-x) LixTaO3

Optical second-harmonic-generation(SHG) observations and precise X-ray diffraction experiments have been performed on quantum paraelectrics KTaO3 (KTO) and relaxor K(1-x)LixTaO3 with x=3% (KLT-3) and 7% (KLT-7). It is found in KLT-3 and KLT-7 that a pretransitional region exists between two characteristic temperatures Td and Tp (<Td). The average symmetry of the region is tetragonal with a weak lattice-deformation but non-polar in average. The temperature interval between Td and Tp is consistent with the interval on which neutron diffuse scatterings have been previously reported. These facts strongly suggest that polar micro-regions (PMRs) nucleate around Td and grow toward Tp. Below Tp, a larger deformation and a field-induced SH intensity start to develop, while no significant SHG appear in zero-field cooling process. The temperature dependence of the SH intensity below Tp coincides well with that of the tetragonality determined from the lattice deformation. The Landau-Devonshire phenomenological approach suggests that the ferroelectric phase transition at Tp is of first order and that it approaches the second order transition with the decrease of Li concentration. A marked increase of neutron diffraction intensities below Tp indicates that PMRs are transformed to ferroelectric micro-domains at Tp, and the micro-domains change to macroscopic ones under the electric field below Tp.Comment: 31 pages, 10 figure

The polarizability model for ferroelectricity in perovskite oxides

This article reviews the polarizability model and its applications to ferroelectric perovskite oxides. The motivation for the introduction of the model is discussed and nonlinear oxygen ion polarizability effects and their lattice dynamical implementation outlined. While a large part of this work is dedicated to results obtained within the self-consistent-phonon approximation (SPA), also nonlinear solutions of the model are handled which are of interest to the physics of relaxor ferroelectrics, domain wall motions, incommensurate phase transitions. The main emphasis is to compare the results of the model with experimental data and to predict novel phenomena.Comment: 55 pages, 35 figure