arXiv subjects

L. Bellaiche

Publications and source records attributed to L. Bellaiche.

At least 55 records · Page 3Linked to original sources

arXiv2015

Predicting a Ferrimagnetic Phase of Zn2FeOsO6 with Strong Magnetoelectric Coupling

Multiferroic materials, in which ferroelectric and magnetic ordering coexist, are of fundamental interest for the development of novel memory devices that allow for electrical writing and non-destructive magnetic readout operation. The great challenge is to create room temperature multiferroic materials with strongly coupled ferroelectric and ferromagnetic (or ferrimagnetic) orderings. BiFeO3 has been the most heavily investigated single-phase multiferroic to date due to the coexistence of its magnetic order and ferroelectric order at room temperature. However, there is no net magnetic moment in the cycloidal (antiferromagnetic-like) magnetic state of bulk BiFeO3, which severely limits its realistic applications in electric field controlled spintronic devices. Here, we predict that double perovskite Zn2FeOsO6 is a new multiferroic with properties superior to BiFeO3. First, there are strong ferroelectricity and strong ferrimagnetism at room temperature in Zn2FeOsO6. Second, the easy-plane of the spontaneous magnetization can be switched by an external electric field, evidencing the strong magnetoelectric coupling existing in this system. Our results suggest that ferrimagnetic 3d-5d double perovskite may therefore be used to achieve voltage control of magnetism in future spintronic devices.

cond-mat.mtrl-sci↗

arXiv2015

Giant Surface Charge Density of Graphene Resolved From Scanning Tunneling Microscopy and First-Principles Theory

In this work, systematic constant-bias, variable-current scanning tunneling microscopy (STM) measurements and STM simulations from density-functional theory are made, yielding critical insights into the spatial structure of electrons in graphene. A foundational comparison is drawn between graphene and graphite, showing the surface charge density of graphene to be 300 percent that of graphite. Furthermore, simulated STM images reveal that high-current STM better resolves graphenes honeycomb bonding structure because of a retraction which occurs in the topmost dangling bond orbitals.

cond-mat.mes-hall↗

arXiv2015

Atomic Control of Strain in Freestanding Graphene

In this study, we describe a new experimental approach based on constant-current scanning tunneling spectroscopy to controllably and reversibly pull freestanding graphene membranes up to 35 nm from their equilibrium height. In addition, we present scanning tunneling microscopy (STM) images of freestanding graphene membranes with atomic resolution. Atomic-scale corrugation amplitudes 20 times larger than the STM electronic corrugation for graphene on a substrate were observed. The freestanding graphene membrane responds to a local attractive force created at the STM tip as a highly-conductive yet flexible grounding plane with an elastic restoring force. We indicate possible applications of our method in the controlled creation of pseudo-magnetic fields by strain on single-layer graphene.

cond-mat.mes-hall↗

arXiv2015

A Pathway between Bernal and Rhombohedral Stacked Graphene Layers with Scanning Tunneling Microscopy

Horizontal shifts in the top layer of highly oriented pyrolytic graphite, induced by a scanning tunneling microscope (STM) tip, are presented. Excellent agreement is found between STM images and those simulated using density functional theory. First-principle calculations identify that the low-energy barrier direction of the top layer displacement is toward a structure where none of the carbon pz orbitals overlap, while the high-energy barrier direction is toward AA stacking. Each directional shift yields a real-space surface charge density similar to graphene; however the low-energy barrier direction requires only one bond length to convert ABA (Bernal) to ABC (rhombohedral).

cond-mat.mes-hall↗

arXiv2015

Electronic transition from graphite to graphene via controlled movement of the top layer with scanning tunneling microscopy

A series of measurements using a technique called electrostatic-manipulation scanning tunneling microscopy (EM-STM) were performed on a highly-oriented pyrolytic graphite surface. The electrostatic interaction between the STM tip and the sample can be tuned to produce both reversible and irreversible large-scale movement of the graphite surface. Under this influence, atomic-resolution STM images reveal that a continuous electronic transition from triangular symmetry, where only alternate atoms are imaged, to hexagonal symmetry can be systematically controlled. Density functional theory (DFT) calculations reveal that this transition can be related to vertical displacements of the top layer of graphite relative to the bulk. Evidence for horizontal shifts in the top layer of graphite is also presented. Excellent agreement is found between experimental STM images and those simulated using DFT.

cond-mat.mes-hall↗

arXiv2015

New Scanning Tunneling Microscopy Technique Enables Systematic Study of the Unique Electronic Transition from Graphite to Graphene

A series of measurements using a novel technique called electrostatic-manipulation scanning tunneling microscopy were performed on a highly-oriented pyrolytic graphite (HOPG) surface. The electrostatic interaction between the STM tip and the sample can be tuned to produce both reversible and irreversible large-scale vertical movement of the HOPG surface. Under this influence, atomic-resolution STM images reveal that a continuous electronic reconstruction transition from a triangular symmetry, where only alternate atoms are imaged, to a honeycomb structure can be systematically controlled. First-principles calculations reveal that this transition can be related to vertical displacements of the top layer of graphite relative to the bulk. Detailed analysis of the band structure predicts that a transition from parabolic to linear bands occurs after a 0.09 nm displacement of the top layer.

cond-mat.mes-hall↗

arXiv2015

Quantum Anomalous Hall Effect in Graphene Proximity Coupled to an Antiferromagnetic Insulator

We propose realizing the quantum anomalous Hall effect by proximity coupling graphene to an antiferromagnetic insulator that provides both broken time-reversal symmetry and spin-orbit coupling. We illustrate our idea by performing ab initio calculations for graphene adsorbed on the (111) surface of BiFeO3. In this case, we find that the proximity-induced exchange field in graphene is about 70 meV, and that a topologically nontrivial band gap is opened by Rashba spin-orbit coupling. The size of the gap depends on the separation between the graphene and the thin film substrate, which can be tuned experimentally by applying external pressure.

cond-mat.mes-hall↗

arXiv2014

Prediction of a Stable Post-Post-Perovskite Structure from First Principles

A novel stable crystallographic structure is discovered in a variety of ABO3, ABF3 and A2O3 compounds (including materials of geological relevance, prototypes of multiferroics, exhibiting strong spin-orbit effects, etc...), via the use of first principles. This novel structure appears under hydrostatic pressure, and is the first "post-post-perovskite" phase to be found. It provides a successful solution to experimental puzzles in important systems, and is characterized by one-dimensional chains linked by group of two via edge-sharing oxygen/fluorine octahedra. Such unprecedented organization automatically results in anisotropic elastic properties and new magnetic arrangements. Depending on the system of choice, this post-post-perovskite structure also possesses electronic band gaps ranging from zero to ~ 10 eV being direct or indirect in nature, which emphasizes its "universality" and its potential to have striking, e.g., electrical or transport phenomena.

cond-mat.mtrl-sci↗

arXiv2014

First-principles study of the multi-mode anti-ferroelectric transition of PbZrO3

We have studied ab initio the phase transition in PbZrO3, a perovskite oxide usually presented as the prototypic anti-ferroelectric material. Our work reveals the crucial role that anti-ferrodistortive modes -- involving concerted rotations of the oxygen octahedra in the structure -- play in the transformation, as they select the observed anti-ferroelectric phase, among competing structural variants, via a cooperative trilinear coupling.

cond-mat.mtrl-sci↗

arXiv2013

Terahertz dielectric response and coupled dynamics of ferroelectrics and multiferroics from effective Hamiltonian simulations

Ferroelectric and multiferroic materials form an important class of functional materials. Over the last twenty years, first-principles-based effective Hamiltonian approaches have been successfully developed to simulate these materials. In recent years, effective Hamiltonian approaches were further combined with molecular dynamics methods to investigate terahertz dynamical properties of various perovskites. With this combination, a variety of ferroelectric and multiferroic materials, including BaTiO_{3}, Ba(Sr,Ti)O_{3}, Pb(Zr,Ti)O_{3}, BiFeO_{3}, and SrTiO_{3} bulks and films have been simulated, which led to the understanding of complex phenomena and discovery of novel effects. In this review, we first provide technical details about effective Hamiltonians and molecular dynamics simulation. Then, we present applications of the combination of these two techniques to different perovskites. Finally, we also briefly discuss possible future directions of this approach.

cond-mat.mtrl-sci↗

arXiv2013

Natural optical activity and its control by electric field in electrotoroidic systems

We propose the existence, via analytical derivations, novel phenomenologies, and first-principles-based simulations, of a new class of materials that are not only spontaneously optically active, but also for which the sense of rotation can be switched by an electric field applied to them-- via an induced transition between the dextrorotatory and laevorotatory forms. Such systems possess electric vortices that are coupled to a spontaneous electrical polarization. Furthermore, our atomistic simulations provide a deep microscopic insight into, and understanding of, this class of naturally optically active materials.

cond-mat.mtrl-sci↗

arXiv2013

Thickness-dependent polarization of strained BiFeO3 films with constant tetragonality

We measure the remnant polarization of ferroelectric domains in BiFeO3 films down to 3.6 nm using low energy electron and photoelectron emission microscopy. The measured polarization decays strongly below a critical thickness of 5-7 nm predicted by continuous medium theory whereas the tetragonal distortion does not change. We resolve this apparent contradiction using first-principles-based effective Hamiltonian calculations. In ultra thin films the energetics of near open circuit electrical boundary conditions, i.e. unscreened depolarizing field, drive the system through a phase transition from single out-of-plane polarization to a nanoscale stripe domains, giving rise to an average remnant polarization close to zero as measured by the electron microscopy whilst maintaining the relatively large tetragonal distortion imposed by the non-zero polarization state of each individual domain.

cond-mat.mtrl-sci↗

arXiv2012

Emergence of central mode in the paraelectric phase of ferroelectric perovskites

THz-range dielectric spectroscopy and first-principle-based effective-Hamiltonian molecular dynamics simulations were employed to elucidate the dielectric response in the paraelectric phase of (Ba,Sr)TiO3 solid solutions. Analysis of the resulting dielectric spectra suggests the existence of a crossover between two different regimes: a higher-temperature regime governed by the soft mode only versus a lower-temperature regime exhibiting a coupled soft mode/central mode dynamics. Interestingly, a single phenomenological coupling model can be used to adjust the THz dielectric response in the entire range of the paraelectric phase (i.e., even at high temperature). We conclude that the central peak is associated with thermally activated processes, and that it cannot be discerned anymore in the dielectric spectra when the rate of these thermally activated processes exceeds certain characteristic frequency of the system.

cond-mat.mtrl-sci↗

arXiv2012

Study of strain effect on in-plane polarization in epitaxial BiFeO3 thin films using planar electrodes

Epitaxial strain plays an important role in determining physical properties of perovskite ferroelectric oxide thin films. However, it is very challenging to directly measure properties such as polarization in ultrathin strained films using traditional sandwich capacitor devices, because of high leakage current. We employed a planar electrode device with different crystallographical orientations between electrodes along different electric field orientation to directly measure the in-plane polarization-electric field (P-E) hysteresis loops in fully strained thin films. At high misfit strains such as -4.4%, the pure Tetrogonal-like phase is obtained and its polarization vector is constrained to lie in the (010) plane with a significantly large in-plane component, ~44 μC/cm2. First-principle calculations are carried out in parallel, and provide a good agreement with the experimental results. Our results pave the way to design in-plane devices based on T-like BFO and the strategy proposed here can be expanded to study all other similar strained multiferroic ultrathin films.

cond-mat.mtrl-sci↗

arXiv2012

Finite-Temperature Properties of Ba(Zr,Ti)O$_3$ Relaxors From First Principles

A first-principles-based technique is developed to investigate properties of Ba(Zr,Ti)O$_3$ relaxor ferroelectrics as a function of temperature. The use of this scheme provides answers to important, unresolved and/or controversial questions, such as: what do the different critical temperatures usually found in relaxors correspond to? Do polar nanoregions really exist in relaxors? If yes, do they only form inside chemically-ordered regions? Is it necessary that antiferroelectricity develops in order for the relaxor behavior to occur? Are random fields and random strains really the mechanisms responsible for relaxor behavior? If not, what are these mechanisms? These {\it ab-initio-based} calculations also leads to a deep microscopic insight into relaxors.

cond-mat.mtrl-sci↗

arXiv2012

Giant direct magnetoelectric effect in strained multiferroic heterostructures

The direct magnetoelectric (ME) effect mediated by lattice strains induced in a ferroelectric film by a ferromagnetic substrate is evaluated using first-principles-based calculations. To that end, the strain sensitivity of ferroelectric polarization and the film permittivity are calculated as a function of the in-plane biaxial strain for Pb(Zr0.52Ti0.48)O3 films under various depolarizing fields. It is found that the ME voltage coefficient varies nonmonotonically with this strain and may reach giant values exceeding 100 Vcm-1 Oe-1 over a strain range that can be controlled through the electrical boundary conditions.

cond-mat.mtrl-sci↗

arXiv2011

Geometric frustration in compositionally modulated ferroelectrics

Geometric frustration is a broad phenomenon that results from an intrinsic incompatibility between some fundamental interactions and the underlying lattice geometry1-7. Geometric frustration gives rise to new fundamental phenomena and is known to yield intriguing effects, such as the formation of exotic states like spin ice, spin liquids and spin glasses1-7. It has also led to interesting findings of fractional charge quantization and magnetic monopoles5,6. Geometric frustration related mechanisms have been proposed to understand the origins of relaxor behavior in some multiferroics, colossal magnetocapacitive coupling and unusual and novel mechanisms of high Tc superconductivity1-5. Although geometric frustration has been particularly well studied in magnetic systems in the last 20 years or so, its manifestation in the important class formed by ferroelectric materials (that are compounds exhibiting electric rather than magnetic dipoles) is basically unknown. Here, we show, via the use of a first-principles-based technique, that compositionally graded ferroelectrics possess the characteristic "fingerprints" associated with geometric frustration. These systems have a highly degenerate energy surface and exhibit original critical phenomena. They further reveal exotic orderings with novel stripe phases involving complex spatial organization. These stripes display spiral states, topological defects and curvature. Compositionally graded ferroelectrics can thus be considered as the "missing" link that brings ferroelectrics into the broad category of materials able to exhibit geometric frustration. Our ab-initio calculations allow a deep microscopic insight into this novel geometrically frustrated system.

cond-mat.mtrl-sci↗

arXiv2011

Prediction of the Magnetotoroidic Effect from Atomistic Simulations

An effective Hamiltonian technique is used to investigate the effect of applying curled electric fields on physical properties of stress-free BiFeO3 dots being under open-circuit electrical boundary conditions. It is discovered that such fields can lead to a control of not only the magnitude but also the direction of the magnetization. On a microscopic point of view, such control originates from the field-induced transformation or switching of electrical vortices and their couplings with oxygen octahedral tilts and magnetic dipoles. This control involves striking intermediate states, and constitutes a novel phenomenon that can be termed as "magnetotoroidic" effect.

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