arXiv subjects

Jorge Iniguez

Publications and source records attributed to Jorge Iniguez.

At least 19 recordsLinked to original sources

arXiv2023

Manipulating chiral-spin transport with ferroelectric polarization

A collective excitation of the spin structure in a magnetic insulator can transmit spin-angular momentum with negligible dissipation. This quantum of a spin wave, introduced more than nine decades ago, has always been manipulated through magnetic dipoles, (i.e., timereversal symmetry). Here, we report the experimental observation of chiral-spin transport in multiferroic BiFeO3, where the spin transport is controlled by reversing the ferroelectric polarization (i.e., spatial inversion symmetry). The ferroelectrically controlled magnons produce an unprecedented ratio of up to 18% rectification at room temperature. The spin torque that the magnons in BiFeO3 carry can be used to efficiently switch the magnetization of adja-cent magnets, with a spin-torque efficiency being comparable to the spin Hall effect in heavy metals. Utilizing such a controllable magnon generation and transmission in BiFeO3, an alloxide, energy-scalable logic is demonstrated composed of spin-orbit injection, detection, and magnetoelectric control. This observation opens a new chapter of multiferroic magnons and paves an alternative pathway towards low-dissipation nanoelectronics.

physics.app-ph↗

arXiv2023

A 2D ferroelectric vortex lattice in twisted BaTiO3 freestanding layers

The wealth of complex polar topologies recently found in nanoscale ferroelectrics result from a delicate balance between the materials intrinsic tendency to develop a homogeneous polarization and the electric and mechanic boundary conditions imposed upon them. Ferroelectric dielectric interfaces are model systems where polarization curling originates from open circuit like electric boundary conditions, to avoid the build-up of polarization charges through the formation of flux closure domains that evolve into vortex like structures at the nanoscale. Interestingly, while ferroelectricity is known to couple strongly to strain (both homogeneous and inhomogeneous), the effect of mechanical constraints on thin film nanoscale ferroelectrics has been comparatively less explored because of the relative paucity of strain patterns that can be implemented experimentally. Here we show that the stacking of freestanding ferroelectric perovskite layers with controlled twist angles opens an unprecedented opportunity to tailor these topological nanostructures in a way determined by the lateral strain modulation associated to the twisting. Interestingly, we find that a peculiar pattern of polarization vortices and antivortices emerges from the flexoelectric coupling of polarization to strain gradients. This finding opens exciting opportunities to create two-dimensional high density vortex crystals that would allow us to explore novel physical effects and functionalities.

cond-mat.mes-hall↗

arXiv2020

A three-order-parameter bistable magnetoelectric multiferroic metal

Using first-principles calculations we predict that the layered-perovskite metal Bi$_5$Mn$_5$O$_{17}$ is a ferromagnet, ferroelectric, and ferrotoroid which may realize the long sought-after goal of a room-temperature ferromagnetic single-phase multiferroic with large, strongly coupled, primary-order polarization and magnetization. Bi$_5$Mn$_5$O$_{17}$ has two nearly energy-degenerate ground states with mutually orthogonal vector order parameters (polarization, magnetization, ferrotoroidicity), which can be rotated globally by switching between ground states. Giant cross-coupling magnetoelectric and magnetotoroidic effects, as well as optical non-reciprocity, are thus expected. Importantly, Bi$_5$Mn$_5$O$_{17}$ should be thermodynamically stable in O-rich growth conditions, and hence experimentally accessible.

cond-mat.mtrl-sci↗

arXiv2018

Giant Direct and Inverse Electrocaloric Effects in Multiferroic Thin Films

Refrigeration systems based on compression of greenhouse gases are environmentally threatening and cannot be scaled down to on-chip dimensions. In the vicinity of a phase transition caloric materials present large thermal responses to external fields, which makes them promising for developing alternative solid-state cooling devices. Electrocaloric effects are particularly well-suited for portable refrigeration applications; however, most electrocaloric materials operate best at non-ambient temperatures or require the application of large electric fields. Here, we predict that modest electric fields can yield giant room-temperature electrocaloric effects in multiferroic BiCoO$_{3}$ (BCO) thin films. Depending on the orientation of the applied field the resulting electrocaloric effect is either direct (heating) or inverse (cooling), which may enable the design of enhanced refrigeration cycles. We show that spin-phonon couplings and phase competition are the underlying causes of the disclosed caloric phenomena. The dual electrocaloric response of BCO thin films can be effectively tuned by means of epitaxial strain and we anticipate that other control strategies like chemical substitution are also possible.

cond-mat.mtrl-sci↗

arXiv2018

Meta-screening and permanence of polar distortion in metallized ferroelectrics

Ferroelectric materials are characterized by a spontaneous polar distortion. The behavior of such distortions in the presence of free charge is the key to the physics of metallized ferroelectrics in particular, and of structurally-polar metals more generally. Using first-principles simulations, here we show that a polar distortion resists metallization and the attendant suppression of long-range dipolar interactions in the vast majority of a sample of 11 representative ferroelectrics. We identify a meta-screening effect, occurring in the doped compounds as a consequence of the charge rearrangements associated to electrostatic screening, as the main factor determining the survival of a non-centrosymmetric phase. Our findings advance greatly our understanding of the essentials of structurally-polar metals, and offer guidelines on the behavior of ferroelectrics upon field-effect charge injection or proximity to conductive device elements.

cond-mat.mtrl-sci↗

arXiv2018

Energetics of oxygen-octahedra rotations in perovskite oxides from first principles

We use first-principles methods to study oxygen-octahedra rotations in ABO3 perovskite oxides. We focus on the short-period, perfectly antiphase or in-phase, tilt patterns that characterize most compounds and control their physical (e.g., conductive, magnetic) properties. Based on an analytical form of the relevant potential energy surface, we discuss the conditions for the stability of polymorphs presenting different tilt patterns, and obtain numerical results for a collection of thirty-five representative materials. Our results reveal the mechanisms responsible for the frequent occurrence of a particular structure that combines antiphase and in-phase rotations, i.e., the orthorhombic Pbnm phase displayed by about half of all perovskite oxides and by many non-oxidic perovskites. The Pbnm phase benefits from the simultaneous occurrence of antiphase and in-phase tilt patterns that compete with each other, but not as strongly as to be mutually exclusive. We also find that secondary antipolar modes, involving the A cations, contribute to weaken the competition between different tilts and play a key role in their coexistence. Our results thus confirm and better explain previous observations for particular compounds. Interestingly, we also find that strain effects, which are known to be a major factor governing phase competition in related (e.g., ferroelectric) perovskite oxides, play no essential role as regards the relative stability of different rotational polymorphs. Further, we discuss why the Pbnm structure stops being the ground state in two opposite limits, for large and small A cations, showing that very different effects become relevant in each case. Our work thus provides a comprehensive discussion on these all-important and abundant materials, which will be useful to better understand existing compounds as well as to identify new strategies for materials engineering.

cond-mat.mtrl-sci↗

arXiv2017

Structurally Triggered Metal-Insulator Transition in Rare-Earth Nickelates

Rare-earth nickelates form an intriguing series of correlated perovskite oxides. Apart from LaNiO3, they exhibit on cooling a sharp metal-insulator electronic phase transition, a concurrent structural phase transition and a magnetic phase transition toward an unusual antiferromagnetic spin order. Appealing for various applications, full exploitation of these compounds is still hampered by the lack of global understanding of the interplay between their electronic, structural and magnetic properties. Here, we show from first-principles calculations that the metal-insulator transition of nickelates arises from the softening of an oxygen breathing distortion, structurally triggered by oxygen-octahedra rotation motions. The origin of such a rare triggered mechanism is traced back in their electronic and magnetic properties, providing a united picture. We further develop a Landau model accounting for the evolution of the metal-insulator transition in terms of the $R cations and rationalising how to tune this transition by acting on oxygen rotation motions.

cond-mat.mtrl-sci↗

arXiv2017

Novel magnetoelectric effects via penta-linear interactions

Magnetoelectric multiferroic materials, particularly with the perovskite structure, are receiving a lot of attention because of their inherent coupling between electrical polarization and magnetic ordering. However, very few types of direct coupling between polarization and magnetization are known, and it is unclear whether they can be useful to the design of novel spintronic devices exploiting the control of magnetization by electric fields. For instance, the typical bi-quadratic coupling only allows to change the magnitude of the magnetization by an electric field, but it does not permit an electric-field-induced switching of the magnetization. Similarly, the so-called Lifshitz invariants allow an electric-field control of complicated magnetic orderings, but not of the magnetization. Here, we report the discovery of novel direct couplings between polarization and magnetization in epitaxial perovskite films, via the use of first-principles methods and the development of an original Landau-type phenomenological theory. Our results feature penta-linear interactions involving the ferromagnetic and anti-ferromagnetic vectors as well as the polar distortions and oxygen octahedral tilting, and permit a number of striking effects. Examples include a continuous electric-field control of the magnetization magnitude and sign, and the discrete switching of the magnetization magnitude. Thus, the high-order, penta-linear couplings demonstrated in this work may open new paths towards novel magneto-electric effects, as well as, spintronic and magnonic devices.

physics.app-ph↗

arXiv2016

Multiple structural transitions driven by spin-phonon couplings in a perovskite oxide

Spin-phonon interactions are central to many interesting phenomena, ranging from superconductivity to magnetoelectric effects. Yet, they are believed to have a negligible influence on the structural behavior of most materials. For example, magnetic perovskite oxides often undergo structural transitions accompanied by magnetic signatures whose minuteness suggests that the underlying spin-phonon couplings are largely irrelevant. Here we present an exception to this rule, showing that novel effects can occur as a consequence. Our first-principles calculations reveal that spin-phonon interactions are essential to reproduce the experimental observations on the phase diagram of magnetoelectric multiferroic BiCoO$_{3}$. Moreover, we predict that, under compression, these couplings lead to an unprecedented temperature-driven double-reentrant sequence of ferroelectric transitions. We propose how to modify BiCoO$_{3}$ via chemical doping to reproduce such striking effects at ambient conditions, thereby yielding useful multifunctionality.

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↗

arXiv2014

Ferroelectricity at ferroelectric domain walls

We present a first-principles study of model domain walls (DWs) in prototypic ferroelectric PbTiO3. At high temperature the DW structure is somewhat trivial, with atoms occupying high- symmetry positions. However, upon cooling the DW undergoes a symmetry-breaking transition characterized by a giant dielectric anomaly and the onset of a large and switchable polarization. Our results thus corroborate previous arguments for the occurrence of ferroic orders at structural DWs, providing a detailed atomistic picture of a temperature-driven DW-confined transformation. Beyond its relevance to the field of ferroelectrics, our results highlight the interest of these DWs in the broader areas of low-dimensional physics and phase transitions in strongly-fluctuating systems.

cond-mat.mtrl-sci↗

arXiv2014

Ultrafast switching of the electric polarization and magnetic chirality in BiFeO3 by an electric field

Using a first-principles-based effective Hamiltonians within molecular dynamics simulations, we discover that applying an electric field that is opposite to the initial direction of the polarization results in a switching of both the polarization and the magnetic chirality vector of multiferroic BiFeO3 at an ultrafast pace (namely of the order of picoseconds). We discuss the origin of such a double ultrafast switching, which is found to involve original intermediate magnetic states and may hold promise for designing various devices.

cond-mat.mtrl-sci↗

arXiv2013

Electric control of the magnetization in BiFeO$_3$/LaFeO$_3$ superlattices

First-principles techniques are used to investigate the behavior of BiFeO$_{3}$/LaFeO$_{3}$ perovskite oxide superlattices epitaxially grown on a (001)-SrTiO$_3$ substrate. The calculations show that 1/1 superlattices exhibit a $Pmc2_1$ ground state combining a trilinear coupling of one polar and two oxygen rotational lattice modes, and weak ferromagnetism. The microscopic mechanism allowing one to manipulate the magnetization with an electric field in such systems is presented and its dependence on strain and chemical substitution is discussed. BiFeO$_{3}$/LaFeO$_{3}$ artificial superlattices appear to be good candidates to achieve electric switching of magnetization at room temperature.

cond-mat.mtrl-sci↗

arXiv2011

Ab initio study of proper topological ferroelectricity in layered perovskite La2Ti2O7

We present a first-principles investigation of ferroelectricity in layered perovskite oxide La2Ti2O7 (LTO), one of the compounds with highest Curie temperature known (1770 K). Our calculations reveal that LTO's ferroelectric transition results from the condensation of two soft modes that have the same symmetry and are strongly coupled anharmonically. Further, the leading instability mode essentially consists of rotations of the oxygen octahedra that are the basic building block of the perovskite structure; remarkably, because of the particular topology of the lattice, such O6 rotations give raise to a spontaneous polarization in LTO. The effects discussed thus constitute an example of how nano-structuring -- provided here by the natural layering of LTO -- makes it possible to obtain a significant polar character in structural distortions that are typically non-polar. We discuss the implications of our findings as regards the design of novel multifunctional materials. Indeed, the observed proper ferroelectricity driven by O6 rotations provides the ideal conditions to obtain strong magnetoelectric effects.

cond-mat.mtrl-sci↗

arXiv2009

Tuning the atomic and domain structure of epitaxial films of multiferroic BiFeO3

Recent works have shown that the domain walls of room-temperature multiferroic BiFeO3 (BFO) thin films can display distinct and promising functionalities. It is thus important to understand the mechanisms underlying domain formation in these films. High-resolution x-ray diffraction and piezo-force microscopy, combined with first-principles simulations, have allowed us to characterize both the atomic and domain structure of BFO films grown under compressive strain on (001)-SrTiO3, as a function of thickness. We derive a twining model that describes the experimental observations and explains why the 71o domain walls are the ones commonly observed in these films. This understanding provides us with a new degree of freedom to control the structure and, thus, the properties of BiFeO3 thin films.

cond-mat.mtrl-sci↗

arXiv2009

Magnetoelectric response of multiferroic BiFeO3 and related materials

We present a first-principles scheme for computing the magnetoelectric response of multiferroics. We apply our method to BiFeO3 (BFO) and related compounds in which Fe is substituted by other magnetic species. We show that under certain relevant conditions -- i.e., in absence of incommensurate spin modulation, as in BFO thin films and some BFO-based solid solutions -- these materials display a large linear magnetoelectric response. Our calculations reveal the atomistic origin of the coupling and allow us to identify the most promising strategies to enhance it.

cond-mat.mtrl-sci↗

arXiv2008

Pressure-induced structural, electronic, and magnetic effects in BiFeO3

We present a first-principles study of multiferroic BiFeO3 at high pressures. Our work reveals the main structural (change in Bi's coordination and loss of ferroelectricity), electronic (spin crossover and metallization), and magnetic (loss of order) effects favored by compression and how they are connected. Our results are consistent with the striking manifold transition observed experimentally by Gavriliuk et al. [Phys. Rev. B 77, 155112 (2008)] and provide an explanation for it.

cond-mat.mtrl-sci↗

arXiv2008

Theoretical investigation of hydrogen storage in metal-intercalated graphitic materials

We have used first-principles methods to investigate how metal atoms dispersed in the interlayer space of graphitic materials affect their hydrogen-binding properties. We have considered ideal stage-one metal-intercalated graphites of various compositions as representative model systems. Our calculations suggest that alkaline earth metals can significantly enhance the hydrogen storage properties: for example, Be and Mg atoms would act as binding sites of three or four hydrogen molecules, with binding energies per H$_2$ in the 0.2--0.7 eV range, as required for applications. We also find that alkali and transition metals are not as effective in enhancing the storage capacity.

cond-mat.mtrl-sci↗