arXiv subjects

Laurent Bellaiche

Publications and source records attributed to Laurent Bellaiche.

71 records · Page 4Linked to original sources

arXiv2022

Zeeman effect in centrosymmetric antiferromagnets controlled by an electric field

Centrosymmetric antiferromagnetic semiconductors, although abundant in nature, seem less promising than ferromagnets and ferroelectrics for practical applications in semiconductor spintronics. As a matter of fact, the lack of spontaneous polarization and magnetization hinders the efficient utilization of electronic spin in these materials. Here, we propose a paradigm to harness electronic spin in centrosymmetric antiferromagnets via Zeeman spin splittings of electronic energy levels -- termed as spin Zeeman effect -- which is controlled by electric field.By symmetry analysis, we identify twenty-one centrosymmetric antiferromagnetic point groups that accommodate such a spin Zeeman effect. We further predict by first-principles that two antiferromagnetic semiconductors, Fe$_2$TeO$_6$ and SrFe$_2$S$_2$O, are excellent candidates showcasing Zeeman splittings as large as $\sim$55 and $\sim$30 meV, respectively, induced by an electric field of 6 MV/cm. Moreover, the electronic spin magnetization associated to the splitting energy levels can be switched by reversing the electric field. Our work thus sheds light on the electric-field control of electronic spin in antiferromagnets, which broadens the scope of application of centrosymmetric antiferromagnetic semiconductors.

cond-mat.mtrl-sci↗

arXiv2022

Spin-current driven Dzyaloshinskii-Moriya interaction in the multiferroic BiFeO3 from first-principles

The electrical control of magnons opens up new ways to transport and process information for logic devices. In magnetoelectrical multiferroics, the Dzyaloshinskii-Moriya (DM) interaction directly allow for such a control and, hence, is of major importance. We determine the origin and the strength of the (converse) spin current DM interaction in the R3c bulk phase of the multiferroic BiFeO3 based on density functional theory. Our data supports only the existence of one DM interaction contribution originating from the spin current model. By exploring then magnon dispersion in the full Brillouin Zone, we show that the exchange is isotropic, but the DM interaction and anisotropy prefer any propagation and any magnetization direction within the full (111) plane. Our work emphasizes the significance of the asymmetric potential induced by the spin current over the structural asymmetry induced by the anionic octahedron in multiferroics such as BiFeO3.

cond-mat.mtrl-sci↗

arXiv2022

Two-Dimensional Organic-Inorganic Room-Temperature Multiferroic

Organic-inorganic multiferroics are promising for the next generation of electronic devices. To date, dozens of organic-inorganic multiferroics have been reported; however, most of them show magnetic Curie temperature much lower than room temperature, which drastically hampers their application. Here, by performing first-principle calculations and building effective model Hamiltonians, we reveal a molecular orbital-mediated magnetic coupling mechanism in two-dimensional Cr(pyz)2 (pyz=pyrazine), and the role that the valence state of the molecule plays in determining the magnetic coupling type between metal ions. Based on these, we demonstrate that a two-dimensional organic-inorganic room-temperature multiferroic, Cr(h-fpyz)2 (h-fpyz= half-fluoropyrazine), can be rationally designed by introducing ferroelectricity in Cr(pyz)2 while keeping the valence state of the molecule unchanged. Our work not only reveals the origin of magnetic coupling in 2D organic-inorganic systems, but also provides a way to design room temperature multiferroic materials rationally.

cond-mat.mtrl-sci↗

arXiv2022

Stability of ferroelectric bubble domains

Nanoscale ferroelectric topologies such as vortices, anti-vortices, bubble patterns etc. are stabilized in thin films by a delicate balance of both mechanical and electrical boundary conditions. A systematic understanding of the phase stability of bubble domains, particularly when the above factors act simultaneously, remains elusive. Here we present first-principle-based simulations in combination with scanning probe microscopy of ultrathin epitaxial (001) PbZr0.4Ti0.6O3 heterostructures to address this gap. The simulations predict that as-grown labyrinthine domains will transform to bubbles under combinations of reduced film thickness, increased mechanical pressure and/or improved electrical screening. These topological transitions are explained by a common fundamental mechanism. Namely, we argue that, independently of the nature of the driving force, the evolution of the domain morphology allows the system to conserve its original residual depolarization field. Thereby, the latter remains pinned to a value determined by an external or built-in electric bias. To verify our predictions, we then exploit tomographic atomic force microscopy to achieve the concurrent effect of reducing film thickness and increased mechanical stimulus. The results provide a systematic understanding of phase stability and demonstrate controlled manipulation of nanoscale ferroelectric bubble domains.

cond-mat.mtrl-sci↗

arXiv2021

Magnetoelastic standing waves induced in UO$_{2}$ by microsecond magnetic field pulses

Magnetoelastic measurements in the piezomagnetic antiferromagnet UO$_{2}$ were performed via the fiber Bragg grating method in magnetic fields up to $150\,\mathrm{T}$ generated by a single-turn coil setup. We show that in short timescales, order of a few micro seconds, pulsed-magnetic fields excite mechanical resonances at temperatures ranging from $10\,\mathrm{K}$ to $300\,\mathrm{K}$, in the paramagnetic as well as within the robust antiferromagnetic state of the material. These resonances, which are barely attenuated within the 100 ms observations, are attributed to the strong magnetoelastic coupling in UO$_{2}$ combined with the high crystallographic quality of the single crystal samples. They compare well with mechanical resonances obtained by a resonant ultrasound technique and superimpose on the known non-monotonic magnetostriction background. A clear phase-shift of $π$ in the lattice oscillations is, unexpectedly, observed in the antiferromagnetic state when the magnetic field overcomes the piezomagnetic switch-field $H_c \simeq -18\,\mathrm{T}$. We further present simulations and a theoretical argument to explain the observed phenomena.

cond-mat.mtrl-sci↗

arXiv2021

Super-R BiFeO$_3$: Epitaxial stabilization of a low-symmetry phase with giant electromechanical response

Piezoelectrics interconvert mechanical energy and electric charge and are widely used in actuators and sensors. The best performing materials are ferroelectrics at a morphotropic phase boundary (MPB), where several phases can intimately coexist. Switching between these phases by electric field produces a large electromechanical response. In the ferroelectric BiFeO$_3$, strain can be used to create an MPB-like phase mixture and thus to generate large electric field dependent strains. However, this enhanced response occurs at localized, randomly positioned regions of the film, which potentially complicates nanodevice design. Here, we use epitaxial strain and orientation engineering in tandem - anisotropic epitaxy - to craft a hitherto unavailable low-symmetry phase of BiFeO$_3$ which acts as a structural bridge between the rhombohedral-like and tetragonal-like polymorphs. Interferometric displacement sensor measurements and first-principle calculations reveal that under external electric bias, this phase undergoes a transition to the tetragonal-like polymorph, generating a piezoelectric response enhanced by over 200%, and associated giant field-induced reversible strain. These results offer a new route to engineer giant electromechanical properties in thin films, with broader perspectives for other functional oxide systems.

cond-mat.mtrl-sci↗

arXiv2020

Effect of the polar distortion on the thermoelectric properties of GeTe

First principle calculations are performed to investigate the effect of polar order strength on the thermoelectric (TE) properties of GeTe alloy in its rhombohedral structure. The variation in the polarization state using various ferroelectric distortions λ (λ=0,0.5,1.0,1.25,1.5) allows to change the thermoelectric properties to a large extent. The polar structure with a high polarization mode (λ=1.5) tends to show a higher TE efficiency than the cubic structure at high temperatures. Thus, polarization engineering may play a key role in designing efficient thermoelectric devices. In particular, high TE performances could be achieved by growing epitaxial GeTe films that bi-axially compress the directions perpendicular to the polar axis, which may help to tune the Curie temperature.

physics.comp-ph↗

arXiv2019

Uncompensated Polarization in Incommensurate Modulations of Perovskite Antiferroelectrics

Complex polar structures of incommensurate modulations (ICMs) are revealed in chemically modified PbZrO$_3$ perovskite antiferroelectrics using advanced transmission electron microscopy techniques. The Pb-cation displacements, previously assumed to arrange in a fully-compensated antiparallel fashion, are found to be either antiparallel but with different magnitudes, or in a nearly orthogonal arrangement in adjacent stripes in the ICMs. Ab initio calculations corroborate the low-energy state of these arrangements. Our discovery corrects the atomic understanding of ICMs in PbZrO$_3$-based perovskite antiferroelectrics.

cond-mat.mtrl-sci↗

arXiv2019

Strain Control and Layer-Resolved Switching of Negative Capacitance in BaTiO$_3$/SrTiO$_3$ Superlattices

Negative capacitance in BaTiO$_3$/SrTiO$_3$ superlattices is investigated by Monte Carlo simulations in an atomistic effective Hamiltonian model, using fluctuation formulas for responses to the local macroscopic field that incorporates depolarizing fields. We show epitaxial strain can tune the negative capacitance of the BaTiO$_3$ ferroelectric layer and the overall capacitance of the system over a broad temperature range. In addition, we predict and explain an original switching of the negative capacitance from the BaTiO$_3$ layer to the SrTiO$_3$ layer at low temperatures for intermediate strains. Our results indicate how the diffusive character of the multidomain transition in these superlattices improves their viability for capacitance applications.

cond-mat.mtrl-sci↗

arXiv2019

Ferroelectricity with Asymmetric Hysteresis in Metallic LiOsO3 Ultrathin Films

Bulk LiOsO3 was experimentally identified as a "ferroelectric" metal where polar distortions coexist with metallicity [Shi et al., Nature Materials 12, 1024 (2013)]. It is generally believed that polar displacements in a "ferroelectric" metal cannot be switched by an external electric field. Here, via comprehensive density functional theory calculations, we demonstrate that a two-unit-cell-thick LiOsO3 thin film exhibits a ferroelectric ground state having an out-of-plane electric dipole moment that can be switched by an external electric field. Moreover, its dipole moment-versus-electric-field hysteresis loop is asymmetric because only surface Li ions'displacements are reversed by external electric field whereas the field-induced force on inner Li atoms are nearly fully screened by itinerant electrons. As a relevant by-product of our study, we also extend the concept of "Born effective charge" to finite metallic systems, and show its usefulness to rationalize the observed effects.

physics.comp-ph↗

arXiv2018

On the magnetoelastic and magnetoelectric couplings across the antiferromagnetic transition in multiferroic BiFeO3

Clear anomalies in the lattice thermal expansion (deviation from linear variation) and elastic properties (softening of the sound velocity) at the antiferromagnetic-to-paramagnetic transition are observed in the prototypical multiferroic BiFeO3 using a combination of picosecond acoustic pump-probe and high-temperature X-ray diffraction experiments. Similar anomalies are also evidenced using first-principles calculations supporting our experimental findings. Those calculations in addition to a simple Landau-like model we also developed allow to understand the elastic softening and lattice change at T_N as a result of magnetostriction combined with electrostrictive and magnetoelectric couplings which renormalize the elastic constants of the high-temperature reference phase when the critical T_N temperature is reached.

cond-mat.mtrl-sci↗

arXiv2018

Intrinsic Origin of Enhancement of Ferroelectricity in SnTe Ultrathin Films

Previous studies showed that, as ferroelectric films become thinner, their Curie temperature (Tc) and polarization below Tc both typically decrease. In contrast, a recent experiment [Chang et al., Science 353, 274 (2016)] observed that atomic-thick SnTe films have a higher Tc than their bulk counterpart, which was attributed to extrinsic effects. Here, we find, using first-principles calculations, that the 0K energy barrier for the polarization switching (which is a quantity directly related to Tc) is higher in most investigated defect-free SnTe ultrathin films than that in bulk SnTe, and that the 5-unit-cell (UC) SnTe thin film has the largest energy barrier as a result of an interplay between hybridization interactions and Pauli repulsions. Further simulations, employing a presently developed effective Hamiltonian, confirm that free-standing defect-free SnTe thin films have a higher Tc than bulk SnTe, except for the 1-UC case. Our work therefore demonstrates the possibility to intrinsically enhance ferroelectricity of ultrathin films by reducing their thickness.

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↗

arXiv2015

A multiferroic on the brink: uncovering the nuances of strain-induced transitions in BiFeO$_3$

Bismuth ferrite (BiFeO$_3$) is one of the very few known single-phase multiferroic materials. While the bulk compound is rhombohedral (R), the discovery of an epitaxial strain-induced structural transition into a so-called 'super tetragonal-phase' (T-phase) in this material incited a flurry of research activity focused on gaining an understanding of this phase transition and its possible functionalities. This metastable phase of BiFeO$_3$ is also multiferroic, with giant ferroelectric polarization and coexisting antiferromagnetic order, but above all it is the strain relaxation-induced phase mixtures and their outstanding piezoelectric and magnetoelectric responses which continue to intrigue and motivate the physicist and materials scientist communities. Here, we review the research into the T-phase and mixed-phase BiFeO$_3$ system. We begin with a brief summary of the history of the T-phase and an analysis of the structure of the various phases reported in the literature. We then address important questions regarding the symmetry and octahedral rotation patterns and the (as yet underexplored) important role of chemistry in the formation of the metastable T-phase. We follow by describing the phase transitions in this material, and how these may hold promise for large magnetoelectric responses. Finally we point out some experimental challenges inherent to the study of such a system, and potential pathways for how they may be overcome. It is our intention with this work to highlight important issues that, in our opinion, should be carefully considered by the community in order to use this fascinating materials system for a new paradigm of functionality.

cond-mat.mtrl-sci↗

arXiv2014

Prediction of novel interface-driven spintronic effects

The recently-proposed coupling between the angular momentum density and magnetic moment [A. Raeliarijaona et al, Phys. Rev. Lett. 110, 137205 (2013)] is shown here to result in the prediction of (i) novel spin currents generated by an electrical current and (ii) new electrical currents induced by a spin current in systems possessing specific interfaces between two different materials. Some of these spin (electrical) currents can be reversed near the interface by reversing the applied electrical (spin) current. Similarities and differences between these novel spintronic effects and the well-known spin Hall and inverse spin Hall effects are also discussed.

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

Novel magnetic arrangement and structural phase transition induced by spin-lattice coupling in multiferroics

Using an effective Hamiltonian of mutiferroic BiFeO$_3$ (BFO) as a toy model, we explore the effect of the coefficient, C, characterizing the strength of the spin-current interaction, on physical properties. We observe that for larger C values and below a critical temperature, the magnetic moments organize themselves in a novel cycloid which propagates along a low-symmetry direction and is associated with a structural phase transition from polar rhombohedral to a polar triclinic state. We emphasize that both of these magnetic and structural transitions are results of a remarkable self-organization of different solutions of the spin-current model.

cond-mat.mtrl-sci↗