arXiv subjects

Laurent Bellaiche

Publications and source records attributed to Laurent Bellaiche.

At least 55 records · Page 3Linked to original sources

arXiv2024

General theory for longitudinal nonreciprocal charge transport

The longitudinal nonreciprocal charge transport (NCT) in crystalline materials is a highly non-trivial phenomenon, motivating the design of next generation two-terminal rectification devices (e.g., semiconductor diodes beyond PN junctions). The practical application of such devices is built upon crystalline materials whose longitudinal NCT occurs at room temperature and under low magnetic field. However, materials of this type are rather rare and elusive, and theory guiding the discovery of these materials is lacking. Here, we develop such a theory within the framework of semiclassical Boltzmann transport theory. By symmetry analysis, we classify the complete 122 magnetic point groups with respect to the longitudinal NCT phenomenon. The symmetry-adapted Hamiltonian analysis further uncovers a previously overlooked mechanism for this phenomenon. Our theory guides the first-principles prediction of longitudinal NCT in multiferroic ε-Fe2O3 semiconductor that possibly occurs at room temperature, without the application of external magnetic field. These findings advance our fundamental understandings of longitudinal NCT in crystalline materials, and aid the corresponding materials discoveries.

cond-mat.mtrl-sci↗

arXiv2024

Non-volatile spin transport in a single domain multiferroic

Antiferromagnets have attracted significant attention in the field of magnonics, as promising candidates for ultralow-energy carriers for information transfer for future computing. The role of crystalline orientation distribution on magnon transport has received very little attention. In multiferroics such as BiFeO$_3$ the coupling between antiferromagnetic and polar order imposes yet another boundary condition on spin transport. Thus, understanding the fundamentals of spin transport in such systems requires a single domain, a single crystal. We show that through Lanthanum(La) substitution, a single ferroelectric domain can be engineered with a stable, single-variant spin cycloid, controllable by an electric field. The spin transport in such a single domain displays a strong anisotropy, arising from the underlying spin cycloid lattice. Our work shows a pathway to understand the fundamental origins of spin transport in such a single domain multiferroic.

cond-mat.mtrl-sci↗

arXiv2024

Electro-optic properties from ab initio calculations in two-dimensional materials

Electro-optic (EO) effects relate the change of optical constants by low-frequency electric fields. Thanks to the advent of Density Functional Perturbation Theory (DFPT), the EO properties of bulk three-dimensional (3D) materials can now be calculated in an ab initio way. However, the use of periodic boundary conditions in most Density Functional Theory codes imposes to simulate two-dimensional (2D) materials using slabs surrounded by a large layer of vacuum. The EO coefficients predicted from such calculations, if not rescaled properly, can severely deviate from the real EO properties of 2D materials. The present work discusses the issue and introduces the rescaling relationships allowing to recover the true EO properties.

cond-mat.mtrl-sci↗

arXiv2024

Ultrastrong coupling between polar distortion and optical properties in ferroelectric MoBr$_2$O$_2$

Tuning the properties of materials using external stimuli is crucial for developing versatile smart materials. A strong coupling among order parameters within a single-phase material constitutes a potent foundation for achieving precise property control. However, cross-coupling is pretty weak in most single materials. Leveraging first principles calculations, we demonstrate the layered mixed anion compound MoBr$_2$O$_2$ exhibits electric-field switchable spontaneous polarization and ultrastrong coupling between polar distortion and electronic structures as well as optical properties. It offers feasible avenues of achieving tunable Rashba spin-splitting, electrochromism, thermochromism, photochromism, and nonlinear optics by applying an external electric field to a single domain sample, heating, as well as intense light illumination. Additionally, it exhibits an exceptionally large photostrictive effect. These findings not only showcase the feasibility of achieving multiple order parameter coupling within a single material, but also pave the way for comprehensive applications based on property control, such as energy harvesting, information processing, and ultrafast control.

cond-mat.mtrl-sci↗

arXiv2023

Revealing the Three-Dimensional Arrangement of Polar Topology in Nanoparticles

In the early 2000s, low dimensional systems were predicted to have topologically nontrivial polar structures, such as vortices or skyrmions, depending on mechanical or electrical boundary conditions. A few variants of these structures have been experimentally observed in thin film model systems, where they are engineered by balancing electrostatic charge and elastic distortion energies. However, the measurement and classification of topological textures for general ferroelectric nanostructures have remained elusive, as it requires mapping the local polarization at the atomic scale in three dimensions. Here we unveil topological polar structures in ferroelectric BaTiO3 nanoparticles via atomic electron tomography, which enables us to reconstruct the full three-dimensional arrangement of cation atoms at an individual atom level. Our three-dimensional polarization maps reveal clear topological orderings, along with evidence of size-dependent topological transitions from a single vortex structure to multiple vortices, consistent with theoretical predictions. The discovery of the predicted topological polar ordering in nanoscale ferroelectrics, independent of epitaxial strain, widens the research perspective and offers potential for practical applications utilizing contact-free switchable toroidal moments.

cond-mat.mtrl-sci↗

arXiv2023

Engineering magnetic domain wall energies in multiferroic BiFeO$_3$ via epitaxial strain

Epitaxial strain has emerged as a powerful tool to tune magnetic and ferroelectric properties in functional materials such as in multiferroic perovskite oxides. Here, we use first-principles calculations to explore the evolution of magnetic interactions in the antiferromagnetic multiferroic BiFeO$_3$ (BFO), one of the most promising multiferroics for future technology. The epitaxial strain in BFO(001) oriented film is varied between $\varepsilon_{xx,yy}$ $\in$ $[-2\%, +2\%]$. We find that both strengths of the exchange interaction and Dzyaloshinskii-Moriya interaction (DMI) decrease linearly from compressive to tensile strain whereas the uniaxial magnetocrystalline anisotropy follows a parabolic behavior which lifts the energy degeneracy of the (111) easy plane of bulk BFO. From the trends of the magnetic interactions we can explain the destruction of cycloidal order in compressive strain as observed in experiments due to the increasing anisotropy energy. For tensile strain, we predict that the ground state remains unchanged as a function of strain. By using the domain wall (DW) energy, we envision the region where isolated chiral magnetic texture might occur as function of strain i.e. where the DW and the spin spiral energy are equal. This transition between $-1.5\%$ and $-0.5\%$ of strain should allow topologically stable magnetic states such as antiferromagnetic skyrmions and merons to occur. Hence, our work should trigger experimental and theoretical investigations in this range of strain.

cond-mat.mtrl-sci↗

arXiv2023

Towards Ultimate Memory with Single-Molecule Multiferroics

The demand for high-density storage is urgent in the current era of data explosion. Recently, several single-molecule (-atom) magnets/ferroelectrics have been reported to be promising candidates for high-density storage. As another promising candidate, single-molecule multiferroics are not only small but also possess ferroelectric and magnetic orderings, which can sometimes be strongly coupled and used as data storages to realize the combination of electric writing and magnetic reading. However, they have been rarely proposed, and never been experimentally reported. Here, by building Hamiltonian models, we propose a new model of single-molecule multiferroic in which electric dipoles and magnetic moments are parallel and can rotate with the rotation of the single molecule. Furthermore, with performing spin-lattice dynamics simulations, we reveal the conditions (e.g., large enough single-ion anisotropy and appropriate electric field) under which the new single-molecule multiferroic can arise. Based on this model, as well as first-principles calculations, a realistic example Co(NH3)4N@SWCNT is constructed and numerically confirmed to demonstrate the feasibility of the new single-molecule multiferroic model. Our work not only sheds light on the discovery of single-molecule multiferroics but also provides a new guideline to design multifunctional materials for ultimate memory devices.

cond-mat.mtrl-sci↗

arXiv2023

Engineering ferroelectricity in monoclinic hafnia

Ferroelectricity in the complementary metal-oxide semiconductor (CMOS)-compatible hafnia (HfO$_2$) is crucial for the fabrication of high-integration nonvolatile memory devices. However, the capture of ferroelectricity in HfO$_2$ requires the stabilization of thermodynamically-metastable orthorhombic or rhombohedral phases, which entails the introduction of defects (e.g., dopants and vacancies) and pays the price of crystal imperfections, causing unpleasant wake-up and fatigue effects. Here, we report a theoretical strategy on the realization of robust ferroelectricity in HfO$_2$-based ferroelectrics by designing a series of epitaxial (HfO$_2$)$_1$/(CeO$_2$)$_1$ superlattices. The advantages of the designated ferroelectric superlattices are defects free, and most importantly, on the base of the thermodynamically stable monoclinic phase of HfO$_2$. Consequently, this allows the creation of superior ferroelectric properties with an electric polarization $>$25 $μ$C/cm$^2$ and an ultralow polarization-switching energy barrier at $\sim$2.5 meV/atom. Our work may open an entirely new route towards the fabrication of high-performance HfO$_2$ based ferroelectric devices.

cond-mat.mtrl-sci↗

arXiv2023

Highly spin-polarized carriers and strong ferromagnetism in doped perovskite antiferromagnetic semiconductors

In semiconductor spintronics, the generation of highly spin-polarized carriers and the efficient probe of spin order (due to strong ferromagnetism) -- at or above room temperature -- are crucial because it allows for the design of spin-based semiconductor devices. Usually, such goals were fulfilled in room-temperature ferromagnetic semiconductors, being rare materials in nature. While room-temperature antiferromagnetic semiconductors are plentiful, the possibility for creating highly spin-polarized carriers and strong ferromagnetism in these materials remain to be unraveled. Here, we explore such a possibility by first-principles simulations, working with CaTcO$_3$ and NaOsO$_3$ perovskites -- being room-temperature antiferromagnetic semiconductors. We find that doping them by electrons or holes results in these materials to be highly spin-polarized, carrying enormous ferromagnetic moments. Doping electrons with moderate carrier density can yield strong ferromagnetism in them, with the ferromagnetic moments being comparable to that in typical ferromagnetic semiconductors. Our work thus indicates the merit of perovskite antiferromagnetic semiconductors in spintronics -- for a possible replacement of ferromagnetic semiconductors.

cond-mat.mtrl-sci↗

arXiv2023

Energy storage properties of ferroelectric nanocomposites

An atomistic effective Hamiltonian technique is used to investigate the finite-temperature energy storage properties of a ferroelectric nanocomposite consisting of an array of BaTiO$_{3}$ nanowires embedded in a SrTiO$_{3}$ matrix, for electric field applied along the long axis of the nanowires. We find that the energy density \textit{versus} temperature curve adopts a nonlinear, mostly temperature-independent response when the system exhibits phases possessing an out-of-plane polarization and vortices while the energy density more linearly increases with temperature when the nanocomposite either only possesses vortices (and thus no spontaneous polarization) or is in a paraelectric and paratoroidic phase for its equilibrium state. Ultrahigh energy density up to $\simeq$140 J/cm$^{3}$ and an ideal 100% efficiency are also predicted in this nanocomposite. A phenomenological model, involving a coupling between polarization and toroidal moment, is further proposed to interpret these energy density results.

cond-mat.mtrl-sci↗

arXiv2023

Hexagonal close-packed polar-skyrmion lattice in ultrathin ferroelectric PbTiO3 films

Polar skyrmions are topologically stable, swirling polarization textures with particle-like characteristics, which hold promise for next-generation, nanoscale logic and memory. While understanding of how to create ordered polar skyrmion lattice structures and how such structure respond to applied electric fields, temperature, and film thickness remains elusive. Here, using phase-field simulations, the evolution of polar topology and the emergence of a phase transition to a hexagonal close-packed skyrmion lattice is explored through the construction of a temperature-electric field phase diagram for ultrathin ferroelectric PbTiO3 films. The hexagonal-lattice skyrmion crystal can be stabilized under application of an external, out-of-plane electric field which carefully adjusts the delicate interplay of elastic, electrostatic, and gradient energies. In addition, the lattice constants of the polar skyrmion crystals are found to increase with film thickness, consistent with expectation from Kittel law. Our studies pave the way for the development of novel ordered condensed matter phases assembled from topological polar textures and related emergent properties in nanoscale ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2023

Electric-field-induced formation and annihilation of skyrmions in two-dimensional magnet

Electric manipulation of skyrmions in 2D magnetic materials has garnered significant attention due to the potential in energy-efficient spintronic devices. In this work, using first-principles calculations and Monte Carlo simulations, we report the electric-field-tunable magnetic skyrmions in MnIn2Te4 monolayer. By adjusting the magnetic parameters, including the Heisenberg exchange interaction, DMI, and MAE, through applying an electric field, the formation or annihilation of skyrmions can be achieved. Our work suggests a platform for experimental realization of the electric-field-tunable magnetic skyrmions in 2D magnets.

cond-mat.mtrl-sci↗

arXiv2023

The anti-symmetric and anisotropic symmetric exchange interactions between electric dipoles in hafnia

The anti-symmetric and anisotropic symmetric exchange interactions between two magnetic dipole moments - responsible for intriguing magnetic textures (e.g., magnetic skyrmions) - have been discovered since last century, while their electric analogues were either hidden for a long time or still not known. As a matter of fact, it is only recently that the anti-symmetric exchange interactions between electric dipoles was proved to exist (with materials hosting such an interaction being still rare) and the existence of anisotropic symmetric exchange interaction between electric dipoles remains to be revealed. Here, by symmetry analysis and first-principles calculations, we identify a candidate material in which our aforementioned exchange interactions between electric dipoles are perceptible. More precisely, we find that various phases of hafnia showcase non-collinear alignment of electric dipoles, which is interpreted by our phenomenological theories. This gives evidence that hafnia simultaneously accommodates anti-symmetric and anisotropic symmetric exchange interactions between electric dipoles. Our findings can hopefully deepen the current knowledge of electromagnetism in ferroelectrics, magnets and multiferroics, and have a potential to guide the discovery of novel states of matter (e.g., electric skyrmions) in hafnia and related materials.

cond-mat.mtrl-sci↗

arXiv2023

Flexoelectricity-stabilized ferroelectric phase with enhanced reliability in ultrathin La:HfO2 films

Doped HfO2 thin films exhibit robust ferroelectric properties even for nanometric thicknesses, are compatible with current Si technology and thus have great potential for the revival of integrated ferroelectrics. Phase control and reliability are core issues for their applications. Here we show that, in (111)-oriented 5%La:HfO2 (HLO) epitaxial thin films deposited on (La0.3Sr0.7)(Al0.65Ta0.35)O3 substrates, the flexoelectric effect, arising from the strain gradient along the films normal, induces a rhombohedral distortion in the otherwise Pca21 orthorhombic structure. Density functional calculations reveal that the distorted structure is indeed more stable than the pure Pca21 structure, when applying an electric field mimicking the flexoelectric field. This rhombohedral distortion greatly improves the fatigue endurance of HLO thin films by further stabilizing the metastable ferroelectric phase against the transition to the thermodynamically stable non-polar monoclinic phase during repetitive cycling. Our results demonstrate that the flexoelectric effect, though negligibly weak in bulk, is crucial to optimize the structure and properties of doped HfO2 thin films with nanometric thicknesses for integrated ferroelectric applications.

cond-mat.mtrl-sci↗

arXiv2023

Dynamics of polar vortex crystallization

Vortex crystals are commonly observed in ultra-thin ferroelectrics. However, a clear physical picture of origin of this topological state is currently lacking. Here, we show that vortex crystallization in ultra-thin Pb(Zr0.4,Ti0.6)O3 films stems from the softening of a phonon mode and can be thus described as a SU(2) symmetry-breaking transition. This result sheds light on the topology of the polar vortex patterns and bridges polar vortices with smectic phases, spin spirals, and other modulated states. Finally, we predict an ac-field driven resonant switching of the vortex tube orientation which could enable new low-power electronic technologies.

cond-mat.mtrl-sci↗

arXiv2023

Dynamical control of topology in ferroelectric skyrmions via twisted light

Twisted light carries a non-zero orbital angular momentum, that can be transferred from light to electrons and particles ranging from nanometers to micrometers. Up to now, the interplay between twisted light with dipolar systems has scarcely been explored, though the latter bear abundant forms of topologies such as skyrmions and embrace strong light-matter coupling. Here, using first-principles-based simulations, we show that twisted light can excite and drive dynamical polar skyrmions and transfer its nonzero winding number to ferroelectric ultrathin films. The skyrmion is successively created and annihilated alternately at the two interfaces, and experiences a periodic transition from a markedly "Bloch" to "Neel" character, accompanied with the emergence of a "Bloch point" topological defect with vanishing polarization. The dynamical evolution of skyrmions is connected to a constant jump of topological number between "0" and "1" over time. These intriguing phenomena are found to have an electrostatic origin. Our study thus demonstrates that, and explains why, this unique light-matter interaction can be very powerful in creating and manipulating topological solitons in functional materials.

cond-mat.mes-hall↗

arXiv2022

Microscopic Origin of the Electric Dzyaloshinskii-Moriya Interaction

The microscopic origin of the electric Dzyaloshinskii-Moriya interaction (eDMI) is unveiled and discussed by analytical analysis and first-principles based calculations. As similar to the magnetic Dzyaloshinskii-Moriya interaction (mDMI), eDMI also originates from electron-mediated effect and more specifically from certain electron hoppings that are being activated due to certain local inversion symmetry breaking. However, the eDMI energy is found to be at least a third-order interaction in atomic displacements instead of bilinear in magnetic dipole moments for mDMI. Furthermore, the eDMI energy form is presented, and we find that novel electrical topological defects (namely, chiral electric bobbers) can arise from this eDMI. Thus unraveling the microscopic origin of eDMI has the potential to lead to, and explain, the discovery of novel polar topological phases.

cond-mat.mtrl-sci↗

arXiv2022

A new look at the temperature-dependent properties of the antiferroelectric model PbZrO3: an effective Hamiltonian study

A novel atomistic effective Hamiltonian scheme, incorporating an original and simple bilinear energetic coupling, is developed and used to investigate the temperature dependent physical properties of the prototype antiferroelectric PbZrO3 (PZO) system. This scheme reproduces very well the known experimental hallmarks of the complex Pbam orthorhombic phase at low temperatures and the cubic paraelectric state of Pm 3m symmetry at high temperatures. Unexpectedly, it further predicts a novel intermediate state also of Pbam symmetry, but in which anti-phase oxygen octahedral tiltings have vanished with respect to the Pbam ground state. Interestingly, such new state exhibits a large dielectric response and thermal expansion that remarkably agree with previous experimental observations and the x-ray experiments we performed. We also conducted direct first-principles calculations at 0K which further support such low energy phase. Within this fresh framework, a re-examination of the properties of PZO is thus called for.

cond-mat.mtrl-sci↗