arXiv subjects

L. Bellaiche

Publications and source records attributed to L. Bellaiche.

At least 19 recordsLinked to original sources

arXiv2026

Deformation-Potential-Driven Photostriction in Layered Ferroelectrics

The coupling between electronic excitations and lattice deformation in van der Waals ferroelectrics is governed by a competition between the electron deformation potential and the inverse piezoelectric effect. While theory predicts that piezoelectric screening should drive a polar-axis contraction in monolayer group-IV monochalcogenides, we demonstrate that in multilayer SnS, the deformation potential provides the dominant contribution, driving a polar-axis expansion even within ferroelectric domains. By correlating polarization-resolved second-harmonic generation microscopy with ultrafast reflectance spectroscopy and first-principles calculations, we resolve the anisotropic lattice response and disentangle intrinsic photostrictive strain from extrinsic thin-film interference artifacts. These results establish a microscopic hierarchy of photostrictive mechanisms and position stacking-engineered SnS as a platform for ultrafast optomechanical transduction.

cond-mat.mtrl-sci↗

arXiv2024

Superorders and acoustic modes folding in BiFeO$_3$/LaFeO$_3$ superlattices

Superlattices are materials created by the alternating growth of two chemically different materials. The direct consequence of creating a superlattice is the folding of the Brillouin zone which gives rise to additional electronic bands and phonon modes. This has been successfully exploited to achieve new transport and optical properties in semiconductor superlattices, for example. Here, we show that multiferroic BiFeO$_3$/LaFeO$_3$ superlattices are more than just periodic chemical stacking. Using transmission electron microscopy, X-ray diffraction and first-principles calculations, we demonstrate the existence of a new order of FeO$_6$ octahedra, with a period along the growth direction about twice that of the chemical supercell, i.e. a superorder. The effect of this new structural order on the lattice dynamics is studied with ultrafast optical pump-probe experiments. While a mode at 1.2 THz is attributed solely to the chemical modulation of the superlattice, the existence of another 0.7 THz mode seems to be explained only by a double Brillouin zone folding in agreement with the structural description. Our work shows that multiferroic BiFeO$_3$/LaFeO$_3$ superlattices can be used to tune the spectrum of coherent THz phonons, and potentially that of magnons or electromagnons.

cond-mat.mtrl-sci↗

arXiv2023

Quantum criticality at cryogenic melting of polar bubble lattices

Quantum fluctuations (QFs) caused by zero-point phonon vibrations (ZPPVs) are known to prevent the occurrence of polar phases in bulk incipient ferroelectrics down to 0K1-3. On the other hand, little is known about the effects of QFs on the recently discovered topological patterns in ferroelectric nanostructures4-9. Here, by using an atomistic effective Hamiltonian within classical Monte Carlo (CMC) and path integral quantum Monte Carlo (PI-QMC)1,3,10,11, we unveil how QFs affect the topology of several dipolar phases in ultrathin Pb(Zr0.4Ti0.6)O3 (PZT) films. In particular, our PI-QMC simulations show that the ZPPVs do not suppress polar patterns but rather stabilize the labyrinth4, bimeron5 and bubble phases12,13 within a wider range of bias field magnitudes. Moreover, we reveal that quantum fluctuations induce a quantum critical point (QCP) separating a hexagonal bubble lattice from a liquid-like state characterized by spontaneous motion, creation and annihilation of polar bubbles at cryogenic temperatures. Finally, we show that the discovered quantum melting is associated with anomalous physical response, as, e.g., demonstrated by a negative longitudinal piezoelectric coefficient.

cond-mat.mtrl-sci↗

arXiv2023

Strain Dependent Spin Hall Magnetoresistance in the Multiferroic Antiferromagnet BiFeO$_3$

The spin Hall magnetoresistance (SMR) of epitaxial BiFeO$_3$ thin films is investigated. SMR consistent with ferromagnetic interfacial states for BiFeO$_3$ films fabricated on (001) SrTiO$_3$ (R' BFO) and LaAlO$_3$ (T' BFO) substrates is found, albeit with different temperature dependencies. For T' BFO, the SMR is enhanced at room temperature, and decays with reduced temperatures. By contrast, R' BFO shows a monotonic decrease in SMR response with increasing temperature, mirroring the trend of a weak ferromagnet. Density functional theory shows that this difference originates from the coupling of the applied magnetic field to oxygen octahedral rotation (R') and spin (T') degrees of freedom.

cond-mat.mtrl-sci↗

arXiv2023

Active learning of effective Hamiltonian for super-large-scale atomic structures

The first-principles-based effective Hamiltonian scheme provides one of the most accurate modeling technique for large-scale structures, especially for ferroelectrics. However, the parameterization of the effective Hamiltonian is complicated and can be difficult for some complex systems such as high-entropy perovskites. Here, we propose a general form of effective Hamiltonian and develop an active machine learning approach to parameterize the effective Hamiltonian based on Bayesian linear regression. The parameterization is employed in molecular dynamics simulations with the prediction of energy, forces, stress and their uncertainties at each step, which decides whether first-principles calculations are executed to retrain the parameters. Structures of BaTiO$_3$, Pb(Zr$_{0.75}$Ti$_{0.25}$)O$_3$ and (Pb,Sr)TiO$_3$ system are taken as examples to show the accuracy of this approach, as compared with conventional parametrization method and experiments. This machine learning approach provides a universal and automatic way to compute the effective Hamiltonian parameters for any considered complex systems with super-large-scale (more than $10^7$ atoms) atomic structures.

cond-mat.mtrl-sci↗

arXiv2023

Realistic Spin Model for Multiferroic NiI$_2$

A realistic first-principle-based spin Hamiltonian is constructed for the type-II multiferroic NiI$_2$, using a symmetry-adapted cluster expansion method. Besides single ion anisotropy and isotropic Heisenberg terms, this model further includes the Kitaev interaction and a biquadratic term, and can well reproduce striking features of the experimental helical ground state, that are, {\it e.g.}, a proper screw state, canting of rotation plane, propagation direction and period. Using this model to build a phase diagram, it is demonstrated that, (i) the in-plane propagation direction of $\langle1\bar10\rangle$ is determined by the Kitaev interaction, instead of the long-believed exchange frustrations; and (ii) the canting of rotation plane is also dominantly determined by Kitaev interaction, rather than interlayer couplings. Furthermore, additional Monte Carlo simulations reveal three equivalent domains and different topological defects. Since the ferroelectricity is induced by spins in type-II multiferroics, our work also implies that Kitaev interaction is closely related to the multiferroicity of NiI$_2$.

cond-mat.str-el↗

arXiv2023

Nonlinear phonon Hall effects in ferroelectrics: its existence and non-volatile electrical control

Nonlinear Hall effects have been previously investigated in non-centrosymmetric systems for electronic systems. However, they only exist in metallic systems and are not compatible with ferroelectrics since these latter are insulators, hence limiting their applications. On the other hand, ferroelectrics naturally break inversion symmetry and can induce a non-zero Berry curvature. Here, we show that a non-volatile electric-field control of heat current can be realized in ferroelectrics through the nonlinear phonon Hall effects. More precisely, based on Boltzmann equation under the relaxation-time approximation, we derive the equation for nonlinear phonon Hall effects, and further show that the behaviors of nonlinear phonon (Boson) Hall effects are very different from nonlinear Hall effects for electrons (Fermion). Our work provides a route for electric-field control of thermal Hall current in ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2023

Motion and teleportation of polar bubbles in ultra-thin ferroelectrics

Polar bubble domains are complex topological defects akin to magnetic skyrmions that can spontaneously form in ferroelectric thin films and superlattices. They can be deterministically written and deleted and exhibit a set of properties, such as sub-10 nm radius and room-temperature stability, that are highly attractive for dense data storage and reconfigurable nano-electronics technologies. However, possibilities of controlled motion of electric bubble skyrmions, a critical technology requirement currently remains missing. Here we present atomistic simulations that demonstrate how external electric-field perturbations can induce two types of motion of bubble skyrmions in low-dimensional tetragonal PbZr$_{0.4}$Ti$_{0.6}$O$_3$ systems under residual depolarizing field. Specifically, we show that, depending on the spatial profile and magnitude of the external field, bubble skyrmions can exhibit either a continuous motion driven by the external electric field gradient or a discontinuous, teleportation-like, skyrmion domain transfer. These findings provide the first analysis of dynamics and controlled motion of polar skyrmions that are essential for functionalization of these particle-like domain structures.

cond-mat.mtrl-sci↗

arXiv2022

Origin of negative electrocaloric effect in Pnma-type antiferroelectric perovskites

Anomalous electrocaloric effect (ECE) with decreasing temperature upon application of an electric field is known to occur in antiferroelectrics (AFEs), and previous understanding refers to the field-induced canting of electric dipoles if there is no phase transitions. Here, we use a first-principle-based method to study the ECE in Nd-substituted BiFeO3 (BNFO) perovskite solid solutions, which has the Pnma-type AFE ground state. We demonstrate another scenario to achieve and explain anomalous ECE, emphasizing that explicit consideration of octahedral tiltings is indispensable for a correct understanding. This mechanism may be general for AFEs for which the antipolar mode is not the primary order parameter. We also find that the negative ECE can reach a large magnitude in BNFO.

cond-mat.mtrl-sci↗

arXiv2022

Ferroelectric Solitons Crafted in Epitaxial Bismuth Ferrite Superlattices

In ferroelectrics, complex interactions among various degrees of freedom enable the condensation of topologically protected polarization textures. Known as ferroelectric solitons, these particle-like structures represent a new class of materials with promise for beyond CMOS technologies due to their ultrafine size and sensitivity to external stimuli. Such polarization textures have scarcely been reported in multiferroics. Here, we report a range of soliton topologies in bismuth ferrite strontium titanate superlattices. High-resolution piezoresponse force microscopy and Cs-corrected high-angle annular dark-field scanning transmission electron microscopy reveal a zoo of topologies, and polarization displacement mapping of planar specimens reveals center-convergent and divergent topological defects as small as 3 nm. Phase field simulations verify that some of these topologies can be classed as bimerons, with a topological charge of plus and minus one, and first-principles-based effective Hamiltonian computations show that the co-existence of such structures can lead to non-integer topological charges, a first observation in a BiFeO3-based system. Our results open new opportunities in multiferroic topotronics.

cond-mat.mtrl-sci↗

arXiv2021

Energy storage in lead-free Ba(Zr, Ti)O$_{3}$ relaxor ferroelectrics: Large densities and efficiencies and their origins

An atomistic first-principles-based effective Hamiltonian is used to investigate energy storage in Ba(Zr$_{0.5}$Ti$_{0.5}$)O$_{3}$ relaxor ferroelectrics, both in their bulk and epitaxial films' forms, for electric fields applied along different crystallographic directions. We find that the energy density linearly increases with temperature for electric fields applied along the pseudocubic [001], [110] and [111] directions in Ba(Zr$_{0.5}$Ti$_{0.5}$)O$_{3}$ bulk. For films at room temperature, the energy density adopts different behaviors (i.e., increase versus decrease) with strain depending on the direction of the applied electric fields. We also predicted ultrahigh energy densities (basically larger than 100 J/cm$^{3}$) with an ideal efficiency of 100\% in all these Ba(Zr$_{0.5}$Ti$_{0.5}$)O$_{3}$ systems. In addition, a phenomenological model is used to reveal the origin of all the aforementioned features, and should be applicable to other relaxor ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2021

Complex Spin Hamiltonian Represented by Artificial Neural Network

The effective spin Hamiltonian method is widely adopted to simulate and understand the behavior of magnetism. However, the magnetic interactions of some systems, such as itinerant magnets, are too complex to be described by any explicit function, which prevents an accurate description of magnetism in such systems. Here, we put forward a machine learning (ML) approach, applying an artificial neural network (ANN) and a local spin descriptor to develop effective spin potentials for any form of interaction. The constructed Hamiltonians include an explicit Heisenberg part and an implicit non-linear ANN part. Such a method successfully reproduces artificially constructed models and also sufficiently describe the itinerant magnetism of bulk Fe3GeTe2. Our work paves a new way for investigating complex magnetic phenomena (e.g., skyrmions) of magnetic materials.

cond-mat.mtrl-sci↗

arXiv2021

Ultrahigh energy storage density in epitaxial AlN/ScN superlattices

Dielectric and antiferroelectric materials are particularly promising for high-power energy-storage applications. However, relatively low energy density greatly hinders their usage in storage technologies. Here, we report first-principles-based calculations predicting that epitaxial and initially non-polar AlN/ScN superlattices can achieve an ultrahigh energy density of up to 200 J/cm$^{\textrm{3}}$, accompanied by an ideal efficiency of 100%. We also show that high energy density requires the system being neither too close nor too far from a ferroelectric phase transition under zero electric field. A phenomenological model is further proposed to rationalize such striking features.

cond-mat.mtrl-sci↗

arXiv2021

Electrocaloric effects in multiferroics

An atomistic effective Hamiltonian is used to compute electrocaloric (EC) effects in rare-earth substituted BiFeO$_{3}$ multiferroics. A phenomenological model is then developed to interpret these computations, with this model indicating that the EC coefficient is the sum of two terms, that involve electric quantities (polarization, dielectric response), the antiferromagnetic order parameter, and the coupling between polarization and antiferromagnetic order. The first one depends on the polarization and dielectric susceptibility, has the analytical form previously demonstrated for ferroelectrics, and is thus enhanced at the ferroelectric Curie temperature. The second one explicitly involves the dielectric response, the magnetic order parameter and a specific magnetoelectric coupling, and generates a peak of the EC response at the Néel temperature. These atomistic results and phenomenological model may be put in use to optimize EC coefficients.

cond-mat.mtrl-sci↗

arXiv2020

Linear versus nonlinear electro-optic effects in materials

Two schemes are proposed to compute the nonlinear electro-optic (EO) tensor for the first time. In the first scheme, we compute the linear EO tensor of the structure under a finite electric field, while we compute the refractive index of the structure under a finite electric field in the second scheme. Such schemes are applied to Pb(Zr,Ti)O$_{3}$ and BaTiO$_{3}$ ferroelectric oxides. It is found to reproduce a recently observed feature, namely why Pb(Zr$_{0.52}$Ti$_{0.48}$)O$_{3}$ adopts a mostly linear EO response while BaTiO$_{3}$ exhibits a strongly nonlinear conversion between electric and optical properties. Furthermore, the atomistic insight provided by the proposed ab-initio scheme reveals the origin of such qualitatively different responses, in terms of the field-induced behavior of the frequencies of some phonon modes and of some force constants.

cond-mat.mtrl-sci↗

arXiv2020

Berezinskii-Kosterlitz-Thouless Phase in Two-dimensional Ferroelectrics

The celebrated Berezinskii-Kosterlitz-Thouless (BKT) phase transition refers to a topological transition characterized, e.g., by the dissociation of vortex-antivortex pairs in two-dimensional (2D) systems. Such unusual phase has been reported in various types of materials, but never in the new class of systems made by one-unit-cell-thick (1UC) ferroelectrics (also coined as 2D ferroelectrics). Here, the use of a first-principles-based effective Hamiltonian method leads to the discovery of many fingerprints of a BKT phase existing in-between the ferroelectric and paraelectric states of 1UC tin tellurium being fully relaxed. Moreover, epitaxial strain is found to have dramatic consequences on the temperature range of such BKT phase for the 1UC SnTe. Consequently, our predictions extend the playground of BKT theory to a novel class of functional materials, and demonstrate that strain is an effective tool to alter BKT characteristics there.

cond-mat.mtrl-sci↗

arXiv2020

Possible Kitaev Quantum Spin Liquid State in 2D Materials with S=3/2

Quantum spin liquids (QSLs) form an extremely unusual magnetic state in which the spins are highly correlated and fluctuate coherently down to the lowest temperatures, but without symmetry breaking and without the formation of any static long-range-ordered magnetism. Such intriguing phenomena are not only of great fundamental relevance in themselves, but also hold the promise for quantum computing and quantum information. Among different types of QSLs, the exactly solvable Kitaev model is attracting much attention, with most proposed candidate materials, e.g., RuCl$_3$ and Na$_2$IrO$_3$, having an effective $S$=1/2 spin value. Here, via extensive first-principle-based simulations, we report the investigation of the Kitaev physics and possible Kitaev QSL state in epitaxially strained Cr-based monolayers, such as CrSiTe$_3$, that rather possess a $S$=3/2 spin value. Our study thus extends the playground of Kitaev physics and QSLs to 3$d$ transition metal compounds.

cond-mat.mtrl-sci↗

arXiv2019

Origin of sawtooth domain walls in ferroelectrics

Domains and domain walls are among the key factors that determine the performance of ferroelectric materials. In recent years, a unique type of domain walls, i.e., the sawtooth-shaped domain walls, has been observed in BiFeO$_{3}$ and PbTiO$_{3}$. Here, we build a minimal model to reveal the origin of these sawtooth-shaped domain walls. Incorporating this model into Monte-Carlo simulations shows that (i) the competition between the long-range Coulomb interaction (due to bound charges) and short-range interaction (due to opposite dipoles) is responsible for the formation of these peculiar domain walls and (ii) their relative strength is critical in determining the periodicity of these sawtooth-shaped domain walls. Necessary conditions to form such domain walls are also discussed.

cond-mat.mtrl-sci↗