arXiv subjects

Louis Bastogne

Publications and source records attributed to Louis Bastogne.

13 recordsLinked to original sources

arXiv2026

First-order polarization process as an alternative to antiferroelectricity

Antiferroelectrics generate significant interest since their polarization versus electric field (PE) curves show typical double-hysteresis loops appealing for various applications. Unfortunately, antiferroelectrics are rare. In magnetic compounds, magnetization versus magnetic field (M-H) curves can show analogous double hysteresis loops not only in antiferromagnets but also in systems exhibiting field-induced first-order reorientation of the magnetization through a so-called first-order magnetization process. Here, we show that appealing double-hysteresis P-E loops can also appear from an unprecedented first-order polarization process. Focusing on non-polar CaTiO3, which can be turned ferroelectric under tensile strain, we study epitaxial thin films on differently-oriented NdGaO3 substrates using a combination of theoretical and experimental techniques. We uncover that a certain configuration exhibits double-hysteresis P-E loops that we rationalize from a field-induced abrupt rotation of the polarization. Such a first-order polarization process establishes a promising alternative pathway to achieve double hysterisis P-E loops appealing for practical applications.

cond-mat.mtrl-sci↗

arXiv2025

Multimodal Topological Textures Arising from Coupled Structural Orders in SrTiO$_3$

Magnetic spin topological textures recently found their electrical counterparts in polar topologies emerging from the condensation of inhomogeneous polar atomic distortions. Here, we further extend the concept to other non-polar atomic degrees of freedom. Taking SrTiO$_3$ as a prototypical example, we investigate from second-principles atomistic simulations, the equilibrium domain structures and topological textures associated with the natural antiferrodistortive rotations of its oxygen octahedra. % Besides the common 90$^\circ$ antiferrodistortive domain walls (twin boundaries), we identify new metastable 180$^\circ$ domain walls oriented along the $\lbrace100\rbrace_\mathrm{pc}$ direction, when compressive epitaxial strain is applied. These domains exhibit complex antiferrodistortive Bloch- and Néel-like configurations with the later being the most favorable. We also stabilize antiferrodistortive vortex and antivortex structures which are accompanied by co-localized polarization vortices and a complex pattern of the local strain field, giving rise to a trimodal topological structures. Our results extends the concept of topological ordering to non-polar structural degrees of freedom and highlights the role of lattice-mediated couplings in stabilizing complex textures in perovskite oxides.

cond-mat.mtrl-sci↗

arXiv2025

Mechanical coupling of polar topologies and oxygen octahedra rotations in PbTiO$_3$/SrTiO$_3$ superlattices

PbTiO$_3$/SrTiO$_3$ artificial superlattices recently emerged as a prototypical platform for the emergence and study of polar topologies. While previous studies mainly focused on the polar textures inherent to the ferroelectric PbTiO$_3$ layers, the oxygen octahedra rotations inherent to the paraelectric SrTiO$_3$ layers have attracted much little attention. Here, we highlight a biunivocal relationship between distinct polar topologies -- including $a_1/a_2$ domains, polar vortices, and skyrmions -- within the PbTiO$_3$ layers and specific patterns of oxygen octahedra rotations in the SrTiO$_3$ layers. This relationship arises from a strain-mediated coupling between the two materials and is shown to be reciprocal. Through second-principles atomistic simulations, we demonstrate that each polar texture imposes a corresponding rotation pattern, while conversely, a frozen oxygen octahedra rotation dictates the emergence of the associated polar state. This confirms the strong coupling between oxygen octahedra rotations in SrTiO$_3$ and polarization in PbTiO$_3$, highlighting their cooperative role in stabilizing complex polar textures in related superlattices.

cond-mat.mtrl-sci↗

arXiv2025

Role of long-range dipolar interactions in the simulation of the properties of polar crystals using effective atomic potentials

Driven by novel approaches and computational techniques, second-principles atomic potentials are nowadays at the forefront of computational materials science, enabling large-scale simulations of material properties with near-first-principles accuracy. However, their application to polar materials can be challenging, particularly when longitudinal-optical phonon modes are active on the material, as accurately modeling such systems requires incorporating the long-range part of the dipole-dipole interactions. In this study, we challenge the influence of these interactions on the properties of polar materials taking BaTiO$_3$ as paradigmatic example. By comparing models with and without the long-range part of the electrostatic contributions in a systematic way, we demonstrate that even if these interactions are neglected, the models can still provide an overall good description of the material, though they may lead to punctual significant artifacts. Our results propose a pathway to identify when an atomistic potential may be inadequate and needs to be corrected through the inclusion of the long-range part of dipolar interactions.

cond-mat.mtrl-sci↗

arXiv2025

Abinit 2025: New Capabilities for the Predictive Modeling of Solids and Nanomaterials

Abinit is a widely used scientific software package implementing density functional theory and many related functionalities for excited states and response properties. This paper presents the novel features and capabilities, both technical and scientific, which have been implemented over the past 5 years. This evolution occurred in the context of evolving hardware platforms, high-throughput calculation campaigns, and the growing use of machine learning to predict properties based on databases of first principles results. We present new methodologies for ground states with constrained charge, spin or temperature; for density functional perturbation theory extensions to flexoelectricity and polarons; and for excited states in many-body frameworks including GW, dynamical mean field theory, and coupled cluster. Technical advances have extended abinit high-performance execution to graphical processing units and intensive parallelism. Second principles methods build effective models on top of first principles results to scale up in length and time scales. Finally, workflows have been developed in different community frameworks to automate \abinit calculations and enable users to simulate hundreds or thousands of materials in controlled and reproducible conditions.

cond-mat.mtrl-sci↗

arXiv2025

Ferroelectric Properties and Topological Polar Textures of PbTiO$_3$ from a Second-Principles Open-Source Interatomic Potential

We introduce an open-source, fully atomistic second-principles interatomic potential for lead titanate (PbTiO3), a benchmark ferroelectric material known for its strong polarization and hightemperature phase transitions. While density functional theory excels at capturing atomic-scale behavior, it remains computationally prohibitive for large-scale simulations required to explore complex phenomena. Our model addresses this limitation by accurately reproducing key properties of PbTiO3, including domain wall dynamics and different topological textures formation, which are known as key features to next-generation memory and energy-efficient technologies. Validated against DFT data, the model remains predictive across a wide range of conditions. It offers an accessible and efficient framework for high-accuracy large-scale simulations, allowing deeper insights into PbTiO3 and its potential applications.

cond-mat.mtrl-sci↗

arXiv2025

Strain dependence of the Bloch domain component in 180$^\circ$ domains in bulk PbTiO$_{3}$ from first-principles

We investigate the emergence of Bloch-type polarization components in 180$^\circ$ ferroelectric domain walls in bulk PbTiO$_{3}$ under varying mechanical boundary conditions, using first-principles simulations based on density functional theory. A spontaneous Bloch component$-$primarily associated with Pb displacements confined within the PbO domain wall plane$-$condense under realistic strain conditions on top of the Ising-type domain walls. The amplitude and energetic stabilization of this component are highly sensitive to the in-plane lattice parameters. In particular, tensile strains akin to those imposed by DyScO$_{3}$ substrates enhance the Bloch component and lead to energy reductions as large as 10.7 mJ/m$^{2}$ (10.6 meV/$\square$) with respect to the most stable structure including only Ising and Néel components. We identify a relatively flat energy landscape for the Bloch polarization, highlighting the tunability of chiral textures through strain engineering. Our results offer a predictive framework for estimating the strain-dependent onset temperature of Bloch-type domain wall components and provide insight into the design of topologically nontrivial and chiral polar structures in ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2025

Finite-temperature properties and the hidden ferroelectric $R3c$ phase of bulk CaTiO$_3$ from second principles

A second-principles effective interatomic potential is introduced for the prototypical perovskite CaTiO$_3$ (CTO), relying on a Taylor polynomial expansion of the Born-Oppenheimer energy surface around the cubic reference structure, in terms of atomic displacements and macroscopic strains. This model captures various phases of bulk CTO and successfully reproduces, in particular, the structure, energy, and dynamical properties of the nonpolar $Pbnm$ ground state as well as of the hidden ferroelectric $R3c$ phase. Finite-temperature simulations suggest that the still debated sequence of structural phase transitions over heating is $Pbnm \ (a^-a^-c^+) \rightarrow C2/m \ (a^-b^-c^0) \rightarrow I4/mcm \ (a^-c^0c^0) \rightarrow Pm\bar{3}m \ (a^0a^0a^0)$, a sequence during which the oxygen-octahedra rotations around the three pseudocubic axes vanish successively. Although never experimentally observed in bulk, the ferroelectric $R3c$ phase appears to be metastable and at an energy only slightly above the $Pbnm$ ground state at 0 K. The simulations confirm that, if induced in some way, the $R3c$ phase remains stable up to about 300 K and shows ferroelectric properties. Furthermore, we find that the minimum energy path connecting the $Pbnm$ and $R3c$ phases involves localized layer-by-layer flipping of octahedral rotations, a mechanism which is shown to be at play during the thermal destabilization process of the $R3c$ phase toward the $Pbnm$ ground state. The proximity of the $R3c$ phase with the $Pbnm$ ground state suggests that the former could be stabilized under electric field. However, due to the large energy barrier, the field required for the $Pbnm$-to-$R3c$ transition appears to be extremely large, consistent with the fact that bulk CTO was never reported to be ferroelectric nor antiferroelectric.

cond-mat.mtrl-sci↗

arXiv2025

Switchable Skyrmion-Antiskyrmion Tubes in Rhombohedral BaTiO$_\mathrm{3}$ and Related Materials

Skyrmions are stable topological textures that have garnered substantial attention within the ferroelectric community for their exotic functional properties. While previous studies have questioned the feasibility of [001]$_{\text{pc}}$ skyrmion tubes in rhombohedral BaTiO$_3$ due to the high energy cost of 180$^\circ$ domain walls, we demonstrate here their stabilization with topological charges of $\mathcal{Q} = \pm 1$ from density functional theory and second-principles calculations. By enabling extensive vortex and antivortex polarization configurations, the expected prohibitive energetic barriers are overcomed while preserving the topological nature of the structures. Notably, we extend these findings to demonstrate the appearance of skyrmion and antiskyrmion tubes in other related materials, highlighting their broader relevance. Furthermore, our computational experiments indicate that these structures can be directly stabilized and reversibly switched by applied electric fields, establishing a straightforward route for their practical realization and functional control in nanoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2025

Inhomogeneous Electric Fields for Precise Control and Displacement of Polar Textures

Since the discovery of polar topological textures, achieving efficient control and manipulation of them has emerged as a significant challenge for their integration into nanoelectronic devices. In this study, we use second principles molecular dynamic simulations to demonstrate the precise and reversible control of domain arrangements stabilizing diverse polarization textures through the application of various inhomogeneous electric fields. Furthermore, we conduct an in-depth study of ferroelectric domain motion under such fields, revealing features consistent with creep dynamics and establishing an upper limit for their propagation speed. Notably, our findings show that domain walls exhibit an asymmetric inertial response, present at the onset of the dynamics but absent during their cessation. These findings provide valuable insights into the dynamic behavior of polar textures, paving the way for the development of high-speed, low-power nanoelectronic applications.

cond-mat.mtrl-sci↗

arXiv2024

Dynamical manipulation of polar topologies from acoustic phonon pumping

Since the recent discovery of polar topologies, a recurrent question has been in the way to remotely tune them. Many efforts have focused on the pumping of polar optical phonons from optical methods but with limited success, as only switching between specific phases has been achieved so far. Additionally, the correlation between optical pulse characteristics and the resulting phase remains poorly understood. Here, we propose an alternative approach and demonstrate the deterministic and dynamical tailoring of polar topologies using instead acoustic phonon pumping. Our second-principles simulations reveal that by pumping specific longitudinal and transverse acoustic phonons, various topological textures can be induced in materials like BaTiO$_\mathrm{3}$ or PbTiO$_\mathrm{3}$. This method leverages the strong coupling between polarization and strain in these materials, enabling predictable and dynamical control of polar patterns. Our findings open up an alternative possibility for the manipulation of polar textures, inaugurating a promising research direction.

cond-mat.mtrl-sci↗

arXiv2024

Assessing the nature of nanoscale ferroelectric domain walls in lead titanate multilayers

The observation of unexpected polarisation textures such as vortices, skyrmions and merons in various oxide heterostructures has challenged the widely accepted picture of ferroelectric domain walls as being Ising-like. Bloch components in the 180° domain walls of PbTiO3 have recently been reported in PbTiO3/SrTiO3 superlattices and linked to domain wall chirality. While this opens exciting perspectives, the ubiquitous nature of this Bloch component remains to be further explored. In this work, we present a comprehensive investigation of domain walls in PbTiO3/SrTiO3 superlattices, involving a combination of first- and second-principles calculations, phase-field simulations, diffuse scattering calculations, and synchrotron based diffuse x-ray scattering. Our theoretical calculations highlight that the previously predicted Bloch polarisation in the 180° domain walls in PbTiO3/SrTiO3 superlattices might be more sensitive to the boundary conditions than initially thought and is not always expected to appear. Employing diffuse scattering calculations for larger systems we develop a method to probe the complex structure of domain walls in these superlattices via diffuse x-ray scattering measurements. Through this approach, we investigate depolarization-driven ferroelectric polarization rotation at the domain walls. Our experimental findings, consistent with our theoretical predictions for realistic domain periods, do not reveal any signatures of a Bloch component in the centres of the 180° domain walls of PbTiO3/SrTiO3 superlattices, suggesting that the precise nature of domain walls in the ultrathin PbTiO3 layers is more intricate than previously thought and deserves further attention.

cond-mat.mtrl-sci↗

arXiv2024

Finite-temperature properties of antiferroelectric perovskite $\rm PbZrO_3$ from deep learning interatomic potential

The prototypical antiferroelectric perovskite $\rm PbZrO_3$ (PZO) has garnered considerable attentions in recent years due to its significance in technological applications and fundamental research. Many unresolved issues in PZO are associated with large length- and time-scales, as well as finite temperatures, presenting significant challenges for first-principles density functional theory studies. Here, we introduce a deep learning interatomic potential of PZO, enabling investigation of finite-temperature properties through large-scale atomistic simulations. Trained using an elaborately designed dataset, the model successfully reproduces a large number of phases, in particular, the recently discovered 80-atom antiferroelectric $Pnam$ phase and ferrielectric $Ima2$ phase, providing precise predictions for their structural and dynamical properties. Using this model, we investigated phase transitions of multiple phases, including $Pbam$/$Pnam$, $Ima2$ and $R3c$, which show high similarity to the experimental observation. Our simulation results also highlight the crucial role of free-energy in determining the low-temperature phase of PZO, reconciling the apparent contradiction: $Pbam$ is the most commonly observed phase in experiments, while theoretical calculations predict other phases exhibiting even lower energy. Furthermore, in the temperature range where the $Pbam$ phase is thermodynamically stable, typical double polarization hysteresis loops for antiferroelectrics were obtained, along with a detailed elucidation of the structural evolution during the electric-field induced transitions between the non-polar $Pbam$ and polar $R3c$ phases.

cond-mat.mtrl-sci↗