arXiv subjects

Philippe Ghosez

Publications and source records attributed to Philippe Ghosez.

At least 19 recordsLinked to original sources

arXiv2026

The polar discontinuity picture in nickelate superlattices: comparison of the insulating and metallic phases

We present a first-principles study of the formal-charge polar discontinuity in superlattices of BaTiO$_3$ interfaced with SmNiO$_3$ or BiNiO$_3$, comparing the results for the insulating and metallic nickelate phases. Polar discontinuities arising from differently charged layers in perovskites are well-studied in heterostructures such as LaAlO$_3$/SrTiO$_3$, and recently, signatures consistent with such a polar discontinuity have been observed in systems where the formally charged layers would reside in a metal. We first identify signatures of the polar discontinuity in the structure and the density of states of superlattices with BaTiO$_3$ and insulating BiNiO$_3$, and find partial screening by modification of the BiNiO$_3$ charge disproportionation pattern analogous to our previous study on BaTiO$_3$/SmNiO$_3$. We then examine superlattices constructed from the corresponding metallic nickelate phases and find that, despite the presence of screening charges, the qualitative interfacial response is remarkably similar to that of the insulating counterparts. We show that the metallic screening charges have little influence on the apparent formal-charge polar discontinuity and discuss practical limitations of the polar-discontinuity picture when interpreting and quantifying screening at metallic nickelate/ferroelectric interfaces.

cond-mat.mtrl-sci↗

arXiv2026

First-order polarization process as an alternative to antiferroelectricity

Antiferroelectrics generate significant interest since their polarization versus electric field (P-E) 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 hysteresis P-E loops appealing for practical applications.

cond-mat.mtrl-sci↗

arXiv2026

Uniaxial strain tuning of functional properties in antiferroelectric PbZrO3 membrane capacitors

Lead zirconate (PbZrO3, PZO) is a prototypical antiferroelectric (AFE) system promising for applications such as energy storage and neuromorphic computing. However, in conventional thin-film architectures, its functional potential is often limited by substrate clamping. Although emerging freestanding membrane techniques offer an approach to release this clamping and enable dynamic strain engineering, a systematic understanding of how external strain modulates the switching between AFE and ferroelectric (FE) states is missing. In this study, we investigate the uniaxial strain effects on PZO membrane capacitors transferred onto flexible substrates via a gold-bonding method. We demonstrate that in-plane dynamic strain modulates the AFE-FE switching and functional properties. Corroborated by atomistic simulations, we reveal that the strain-dependent evolution arises from the superposition of the intrinsic strain dependence of specific domain orientation variants and extrinsic strain-induced redistribution of the relative population of different domain variants. These findings provide a predictive understanding of uniaxial strain tuning of AFE-FE switching in PZO, and pave the way for exploiting the functional potential of freestanding antiferroelectric membranes.

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arXiv2026

Domain-wall-to-domain interconversion in a polar conducting oxide

Domain walls in ferroic crystals are topological defects with a symmetry distinct from the domain interior, allowing them to display functionalities that are otherwise forbidden in the host material. Despite their unique properties, domain walls are strictly confined to two-dimensional interfaces, which hinders unveiling their true nature and limits their applicability. Here, we demonstrate reversible dimensionality control by expanding nanoscale domain walls into three-dimensional functional regions in polar epitaxial tungsten trioxide ($\text{WO}_3$). This domain-wall-to-domain interconversion is enabled by the conducting, non-polar domain walls adopting the parent-phase structure. An alternating electric field applied through a scanning probe tip induces localized heating, which expands this domain-wall phase into the adjacent polar domains. This approach enables reversible spatial control to switch between mutually exclusive properties of domains (polarity) and domain walls (conductivity), offering a new paradigm for reconfigurable oxide electronics.

cond-mat.mtrl-sci↗

arXiv2026

Polar discontinuity screening by charge disproportionation in ferroelectric-nickelate superlattices

We use density functional theory (DFT) to demonstrate rearrangement of charge disproportionation as a new mechanism for screening polar discontinuities at heterointerfaces. We focus on SmNiO$_3$, a III-III perovskite characterized by an insulating ground state that originates from disproportionation of the electrons at the Ni sites. When interfaced with ferroelectric, II-IV perovskite BaTiO$_3$, this system can display a polar discontinuity whose magnitude is determined by the nature of the interface (NiO$_2$-BaO or SmO-TiO$_2$) and the orientation of the BaTiO$_3$ spontaneous polarization. In the orientation maximizing the interface charge, SmNiO$_3$ compensates by transferring 1 $e$/f.u. between the two interfaces and modifying the disproportionation sequence from Ni$^{4+}$/Ni$^{2+}$ to Ni$^{2+}$/Ni$^{2+}$ at the SmO-TiO$_2$ interface and to Ni$^{4+}$/Ni$^{4+}$ at the NiO$_2$-BaO interface. While this mechanism is potentially universal in all perovskites exhibiting charge disproportionation, our formal analysis of BiNiO$_3$/BaTiO$_3$ superlattices suggests that larger polar discontinuities may need more complex disproportionation patterns for screening.

cond-mat.mtrl-sci↗

arXiv2026

The hidden ferroelectric chiral ground state of silver niobate

Silver niobate is a conventional perovskite oxide compound, known to exhibit a rich polymorphism. Although often classified as antiferroelectric, its low-temperature structure remains unclear. Here, first-principles calculations reveal a previously overlooked and unusual rhombohedral ferroelectric phase with $R3$ symmetry that emerges as the thermodynamic ground state despite its almost degenerate energy and close energetic competition with previously proposed structures. Remarkably, this phase is structurally chiral, with chirality emerging improperly from the coupling between polarization and in-phase rotations of the oxygen octahedra along [111], producing a ferri-chiral state with incomplete cancellation of local chiral motifs. As a consequence, the phase exhibits significant natural optical activity comparable to that of quartz. Although energetically favored, its experimental observation may be hindered by kinetic limitations, potentially contributing to the ongoing controversy surrounding the low-temperature structure of silver niobate.

cond-mat.mtrl-sci↗

arXiv2026

Tilt-driven ferrielectricity in PbZrO$_3$

We reveal a tilt-driven mechanism for ferrielectricity in prototypical antiferroelectric PbZrO$_3$. Specifically, introducing an additional octahedral tilt into the antiferroelectric $Pbam$ phase breaks the symmetry constraint that enforces equal antiparallel dipoles, converting the compensated ``$\uparrow \uparrow \downarrow \downarrow$'' nonpolar configuration into an uncompensated ``$\uparrow \uparrow \downarrow \downarrow$'' polar $Pmc2_1$ phase. First-principles calculations show that the $Pmc2_1$ phase becomes stabilized under lattice contraction and gains increasing free-energy advantage over competing phases at finite temperatures. Atomic-scale imaging directly confirms the presence of $Pmc2_1$-like structures in thin films and single crystals. This work identifies a symmetry-governed, kinetically easily accessible pathway to ferrielectricity and establishes a form of ``competitive'' improper ferroelectricity, with broad implications for antiferroelectrics.

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arXiv2026

Silicon-compatible ideal antiferroelectricity with large digital electromechanical responses enabled by thermal-strain domain engineering

Antiferroelectrics exhibit reversible antipolar-polar transformations, offering a compelling platform for multiple functionalities in modern nanoelectronics, yet deterministic control of antiferroelectric domains and switching pathways remain elusive. Moreover, their integration with ubiquitous silicon-based electronic devices has been limited by the structural and chemical incompatibilities of conventional oxide platforms. Here, we convert the conventional drawback of thermal mismatch into a functional advantage and realize ideal antiferroelectricity in epitaxial PbZrO3 thin films on silicon through thermal tensile-strain engineering, a strain regime unattainable on conventional perovskite substrates. Combined theoretical and experimental studies show that tensile strain stabilizes the (004)o domain, enabling a direct one-step switching, whereas compressive-strain-stabilized (240)o domains switch through intermediate ferrielectric states. The resulting films exhibit near-zero remanent polarization, square double hysteresis, nanosecond switching (~75ns), large reversible electrostrain (~0.6%) and robust operation windows. These findings provide key insights into domain-engineered ideal antiferroelectricity on silicon, opening a viable route toward high-performance antiferroelectric nano-electronic devices.

cond-mat.mtrl-sci↗

arXiv2026

Unlocking Static Polarization and Strain Density Waves in Perovskites by Softening a Hidden Antiferrodistortive Tilt Gradient Mode

Spin density waves (SDWs) represent a fundamental paradigm of spatially modulated order in condensed matter systems, yet their electrical and mechanical analogues polarization and strain density waves (PDWs and StDWs) have remained elusive as equilibrium phases. Here, we introduce a general, symmetry-driven strategy to unlock static PDWs and StDWs in perovskites SrTiO3 and SrMnO3. Using first-principles calculations, we uncover a previously overlooked soft antiferrodistortive tilt gradient mode at small-q wavevector in the phonon dispersion of their presumed Ima2 ground state under moderate tensile strain. Group-theory analysis reveals that a hard polaracoustic phonon, which intrinsically carries PDWs and StDWs, is improperly destabilized by a trilinear coupling with this modulated tilt mode and an inherently uniform tilt mode. This interaction drives a structural transition from the Ima2 phase to a novel lower-energy Pmn21 phase that hosts long-range-ordered PDWs and StDWs. Strikingly, the engineered StDWs in SrMnO3 activate an electrically tunable SDW via the flexomagnetic effect. These discoveries fundamentally revise the strain-phase diagrams of prototypical perovskites and establish a unified phonon-engineering framework that links modulated phonon instabilities to targeted density-wave order, offering new pathways for designing advanced electromechanical and magnetoelectric functionalities.

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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

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

Rational Control of Magnonic and Electronic Band Splittings

We provide a theoretical demonstration of controllable non-relativistic spin splitting in both electronic and magnonic bands via targeted structural distortions tied to specific phonon modes. Using MnF$_2$ as a model system, we identify a $d$-wave magnon band splitting between magnon modes of specific handedness, directly correlated with the non-relativistic spin splitting observed in the electronic structure. Crucially, we show that structural distortions associated with the A$_{2u}$ and A$_{1g}$ phonon modes (8.52 and 9.74 THz) modulate these splittings without altering the antiferromagnetic order. The effect originates from changes in the nonmagnetic ligand environment, highlighting the key role of lattice degrees of freedom in governing spin dynamics. Our findings establish a novel route for structure-mediated control of spin splitting, opening possibilities for tunable magnonic and spintronic functionalities in antiferromagnetic materials.

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

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.

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