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Fernando Gómez-Ortiz

Publications and source records attributed to Fernando Gómez-Ortiz.

At least 19 recordsLinked to original sources

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↗

Emergence of millimeter-wave resonances in self-assembled ferroelectric metamaterials

Resonators are a key component in modern communications and computing. As demand and technological advances push component requirements into the terahertz regime, there is significant research devoted to the search for resonances at these frequencies. While uniform solid-state materials usually do not intrinsically feature resonances in this frequency range, self-assembled periodic arrays of ferroelectric nanodomains may provide an engineering route to design millimeter-wave properties. Here, we utilize prototypical dielectric-ferroelectric SrTiO3/PbTiO3 superlattices to robustly design periodic ferroelectric nano-scale domains. Phase field simulations predict an emergent domain breathing mode in complex polar textures and state-of-the-art millimeter-wave characterization shows evidence for such emergent resonances up to hundreds of GHz. Complex polar textures in these superlattices lead to emergent piezoelectric properties that also result in millimeter-wave resonances, which are predicted by second principles methods and confirmed by direct measurement. The principles investigated in this work suggest a new modality for ferroelectrics in the design of millimeter-wave electronics.

cond-mat.mtrl-sci↗

Implementation of the hybrid exchange-correlation functionals in the SIESTA code

We present an efficient and accurate implementation of hybrid exchange-correlation (XC) functionals in the SIESTA code, enabling large-scale simulations based on Hartree-Fock-type exact exchange combined with strictly localized numerical atomic orbitals (NAOs). Our approach exploits a fitted representation of the NAOs in terms of Gaussian-type orbitals (GTOs), which allows for the analytical evaluation of four-center electron repulsion integrals (ERIs) via the LIBINT library. This framework is seamlessly integrated with SIESTA's real-space grid and sparse-matrix infrastructure, and is combined with multiple screening techniques to control the computational complexity. We also introduce a fully analytical formulation of hybrid-functional forces and a dynamic parallel distribution scheme that ensures excellent scalability. We validate our implementation through benchmark calculations on a broad set of systems (including semiconductors, insulators, and two-dimensional materials) and demonstrate that the HSE06 functional significantly improves the prediction of band gaps compared to PBE, in close agreement with G0W0 and experimental data. We analyze in detail the trade-offs between accuracy and computational efficiency as a function of the number of Gaussians, basis set range, and integral screening thresholds. Our results confirm that hybrid functional calculations in SIESTA are now feasible for large extended systems, making accurate first-principles predictions of electronic and structural properties accessible at scale.

cond-mat.mtrl-sci↗

Structural chirality measurements and computation of handedness in periodic solids

We compare the various chirality measures most widely used in the literature to quantify chiral symmetry in extended solids, i.e., the continuous chirality measure, the Hausdorff distance, and the angular momentum. By studying these functions in an algebraically tractable case, we can evaluate their strengths and weaknesses when applied to more complex crystals. Going beyond those classical calculations, we propose a new method to quantify the handedness of a crystal based on a pseudoscalar function, i.e., the helicity. This quantity, borrowed from hydrodynamics, can be computed from the eigenvector carrying the system from the high-symmetry non-chiral phase to the low-symmetry chiral phase. Different model systems like K$_3$NiO$_2$, CsCuCl$_3$ and MgTi$_2$O$_4$ are used as test cases where we show the superior interest of using helicity to quantify chirality together with the handedness distinction.

cond-mat.mtrl-sci↗

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↗

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↗

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↗

Pathways to crystal chirality An algorithm to identify new displacive chiral phase transitions

We present an algorithm that integrates pseudosymmetry search with first-principles calculations to systematically identify achiral parent structures and establish potential chiral displacive transitions linking them to their corresponding chiral phases within the 22 enantiomorphic space groups. This approach enables a robust exploration of structural relationships, offering new insights into symmetry-driven properties. Our workflow streamlines the discovery of displacive chiral phase transitions driven by soft phonon modes, providing insights into the mechanisms of structural chirality in inorganic materials. We apply this methodology on the chiral phases of TeO$_2$, Na$_2$SeO$_9$, Sr$_2$As$_2$O$_7$, As$_2$O$_5$, Rb$_2$Be$_2$O$_3$, and CaTe$_2$O$_3$. Demonstrating that some do not have a minimal supergroup that allows for an achiral phase; some can have a minimal supergroup, still, no unstable phonon mode exists in the achiral phase; and somewhere the minimal supergroup exists with a soft phonon mode connecting the identified achiral phase and the chiral phase through small continuous displacements.

cond-mat.mtrl-sci↗

Emergence of Transverse Dielectric Response in Ferroelectric Dielectric Heterostructures

We report the emergence of a transverse dielectric response in PbTiO$_{3}$/SrTiO$_{3}$ superlattices hosting polar vortex structures. Using second-principles simulations, we find that an electric field applied along one direction induces significant local polarization responses along orthogonal directions, with magnitudes approaching half that of the diagonal susceptibility components. These off-diagonal responses are strongly dependent on the topology of the vortex structure and can be deterministically tuned or even reversed via homogeneous electric fields or epitaxial strain. Notably, the transverse susceptibilities become comparable to the diagonal components during a field- or strain-induced transition to a polarization wave state. This discovery opens avenues for engineering reconfigurable nanoscale dielectric responses in topologically textured ferroelectric systems.

cond-mat.mtrl-sci↗

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↗

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↗

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↗

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↗

Structural chirality and related properties in the periodic inorganic solids: Review and perspectives

Chirality refers to the asymmetry of objects that cannot be superimposed on their mirror image. It is a concept that exists in various scientific fields and has profound consequences. Although these are perhaps most widely recognized within biology, chemistry, and pharmacology, recent advances in chiral phonons, topological systems, crystal enantiomorphic materials, and magneto-chiral materials have brought this topic to the forefront of condensed matter physics research. Our review discusses the symmetry requirements and the features associated with structural chirality in inorganic materials. This allows us to explore the nature of phase transitions in these systems, the coupling between order parameters, and their impact on the material's physical properties. We highlight essential contributions to the field, particularly recent progress in the study of chiral phonons, altermagnetism, magnetochirality between others. Despite the rarity of naturally occurring inorganic chiral crystals, this review also highlights a significant knowledge gap, presenting challenges and opportunities for structural chirality mostly at the fundamental level, e.g., chiral displacive phase transitions and ferrochirality, possibilities of tuning and switching structural chirality by external means (electric, magnetic, or strain fields), whether chirality could be an independent order parameter, and whether structural chirality could be quantified, etc. Beyond simply summarising this field of research, this review aims to inspire further research in materials science by addressing future challenges, encouraging the exploration of chirality beyond traditional boundaries, and seeking the development of innovative materials with superior or new properties.

cond-mat.mtrl-sci↗

Liquid-crystal-like dynamic transition in ferroelectric/dielectric superlattices

Nanostructured ferroelectrics display exotic multidomain configurations resulting from the electrostatic and elastic boundary conditions they are subject to. While the ferroelectric domains appear frozen in experimental images, atomistic second-principles studies suggest that they may become spontaneously mobile upon heating, with the polar order {\sl melting} in a liquid-like fashion. Here we run molecular dynamics simulations of model systems (PbTiO$_3$/SrTiO$_3$ superlattices) to study the unique features of this transformation. Most notably, we find that the multidomain state looses its translational and orientational orders at different temperatures, resembling the behavior of liquid crystals and yielding an intermediate hexatic-like phase. Our simulations reveal the mechanism responsible for the melting and allow us to characterize the stochastic dynamics in the hexatic-like phase: we find evidence that it is thermally activated, with domain reorientation rates that grow from tens of gigahertzs to terahertzs in a narrow temperature window.

cond-mat.mtrl-sci↗

Kittel law and domain formation mechanism in PbTiO$_3$/SrTiO$_3$ superlattices

We report second-principles simulations on the structural and energetic properties of domains in (PbTiO$_{3}$)$_{n}$/(SrTiO$_{3}$)$_{n}$ superlattices. For the explored layer thickness ($n$ ranging between 8 and 16 unit cells) and lateral sizes of the domains, the most stable configuration corresponds to polar domains separated by a sequence of counter-rotating vortices (clockwise/counterclockwise) perpendicular to the stacking direction and acting as domain walls. The balance between the domain wall energy and the electrostatic energy yields to an optimal domain period $ω$ that is proportional to the square-root of the thickness of the PbTiO$_{3}$ layer, following the Kittel law. For a given lateral size of the simulation box, suboptimal domain structures (with a width larger than the one predicted by the Kittel law) can be obtained in a metastable form. However, at finite temperature, molecular dynamics simulations show the spontaneous change of periodicity, which implies the formation of new domains whose generation is initiated by the nucleation of vortices and antivortices at the interface between the SrTiO$_{3}$ and the PbTiO$_{3}$ layers. The vortices progressively elongate and eventually annihilate with the antivortices yielding the formation of new domains to comply the Kittel law via a topological phase transition.

cond-mat.mtrl-sci↗

Emergent chirality in a polar meron to skyrmion phase transition

Polar skyrmions are predicted to emerge from the interplay of elastic, electrostatic and gradient energies, in contrast to the key role of the anti-symmetric Dzyalozhinskii-Moriya interaction in magnetic skyrmions. With the discovery of topologically-stable polar skyrmions, it is of both fundamental and practical interest to understand the microscopic nature and the possibility of temperature- and strain-driven phase transitions in ensembles of such polar skyrmions. Here, we explore the reversible transition from a skyrmion state (topological charge of -1) to a two-dimensional, tetratic lattice of merons (with topological charge of -1/2) upon varying the temperature and elastic boundary conditions in [(PbTiO3)16/(SrTiO3)16]8 lifted-off membranes. This topological phase transition is accompanied by a change in chirality, from zero-net chirality (in meronic phase) to net-handedness (in skyrmionic phase). To map these changes microscopically required developing new imaging methods. We show how scanning convergent beam electron diffraction provides a robust measure of the local polarization simultaneously with the strain state at sub-nm resolution, while also directly mapping the chirality of each skyrmion. Using this, we demonstrate strain as a crucial order parameter to drive isotropic-to-anisotropic structural transitions of chiral polar skyrmions to non-chiral merons, validated with X-ray reciprocal space mapping and theoretical phase-field simulations. These results revealed by our new measurement methods provide the first illustration of systematic control of rich variety of topological dipole textures by altering the mechanical boundary conditions, which may offer a promising way to control their functionalities in ferroelectric nanodevices using the local and spatial distribution of chirality and order.

cond-mat.mes-hall↗

Berezinskii-Kosterlitz-Thouless phases in ultra-thin PbTiO$_3$/SrTiO$_3$ superlattices

We study the emergence of Berezinskii-Kosterlitz-Thouless (BKT) phases in (PbTiO$_3$)$_3$/(SrTiO$_3$)$_3$ superlattices by means of second-principles simulations. Beyond a threshold tensile epitaxial strain of $ε= 0.25 \%$ the local dipole moments within the superlattices are confined to the film-plane, and thus the polarization can be effectively considered as two-dimensional. The analysis of the decay of the dipole-dipole correlation with the distance, together with the study of the density of defects and its distribution as function of temperature, supports the existence of a BKT phase in a range of temperature mediating the ordered ferroelectric (stable at low $T$), and the disordered paraelectric phase that appears beyond a critical temperature $T_{\rm BKT}$. This BKT phase is characterized by quasi-long-range order (whose signature is a power-law decay of the correlations with the distance), and the emergence of tightly bounded vortex-antivortex pairs whose density is determined by a thermal activation process. The proposed PbTiO$_{3}$/SrTiO$_{3}$ superlattice model and the imposed mechanical boundary conditions are both experimentally feasible, opening the door for the first experimental observation of these new topological phases in ferroelectric materials.

cond-mat.mtrl-sci↗