Motion and teleportation of polar bubbles in low-dimensional ferroelectrics.

Electric bubbles are sub-10nm spherical vortices of electric dipoles that can spontaneously form in ultra-thin ferroelectrics. While the static properties of electric bubbles are well established, little to nothing is known about the dynamics of these particle-like structures. Here, we reveal pathways to realizing both the spontaneous and controlled dynamics of electric bubbles in ultra-thin Pb(Zr0.4Ti0.6)O3 films. In low screening conditions, we find that electric bubbles exhibit thermally-driven chaotic motion giving rise to a liquid-like state. In the high screening regime, we show that bubbles remain static but can be continuously displaced by a local electric field. Additionally, we predict and experimentally demonstrate the possibility of bubble teleportation - a process wherein a bubble is transferred to a new location via a single electric field pulse of a PFM tip. Finally, we attribute the discovered phenomena to the hierarchical structure of the energy landscape.

Topology and control of self-assembled domain patterns in low-dimensional ferroelectrics.

Whilst often discussed as non-trivial phases of low-dimensional ferroelectrics, modulated polar phases such as the dipolar maze and the nano-bubble state have been appraised as essentially distinct. Here we emphasize their topological nature and show that these self-patterned polar states, but also additional mesophases such as the disconnected labyrinthine phase and the mixed bimeron-skyrmion phase, can be fathomed in their plurality through the unifying canvas of phase separation kinetics. Under compressive strain, varying the control parameter, i.e., the external electric field, conditions the nonequilibrium self-assembly of domains, and bridges nucleation and spinodal decomposition via the sequential onset of topological transitions. The evolutive topology of these polar textures is driven by the (re)combination of the elementary topological defects, merons and antimerons, into a plethora of composite topological defects such as the fourfold junctions, the bimeron and the target skyrmion. Moreover, we demonstrate that these manipulable defects are stable at room temperature and feature enhanced functionalities, appealing for devising future topological-based nanoelectronics.

Inverse transition of labyrinthine domain patterns in ferroelectric thin films.

Phase separation is a cooperative process, the kinetics of which underpin the orderly morphogenesis of domain patterns on mesoscopic scales1,2. Systems of highly degenerate frozen states may exhibit the rare and counterintuitive inverse-symmetry-breaking phenomenon3. Proposed a century ago4, inverse transitions have been found experimentally in disparate materials, ranging from polymeric and colloidal compounds to high-transition-temperature superconductors, proteins, ultrathin magnetic films, liquid crystals and metallic alloys5,6, with the notable exception of ferroelectric oxides, despite extensive theoretical and experimental work on the latter. Here we show that following a subcritical quench, the non-equilibrium self-assembly of ferroelectric domains in ultrathin films of Pb(Zr0.4Ti0.6)O3 results in a maze, or labyrinthine pattern, featuring meandering stripe domains. Furthermore, upon increasing the temperature, this highly degenerate labyrinthine phase undergoes an inverse transition whereby it transforms into the less-symmetric parallel-stripe domain structure, before the onset of paraelectricity at higher temperatures. We find that this phase sequence can be ascribed to an enhanced entropic contribution of domain walls, and that domain straightening and coarsening is predominantly driven by the relaxation and diffusion of topological defects. Computational modelling and experimental observation of the inverse dipolar transition in BiFeO3 suggest the universality of the phenomenon in ferroelectric oxides. The multitude of self-patterned states and the various topological defects that they embody may be used beyond current domain and domain-wall-based7 technologies by enabling fundamentally new design principles and topologically enhanced functionalities within ferroelectric films.

Emergent Berezinskii-Kosterlitz-Thouless Phase in Low-Dimensional Ferroelectrics.

Using first-principles-based simulations merging an effective Hamiltonian scheme with scaling, symmetry, and topological arguments, we find that an overlooked Berezinskii-Kosterlitz-Thouless (BKT) phase sustained by quasicontinuous symmetry emerges between the ferroelectric phase and the paraelectric one of BaTiO_{3} ultrathin film, being under tensile strain. Not only do these results provide an extension of BKT physics to the field of ferroelectrics, but they also unveil their nontrivial critical behavior in low dimensions.

Fluctuations and Topological Defects in Proper Ferroelectric Crystals.

Homotopy theory and first-principles-based effective Hamiltonian simulations are combined to investigate the stability of topological defects in proper ferroelectric crystals. We show that, despite a nearly trivial topology of the order parameter space, these materials can exhibit stable topological point defects in their tetragonal polar phase and stable topological line defects in their orthorhombic polar phase. The stability of such defects originates from a novel mechanism of topological protection related to finite-temperature fluctuations of local dipoles.

Topological Point Defects in Relaxor Ferroelectrics.

First-principles-based effective Hamiltonian simulations are used to reveal the hidden connection between topological defects (hedgehogs and antihedgehogs) and relaxor behavior. Such defects are discovered to predominantly lie at the border of polar nanoregions in both Ba(Zr_{0.5}Ti_{0.5})O_{3} (BZT) and Pb(Sc_{0.5}Nb_{0.5})O_{3} (PSN) systems, and the temperature dependency of their density allows us to distinguish between noncanonical (PSN) and canonical (BZT) relaxor behaviors (via the presence or absence of a crossing of a percolation threshold). This density also possesses an inflection point at precisely the temperature for which the dielectric response peaks. Moreover, hedgehogs and antihedgehogs are found to be mobile excitations, and the dynamical nature of their annihilation is demonstrated (using simple hydrodynamical arguments) to follows laws, such as those of Vogel-Fulcher and Arrhenius, that are characteristic of dipolar relaxation kinetics of relaxor ferroelectrics.

Frustration and Self-Ordering of Topological Defects in Ferroelectrics.

A first-principles-based effective Hamiltonian technique is used to investigate the interplay between geometrical frustration and the ordering of topological defects in a ferroelectric nanocomposite consisting of a square array of BaTiO_{3} nanowires embedded in a Ba_{0.15}Sr_{0.85}TiO_{3} matrix. Different arrangements of the wires' chiralities geometrically frustrate the matrix, which in response exhibits point topological defects featuring self-assembled ordered structures spatially fluctuating down to the lowest temperatures. These fluctuations thereby endow the system with residual configurational entropy from which many properties characteristic of geometric frustration, such as the ground state degeneracy and the broadness of the dielectric response, are further found to originate.

Discovery of stable skyrmionic state in ferroelectric nanocomposites.

Non-coplanar swirling field textures, or skyrmions, are now widely recognized as objects of both fundamental interest and technological relevance. So far, skyrmions were amply investigated in magnets, where due to the presence of chiral interactions, these topological objects were found to be intrinsically stabilized. Ferroelectrics on the other hand, lacking such chiral interactions, were somewhat left aside in this quest. Here we demonstrate, via the use of a first-principles-based framework, that skyrmionic configuration of polarization can be extrinsically stabilized in ferroelectric nanocomposites. The interplay between the considered confined geometry and the dipolar interaction underlying the ferroelectric phase instability induces skyrmionic configurations. The topological structure of the obtained electrical skyrmion can be mapped onto the topology of domain-wall junctions. Furthermore, the stabilized electrical skyrmion can be as small as a few nanometers, thus revealing prospective skyrmion-based applications of ferroelectric nanocomposites.

An experimental UHV AFM-STM device for characterizing surface nanostructures under stress/strain at variable temperature.

A compression setup fully integrated in an ultra high vacuum chamber is presented. The system has been designed to combine in situ mechanical test together with near field microscopy at variable temperature, from 90 to 600 K. Compressive stress can be applied on the samples up to 500 MPa at different strain rates ranging from 10(-6) s(-1) to 10(-2) s(-1). The setup performances are highlighted through investigations on Au and Ni3(Al,Ta) single crystals. In particular, it is demonstrated that the high mechanical stability of the original apparatus allows us to follow in situ the evolution of the same area of interest over a large range of temperature and to keep the high spatial resolution offered by near field microscopy, even at high strain levels.

Spin-wave-assisted thermal reversal of epitaxial perpendicular magnetic nanodots.

The magnetic susceptibility of self-organized two-dimensional Co nanodots on Au(111) has been measured as a function of their size in the 2-7 nm diameter range. We show that the activation energy for the thermal reversal displays a power law behavior with the dot volume. Atomic scale simulations based on the Heisenberg Hamiltonian show that this behavior is due to a deviation from the macrospin model for dot size as small as 3 nm in diameter. This discrepancy is attributed to finite temperature effects through the thermal excitation of spin-wave modes inside the particles.

Dominant role of the epitaxial strain in the magnetism of core-shell Co/Au self-organized nanodots.

Self-organized Co nanodots on a Au(111) surface have been surrounded by controlled Au rings that progressively cap the entire dots. The magnetic susceptibility of these dots has been measured in situ as a function of the Au coverage. The blocking temperature increases when the Co bilayer dots are surrounded by the first Au atomic layer and decreases with the subsequent capping. This result cannot be explained by interfacial anisotropy which is generally assumed to be the dominant term in the magnetic anisotropy of nanostructures. Using molecular dynamics simulations, we evidence that the large strain inside the Co clusters is the main driving force for the anisotropy changes during the Au encapsulation.