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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{\deg} 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{\deg} 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{\deg} 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.

The metal-hydride-based topochemical reduction process has produced novel thermodynamically unstable phases across various transition metal oxide series with unusual crystal structures and non-trivial ground states. Here, by such an oxygen (de-) intercalation method we synthesis a novel samarium nickelate with ordered nickel valences associated with tri-component coordination configurations. This structure, with a formula of Sm$_{9}$Ni$_{9}$O$_{22}$ as revealed by four-dimensional scanning transmission electron microscopy, emerges from the intricate planes of {303}$_{\text{pc}}$ ordered apical oxygen vacancies. X-ray spectroscopy measurements and ab-initio calculations show the coexistence of square-planar, pyramidal and octahedral Ni sites with mono-, bi- and tri-valences. It leads to an intense orbital polarization, charge-ordering, and a ground state with a strong electron localization marked by the disappearance of ligand-hole configuration at low-temperature. This new nickelate compound provides another example of previously inaccessible materials enabled by topotactic transformations and presents a unique platform where mixed Ni valence can give rise to exotic phenomena.

We investigate nanoscale domain engineering via epitaxial coupling in a set of SrRuO$_3$/PbTiO$_3$/SrRuO$_3$ heterostructures epitaxially grown on (110)$_o$-oriented DyScO$_3$ substrates. The SrRuO$_3$ layer thickness is kept at 55 unit cells, whereas the PbTiO$_3$ layer is grown to thicknesses of 23, 45 and 90 unit cells. Through a combination of atomic force microscopy, x-ray diffraction and high resolution scanning transmission electron microscopy studies, we find that above a certain critical thickness of the ferroelectric layer, the large structural distortions associated with the ferroelastic domains propagate through the top SrRuO$_3$ layer, locally modifying the orientation of the orthorhombic SrRuO$_3$ and creating a modulated structure that extends beyond the ferroelectric layer boundaries., Comment: 19 pages, 6 figures, supplementary materials. arXiv admin note: text overlap with arXiv:2304.06948

Most perovskite oxides belong to the Pbnm space group, composed by an anisotropic unit cell, A-site antipolar displacements and oxygen octahedral tilts. Mapping the orientation of the orthorhombic unit cell in epitaxial heterostructures that consist of at least one Pbnm compound is often required to understand and control the different degrees of coupling established at their coherent interfaces and, therefore, their resulting physical properties. However, retrieving this information from the strain maps generated with high-resolution scanning transmission electron microscopy can be challenging, because the three pseudocubic lattice parameters are very similar in these systems. Here, we present a novel methodology for mapping the crystallographic orientation in Pbnm systems. It makes use of the geometrical phase analysis algorithm, as applied to aberration-corrected scanning transition electron microscopy images, but in an unconventional way. The method is fast and robust, giving real-space maps of the lattice orientations in Pbnm systems, from both cross-sectional and plan-view geometries and across large fields of view. As an example, we apply our methodology to rare-earth nickelate heterostructures, in order to investigate how the crystallographic orientation of these films depends on various structural constraints that are imposed by the underlying single crystal substrates. We observe that the resulting domain distributions and associated defect landscapes mainly depend on a competition between the epitaxial compressive/tensile and shear strains, together with the matching of atomic displacements at the substrate/film interface. The results point towards strategies for controlling these characteristics by appropriate substrate choice., Comment: 32 pages, 5 figures, 2 tables

We study the complex ferroelastic/ferroelectric domain structure in the prototypical ferroelectric PbTiO3 epitaxially strained on (110)o-oriented DyScO3 substrates, using a combination of atomic force microscopy, laboratory and synchrotron x-ray diffraction and high resolution scanning transmission electron microscopy. We observe that the anisotropic strain imposed by the orthorhombic substrate creates a large asymmetry in the domain configuration, with domain walls macroscopically aligned along one of the two in-plane directions. We show that the periodicity as a function of film thickness deviates from the Kittel law. As the ferroelectric film thickness increases, we find that the domain configuration evolves from flux-closure to a/c-phase, with a larger scale arrangement of domains into superdomains., Comment: v2: figure 5 corrected 18 pages, 5 figures + supplementary materials (2 pages, 2 figures)

The discovery of superconductivity in Nd$_{0.8}$Sr$_{0.2}$NiO$_2$ [1] introduced a new family of layered nickelate superconductors that has now been extended to include a range of Sr-doping [2, 3], Pr or La in place of Nd [4-6], and the 5-layer Nd$_6$Ni$_5$O$_{12}$ [7]. A number of studies indicate that electron correlations are strong in these materials [8-14], and hence a central question is whether or not magnetism is present as a consequence of these interactions. Here we report muon spin rotation/relaxation studies of a series of superconducting infinite-layer nickelates. In all cases we observe an intrinsic magnetic ground state, regardless of the rare earth ion or doping, arising from local moments on the nickel sublattice. The coexistence of magnetism - which is likely to be antiferromagnetic and short-range ordered - with superconductivity is reminiscent of some iron pnictides [15] and heavy fermion compounds [16], and qualitatively distinct from the doped cuprates [17].

Ferroelectric domains in PbTiO$_3$/SrTiO$_3$ superlattices were studied using synchrotron X-ray diffraction. Macroscopic measurements revealed a change in the domain wall orientation from $\left\lbrace 100 \right\rbrace $ to $\left\lbrace 110 \right\rbrace $ crystallographic planes with increasing temperature. The temperature range of this reorientation depends on the ferroelectric layer thickness and domain period. Using a nanofocused beam, local changes in domain wall orientation within the buried ferroelectric layers were imaged, both in structurally uniform regions of the sample and near defect sites and argon ion etched patterns. Domain walls were found to exhibit preferential alignment with the straight edges of the etched patterns as well as with structural features associated with defect sites. The distribution of out-of-plane lattice parameters was mapped around one such feature, showing that it is accompanied by inhomogeneous strain and large strain gradients.

Nucleation processes of mixed-phase states are an intrinsic characteristic of first-order phase transitions, typically related to local symmetry breaking. Direct observation of emerging mixed-phase regions in materials showing a first-order metal-insulator transition (MIT) offers unique opportunities to uncover their driving mechanism. Using photoemission electron microscopy, we image the nanoscale formation and growth of insulating domains across the temperature-driven MIT in NdNiO3 epitaxial thin films. Heteroepitaxy is found to strongly determine the nanoscale nature of the phase transition, inducing preferential formation of striped domains along the terraces of atomically flat stepped surfaces. We show that the distribution of transition temperatures is an intrinsic local property, set by surface morphology and stable across multiple temperature cycles. Our data provides new insights into the MIT of heteroepitaxial nickelates and points to a rich, nanoscale phenomenology in this strongly correlated material.