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The metal-hydride-based “topochemical reduction” process has produced several thermodynamically unstable phases across various transition metal oxide series with unusual crystal structures and nontrivial ground states. Here, by such an oxygen (de-)intercalation method we synthesis a samarium nickelate with ordered nickel valences associated with tri-component coordination configurations. This structure, with a formula of Sm9Ni9O22as revealed by four-dimensional scanning transmission electron microscopy (4D-STEM), emerges from the intricate planes of {303}pcordered 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 nickelate compound provides another example of previously inaccessible materials enabled by topotactic transformations and presents an interesting platform where mixed Ni valence can give rise to exotic phenomena.

Superconductivity in infinite-layer nickelates has stirred much research interest, to which questions regarding the nature of superconductivity remain elusive. A critical leap forward to address these intricate questions is through the growth of high-crystallinity infinite-layer nickelates, including the “parent” phase. Here, we report the synthesis of a high-quality thin-film nickelate, NdNiO2. This is achieved through the growth of a perovskite precursor phase (NdNiO3) of superior crystallinity on the NdGaO3substrate by off-axis RF magnetron sputtering and a low-temperature topochemical reduction using NaH. We observe a nonlinear Hall effect at low temperatures in this “non-doped” phase. We further study the electronic properties using advanced X-ray scattering and first-principles calculations. We observe spectroscopic indications of the enhanced two-dimensionality and a reduced hybridization of Nd 5dand Ni 3dorbitals. These findings unlock new pathways for preparing high-quality infinite-layer nickelates and provide new insights into the intrinsic features of these compounds.

The discovery of superconductivity in Nd0.8Sr0.2NiO2(ref. 1) introduced a new family of layered nickelate superconductors that has now been extended to include a range of strontium doping2,3, praseodymium or lanthanum in place of neodymium4–7, and the five-layer compound Nd6Ni5O12(ref. 8). A number of studies have indicated that electron correlations are strong in these materials9–15, a feature that often leads to the emergence of magnetism. Here we report muon spin rotation/relaxation studies of a series of superconducting infinite-layer nickelates. Regardless of the rare earth ion or doping, we observe an intrinsic magnetic ground state 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 pnictides16and heavy fermion compounds17, and qualitatively distinct from the doped cuprates18.

Simultaneous manipulation of multiple boundary conditions in nanoscale heterostructures offers a versatile route to stabilizing unusual structures and emergent phases. Here, we show that a stable supercrystal phase comprising a three-dimensional ordering of nanoscale domains with tailored periodicities can be engineered in PbTiO3–SrRuO3ferroelectric–metal superlattices. A combination of laboratory and synchrotron X-ray diffraction, piezoresponse force microscopy, scanning transmission electron microscopy and phase-field simulations reveals a complex hierarchical domain structure that forms to minimize the elastic and electrostatic energy. Large local deformations of the ferroelectric lattice are accommodated by periodic lattice modulations of the metallic SrRuO3layers with curvatures up to 107m−1. Our results show that multidomain ferroelectric systems can be exploited as versatile templates to induce large curvatures in correlated materials, and present a route for engineering correlated materials with modulated structural and electronic properties that can be controlled using electric fields.

Negative capacitance is observed in a model system of multidomain ferroelectric–dielectric superlattices; the multidomain state can increase the temperature range over which negative capacitance can be observed.