Gauss's law dictates that the net electric field inside a conductor in electrostatic equilibrium is zero by effective charge screening; free carriers within a metal eliminate internal dipoles that may arise owing to asymmetric charge distributions. Quantum physics supports this view, demonstrating that delocalized electrons make a static macroscopic polarization, an ill-defined quantity in metals--it is exceedingly unusual to find a polar metal that exhibits long-range ordered dipoles owing to cooperative atomic displacements aligned from dipolar interactions as in insulating phases. Here we describe the quantum mechanical design and experimental realization of room-temperature polar metals in thin-film ANiO3 perovskite nickelates using a strategy based on atomic-scale control of inversion-preserving (centric) displacements. We predict with ab initio calculations that cooperative polar A cation displacements are geometrically stabilized with a non-equilibrium amplitude and tilt pattern of the corner-connected NiO6 octahedral--the structural signatures of perovskites--owing to geometric constraints imposed by the underlying substrate. Heteroepitaxial thin-films grown on LaAlO3 (111) substrates fulfil the design principles. We achieve both a conducting polar monoclinic oxide that is inaccessible in compositionally identical films grown on (001) substrates, and observe a hidden, previously unreported, non-equilibrium structure in thin-film geometries. We expect that the geometric stabilization approach will provide novel avenues for realizing new multifunctional materials with unusual coexisting properties.

The metal-insulator transition in correlated materials is usually coupled to a symmetrylowering structural phase transition. This coupling not only complicates the understanding of the basic mechanism of this phenomenon but also limits the speed and endurance of prospective electronic devices. We demonstrate an isostructural, purely electronically driven metal-insulator transition in epitaxial heterostructures of an archetypal correlated material, vanadium dioxide. A combination of thin-film synthesis, structural and electrical characterizations, and theoretical modeling reveals that an interface interaction suppresses the electronic correlations without changing the crystal structure in this otherwise correlated insulator. This interaction stabilizes a nonequilibrium metallic phase and leads to an isostructural metal-insulator transition. This discovery will provide insights into phase transitions of correlated materials and may aid the design of device functionalities.

The control of the in-plane domain evolution in ferroelectric thin films is not only critical to understanding ferroelectric phenomena but also to enabling functional device fabrication. However, in-plane polarized ferroelectric thin films typically exhibit complicated multi-domain states, not desirable for optoelectronic device performance. Here we report a strategy combining interfacial symmetry engineering and anisotropic strain to design single-domain, in-plane polarized ferroelectric BaTiO3 thin films. Theoretical calculations predict the key role of the BaTiO3/PrScO3$${({{{{{\boldsymbol{110}}}}}})}_{{{{{{\bf{O}}}}}}}$$ ( 110 ) O substrate interfacial environment, where anisotropic strain, monoclinic distortions, and interfacial electrostatic potential stabilize a single-variant spontaneous polarization. A combination of scanning transmission electron microscopy, piezoresponse force microscopy, ferroelectric hysteresis loop measurements, and second harmonic generation measurements directly reveals the stabilization of the in-plane quasi-single-domain polarization state. This work offers design principles for engineering in-plane domains of ferroelectric oxide thin films, which is a prerequisite for high performance optoelectronic devices.

The dielectric phase transition behavior of imprinted lead magnesium niobate–lead titanate relaxor ferroelectric thin films was mapped as a function of temperature and dc bias. To compensate for the presence of internal fields, an external electric bias was applied while measuring dielectric responses. The constructed three-dimensional dielectric maps provide insight into the dielectric behaviors of relaxor ferroelectric films as well as the temperature stability of the imprint. The transition temperature and diffuseness of the dielectric response correlate with crystallographic disorder resulting from strain and defects in the films grown on strontium titanate and silicon substrates; the latter was shown to induce a greater degree of disorder in the film as well as a dielectric response lower in magnitude and more diffuse in nature over the same temperature region. Strong and stable imprint was exhibited in both films and can be utilized to enhance the operational stability of piezoelectric devices through domain self-poling.

We report the observation of ferromagnetism in thin films of paramagnetic metal LaNiO3 grown on non-magnetic insulating substrate LaAlO3 (111) substrates. The films exhibit a large hysteresis loop on magnetoresistance and anomalous Hall effect as well as six-fold anisotropic magnetoresistance. Together with the ferroelectricity and inversion symmetry breaking reported in the same system, these results suggest that, by the geometric constraints by the substrate, paramagnetic metals can turn into ferromagnetic semiconductors. The ferromagnetic ground state is consistent with the predicted spin-split Fermi surfaces of spin-orbit-coupled correlated metals. Moreover, our results reveal a positive linear magnetoresistance and a sign reversal of hysteresis loop, which is consistent with the existence of massive Dirac point as predicted by theories.