Polar metals by geometric design

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Abstract

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 distributions1. Quantum physics supports this view2, demonstrating that delocalized electrons make a static macroscopic polarization, an ill-defined quantity in metals3—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 phases4. Here we describe the quantum mechanical design and experimental realization of room-temperature polar metals in thin-filmANiO3 perovskite nickelates using a strategy based on atomic-scale control of inversion-preserving (centric) displacements5. We predict withab initiocalculations that cooperative polarAcation displacements are geometrically stabilized with a non-equilibrium amplitude and tilt pattern of the corner-connected NiO6 octahedra—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 unreported6,7,8,9,10, 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.

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