Polar Metals by Geometric Design

Journal Article · Thu May 05 00:00:00 EDT 2016 · Nature (London)

DOI:https://doi.org/10.1038/nature17628· OSTI ID:1275836

Kim, T. H.; Puggioni, D.; Yuan, Y.; Xie, L.; Zhou, H.; Campbell, N.; Ryan, P. J.; Choi, Y.; Kim, J. -W.; Patzner, J. R.; Ryu, S.; Podkaminer, J. P.; Irwin, J.; Ma, Y.; Fennie, C. J.; Rzchowski, M. S.; Pan, X. Q.; Gopalan, V.; Rondinelli, J. M.; Eom, C. B.

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(1). Quantum physics supports this view(2), demonstrating that delocalized electrons make a static macroscopic polarization, an ill-defined quantity in metals(3)-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(4). Here we describe the quantum mechanical design and experimental realization of room-temperature polar metals in thin-film ANiO(3) perovskite nickelates using a strategy based on atomic-scale control of inversion-preserving (centric) displacements(5). 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 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 unreported(6-10), 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.

• Research Organization: Argonne National Lab. (ANL), Argonne, IL (United States)
• Sponsoring Organization: USDOE Office of Science - Office of Basic Energy Sciences - Scientific User Facilities Division; National Science Foundation (NSF); U.S. Army Research Laboratory - U.S. Army Research Office (ARO)
• DOE Contract Number: AC02-06CH11357
• OSTI ID: 1275836
• Journal Information: Nature (London), Vol. 533, Issue 7601; ISSN 0028-0836
• Publisher: Nature Publishing Group
• Country of Publication: United States
• Language: English