Atomic scale imaging of competing polar states in a Ruddlesden–Popper layered oxide

Greg Stone, Colin Ophus, Turan Birol, Jim Ciston, Che-Hui Lee, Ke Wang, Craig J. Fennie, Darrell G. Schlom, Nasim Alem and Venkatraman Gopalan ()
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Greg Stone: Pennsylvania State University
Colin Ophus: National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory
Turan Birol: University of Minnesota
Jim Ciston: National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory
Che-Hui Lee: Pennsylvania State University
Ke Wang: Materials Characterization Laboratory, Materials Research Institute, Pennsylvania State University
Craig J. Fennie: School of Applied and Engineering Physics, Cornell University
Darrell G. Schlom: Cornell University
Nasim Alem: Pennsylvania State University
Venkatraman Gopalan: Pennsylvania State University

Nature Communications, 2016, vol. 7, issue 1, 1-9

Abstract: Abstract Layered complex oxides offer an unusually rich materials platform for emergent phenomena through many built-in design knobs such as varied topologies, chemical ordering schemes and geometric tuning of the structure. A multitude of polar phases are predicted to compete in Ruddlesden–Popper (RP), An+1BnO3n+1, thin films by tuning layer dimension (n) and strain; however, direct atomic-scale evidence for such competing states is currently absent. Using aberration-corrected scanning transmission electron microscopy with sub-Ångstrom resolution in Srn+1TinO3n+1 thin films, we demonstrate the coexistence of antiferroelectric, ferroelectric and new ordered and low-symmetry phases. We also directly image the atomic rumpling of the rock salt layer, a critical feature in RP structures that is responsible for the competing phases; exceptional quantitative agreement between electron microscopy and density functional theory is demonstrated. The study shows that layered topologies can enable multifunctionality through highly competitive phases exhibiting diverse phenomena in a single structure.

Date: 2016
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DOI: 10.1038/ncomms12572

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