Atomically precise interfaces from non-stoichiometric deposition

Abstract

Complex oxide heterostructures display some of the most chemically abrupt, atomically precise interfaces, which is advantageous when constructing new interface phases with emergent properties by juxtaposing incompatible ground states. One might assume that atomically precise interfaces result from stoichiometric growth, but here we show that the most precise control is obtained for non-stoichiometric growth where differing surface energies can be compensated by surfactant-like effects. For the precise growth of Sr${}_{n+1}$Ti${}_n$O${}_{3n+1}$ Ruddlesden-Popper (RP) phases, stoichiometric deposition leads to the loss of the first RP rock-salt double layer, but growing with a strontium-rich surface layer restores the bulk stoichiometry and ordering of the subsurface RP structure. Our results dramatically expand the materials that can be prepared in epitaxial heterostructures with precise interface control---from just the $n=\infty$ end members (perovskites) to the entire RP family---enabling the exploration of novel quantum phenomena at a richer variety of oxide interfaces.

9 pages, 5 figures

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• The SIESTA method for ab initio order-N materials simulation
• Efficient index handling of multidimensional periodic boundary conditions
• Magnetic effects at the interface between nonmagnetic oxides
• On the Doping and Temperature Dependence of the Mass Enhancement Observed in the Cuprate Bi2212
• First-principles calculation of the band offset at BaO/BaTiO${}_3$ and SrO/SrTiO${}_3$ interfaces
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• Defect engineering in oxide heterostructures by enhanced oxygen surface exchange

Cited by in corpus (30)

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• Engineering mass transport properties in oxide ionic and mixed ionic electronic thin film ceramic conductors for energy applications
• Dynamic Interface Rearrangement in LaFeO${}_3$ / $n$-SrTiO${}_3$ Heterojunctions
• Synthesis and electronic properties of Nd${}_{n+1}$Ni${}_n$O${}_{3n+1}$ Ruddlesden-Popper nickelate thin films
• First-principles Modelling of SrTiO3 based Oxides for Thermoelectric Applications
• A New Line Defect in NdTiO3 Perovskite
• Oxygen Vacancies on SrO-terminated SrTiO3(001) Surfaces studied by Scanning Tunneling Spectroscopy
• Perspective: Heusler interfaces -- opportunities beyond spintronics?
• Ferroelectricity and multiferroicity in anti-Ruddlesden-Popper structures
• SrTiO${}_3$ termination control: A method to tailor the oxygen exchange kinetics
• Epitaxial growth of Ruddlesden-Popper neodymium nickelates Nd${}_{n+1}$Ni${}_n$O${}_{3n+1}$ ($n$ = 1-5)
• In situ monitoring of atomic layer epitaxy via optical ellipsometry
• An efficient and reliable growth method for epitaxial complex oxide films by molecular beam epitaxy
• Dichotomy of the Photo Induced 2-Dimensional Electron Gas on SrTiO${}_3$ Surface Terminations
• In-situ Polarized Neutron Reflectometry: Epitaxial Thin Film Growth of Fe on Cu(001) by DC Magnetron Sputtering
• Magnetic proximity effect at the interface of two-dimensional materials and magnetic oxide insulators
• Nanoscale Sr${}_2$IrO${}_4$ Freestanding Thin-Films for Flexible Electronics
• Stabilization of the perovskite phase in the Y-Bi-O system by using a BaBiO${}_3$ buffer layer
• X-ray absorption spectroscopy study of the electronic and magnetic proximity effects in YBa${}_2$Cu${}_3$O${}_7$/La${}_{2/3}$Ca${}_{1/3}$MnO${}_3$ and La${}_{2-x}$Sr${}_x$CuO${}_4$/La${}_{2/3}$Ca${}_{1/3}$MnO${}_3$ multilayers
• Gigantic-oxidative atomic-layer-by-layer epitaxy for artificially designed complex oxides
• Correlating surface stoichiometry and termination in SrTiO${}_3$ films grown by hybrid molecular beam epitaxy
• Enabling two-dimensional electron gas with high room-temperature electron mobility exceeding 100 cm${}^2$/Vs at a perovskite oxide interface
• Order-Disorder Behavior at Thin Film Oxide Interfaces
• Design and realization of a sputter deposition system for the \textit{in situ-} and \textit{in operando-}use in polarized neutron reflectometry experiments
• Breaking symmetry to create a parallel-plate varactor dielectric with unparalleled microwave performance
• High-sensitivity of initial SrO growth on the residual resistivity in epitaxial thin films of SrRuO${}_3$ on SrTiO${}_3$ (001)
• Atomistic modeling of molecular beam epitaxy growth of SrTiO3 and Sr2TiO4 thin films