Gigantic-oxidative atomic-layer-by-layer epitaxy for artificially designed complex oxides

Abstract

In designing material functionalities for transition metal oxides, lattice structure and d-orbital occupancy are key determinants. However, the modulation of these two factors is inherently limited by the need to balance thermodynamic stability, growth kinetics, and stoichiometry precision, particularly for metastable phases. We introduce a methodology, namely the gigantic-oxidative atomic-layer-by-layer epitaxy (GOALL-Epitaxy), enhancing oxidation power 3-4 orders of magnitude beyond conventional pulsed laser deposition (PLD) and oxide molecular beam epitaxy (OMBE), while ensuring atomic-layer-by-layer growth of designed complex structures. Thermodynamic stability is markedly augmented with stronger oxidation at elevated temperatures, whereas growth kinetics is sustained by laser ablation at lower temperatures. We demonstrate the accurate growth of complex nickelates and cuprates, especially an artificially designed structure with alternating single and double NiO2 layers possessing distinct nominal d-orbital occupancy, as a parent of high-temperature superconductor. The GOALL-Epitaxy enables material discovery within the vastly broadened growth parameter space.

References in corpus (18)

• Theory of Intertwined Orders in High Temperature Superconductors
• Superconductivity near 80 Kelvin in single crystals of La3Ni2O7 under pressure
• Quantum phases driven by strong correlations
• Oxide spin-orbitronics: spin-charge interconversion and topological spin textures
• Anomalously Strong Near-Neighbor Attraction in Doped 1D Cuprate Chains
• Atomically precise interfaces from non-stoichiometric deposition
• Nature of the metal-insulator transition in few-unit-cell-thick LaNiO3 films
• Nanoscale Phonon Spectroscopy Reveals Emergent Interface Vibrational Structure of Superlattices
• Epitaxial growth and electronic structure of Ruddlesden-Popper nickelates (${\mathrm{La}}_{n+1}{\mathrm{Ni}}_n{\mathrm{O}}_{3n+1},n=1-5$)
• Systematic electronic structure in the cuprate parent state from quantum many-body simulations
• Length-scales of interfacial coupling between metal-insulator phases in oxides
• Nodeless superconductivity arising from strong (pi,pi) antiferromagnetism in the infinite-layer electron-doped cuprate Sr1-xLaxCuO2
• High Tc superconductivity at the interface between the CaCuO2 and SrTiO3 insulating oxides
• Cuprate-like Electronic Structures in Infinite-Layer Nickelates with Substantial Hole Dopings
• Design and synthesis of three-dimensional hybrid Ruddlesden-Popper nickelate single crystals
• Electronic Structure of Superconducting Infinite-Layer Lanthanum Nickelates
• Direct observation of nodeless superconductivity and phonon modes in electron-doped copper oxide Sr${}_{1-x}$Nd${}_x$CuO${}_2$
• $\text{In situ}$ preparation of superconducting infinite-layer nickelate thin films with atomically flat surface

Cited by in corpus (6)

• Ambient-pressure superconductivity onset above 40 K in bilayer nickelate ultrathin films
• Angle-resolved photoemission spectroscopy of superconducting (La,Pr)3Ni2O7/SrLaAlO4 heterostructures
• Superconductivity and Electronic Structures of Nickelate Thin Film Superstructures
• Preparation and optimization of high-temperature superconducting Ruddlesden-Popper nickelate thin films
• Nodeless superconducting gap and electron-boson coupling in (La,Pr,Sm)${}_3$Ni${}_2$O${}_7$ films
• Progress of ambient-pressure superconductivity in bilayer nickelate thin films