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The discovery of ambient-pressure nickelate high-temperature superconductivity provides a new platform for probing the underlying superconducting mechanisms. However, the thermodynamic metastability of Ruddlesden-Popper nickelates Lnn+1NinO3n+1 (Ln = lanthanide) presents significant challenges in achieving precise control over their structure and oxygen stoichiometry. This study establishes a systematic approach for growing phase-pure, high-quality Ln3Ni2O7 thin films on LaAlO3 and SrLaAlO4 substrates using gigantic-oxidative atomic-layerby-layer epitaxy. The films grown under an ultrastrong oxidizing ozone atmosphere are superconducting without further post annealing. Specifically, the optimal Ln3Ni2O7/SrLaAlO4 superconducting film exhibitsan onset transition temperature (Tc,onset) of 50 K. Four critical factors governing the crystalline quality and superconducting properties of Ln3Ni2O7 films are identified: 1) precise cation stoichiometric control suppresses secondary phase formation. In a Ni-rich sample (+7%), the thin film forms a Ln4Ni3O10 secondary phase, and the R-T curve correspondingly exhibits metallic behavior. In contrast, a Ni-deficient sample forms a Ln2NiO4 secondary phase, with its R-T curve indicating insulating behavior over the entire temperature range. 2) Complete atomic layer-by-layer coverage minimizes stacking faults. Deviation from ideal monolayer coverage induces in-plane atomic number mismatch, whichdirectly triggers out-of-plane lattice collapse or uplift near bulkequilibrium positions. 3) Optimized interface reconstruction can improve the atomic arrangement at the interface. This can be achieved through methods such as annealing the SrLaAlO4 substrate or pre-depositing a 0.5-unit-cell-thick Ln2NiO4-phase buffer layer, which enhances the energy difference between the Ln-site and Ni-site layers to promote proper stacking. 4) Accurate oxygen content regulation is essential for achieving a single superconducting transition and high Tc,onset. Although the under-oxidized sample demonstrates a relatively high Tc,onset (50 K), it displays a two-step superconducting transition. Conversely, the over-oxidized sample exhibits a reduced Tc,onset of 37 K and similarly manifests a two-step transition. These findings provide valuable insights for the layer-by-layer epitaxy growth of diverse oxide high-temperature superconducting films
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Keywords:
- nickelate superconducting thin film /
- Ruddlesden-Popper phase /
- gigantic-oxidative atomic-layer-by-layer epitaxy /
- surface structure
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