LYU Wei; NIE Zihao; WANG Heng; CHEN Yaqi; HUANG Haoliang; ZHOU Guangdi; XUE Qikun; CHEN Zhuoyu

doi:10.7498/aps.74.20251080

Abstract

The discovery of ambient-pressure nickelate high-temperature superconductivity provides a new platform for further exploring the underlying superconducting mechanisms. However, the thermodynamic metastability of Ruddlesden-Popper nickelates Ln_n+1Ni_nO_3n+1 (Ln = lanthanide) poses significant challenges for precise control over their structures and oxygen stoichiometry. This study establishes a systematic approach to growing phase-pure, high-quality Ln₃Ni₂O₇ thin films on LaAlO₃ and SrLaAlO₄ substrates by using gigantic-oxidative atomic-layer-by-layer epitaxy. The films grown under an ultrastrong oxidizing ozone atmosphere are superconducting without further post-annealing. Specifically, the optimal Ln₃Ni₂O₇/SrLaAlO₄ superconducting film exhibits an onset transition temperature (T_c,onset) of 50 K. Four critical factors governing the crystalline quality and superconducting properties of Ln₃Ni₂O₇ films are identified as follows. 1) Precise cation stoichiometric control suppresses secondary phase formation. In an Ni-rich sample (+7%), the thin film forms an Ln₄Ni₃O₁₀ secondary phase, and the R-T curve correspondingly exhibits metallic behavior. In contrast, an Ni-deficient sample forms an 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, which directly triggers out-of-plane lattice collapse or uplift near bulk-equilibrium 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 T_c,onset. Although the under-oxidized sample demonstrates a relatively high T_c,onset (50 K), it displays a two-step superconducting transition. Conversely, the over-oxidized sample exhibits a reduced T_c,onset of 37 K and similarly manifests a two-step transition. These findings provide valuable insights into the layer-by-layer epitaxy growth of diverse oxide high-temperature superconducting films.

Keywords:

nickelate superconducting thin film /
Ruddlesden-Popper phase /
gigantic-oxidative atomic-layer-by-layer epitaxy /
surface structure

Authors and contacts

Corresponding author: CHEN Zhuoyu, chenzhuoyu@sustech.edu.cn

Funds: Project supported by the National Basic Research Program of China (Grant Nos. 2024YFA1408101, 2022YFA1403101), the National Natural Science Foundation of China (Grant Nos. 92265112, 12374455, 52388201), the Quantum Science Strategic Initiative of Guangdong Province, China (Grant Nos. GDZX2401004, GDZX2201001), the Municipal Funding Co-Construction Program of Shenzhen, China, China (Grant Nos. SZZX2401001, SZZX2301004), and the Science and Technology Program of Shenzhen, China (Grant No. KQTD20240729102026004).

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