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On the Topotactic Phase Transition Achieving Superconducting Infinite-Layer Nickelates.

Yan Li1, Changjiang Liu1, Hong Zheng1

  • 1Materials Science Division, Argonne National Laboratory, Lemont, IL, 60439, USA.

Advanced Materials (Deerfield Beach, Fla.)
|September 2, 2024
PubMed
Summary

Topotactic reduction of nickelates requires an ultrathin surface layer to mediate hydrogen introduction and remove apical oxygens. This process enables defect-free phase transitions crucial for achieving superconductivity in materials like Nd$_{0.8}$Sr$_{0.2}$NiO$_{2}$.

Keywords:
in situ X‐ray characterizationinfinite‐layer nickelatesoxygen octahedral rotationtime‐of‐flight secondary ion mass spectrometrytopotactic phase transition

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Superconductivity

Background:

  • Topotactic reduction is essential for synthesizing superconducting nickelates, such as Nd$_{0.8}$Sr$_{0.2}$NiO$_{2}$, from precursor heterostructures like Nd$_{0.8}$Sr$_{0.2}$NiO$_{3}$/SrTiO$_{3}$.
  • Reproducing superconductivity in these materials is challenging due to the sensitivity and potential damage caused by the reduction process.

Purpose of the Study:

  • To elucidate the structural mechanisms governing the topotactic reduction pathway in nickelate heterostructures.
  • To identify the key factors enabling the successful synthesis of superconducting nickelates and guide future research.

Main Methods:

  • In situ synchrotron-based investigations were employed to study the reduction process.
  • Analysis focused on the interface between Nd$_{0.8}$Sr$_{0.2}$NiO$_{3}$ and SrTiO$_{3}$ during reduction.

Main Results:

  • An ultrathin surface layer on Nd$_{0.8}$Sr$_{0.2}$NiO$_{3}$ mediates hydrogen introduction and apical oxygen removal at the interface.
  • This mediation allows for the stabilization and propagation of the square-planar/perovskite interface without defects.
  • No significant geometric rotations or hydrogen incorporation within the films were observed.

Conclusions:

  • The formation of an intermediate surface layer is critical for defect-free topotactic reduction in nickelates.
  • Understanding this pathway is key to reliably achieving superconductivity in reduced nickelate systems.