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Temperature-dependent dynamic disproportionation in LiNiO2.

Andrey D Poletayev1,2, Robert J Green3,4, Jack E N Swallow5,6

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Nature Communications
|October 23, 2025
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Dynamic disproportionation of nickel ions in lithium nickel oxide (LiNiO2) explains its diverse properties. This finding unifies understanding of nickelate materials for energy and computing applications.

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Condensed Matter Physics

Background:

  • Lithium nickel oxide (LiNiO2) is a key nickelate material with diverse applications.
  • Its complex electronic structure and Ni ion behavior remain incompletely understood.

Purpose of the Study:

  • Investigate the temperature-dependent speciation and spin dynamics of Ni ions in LiNiO2.
  • Develop a unified model explaining the material's diverse physical properties.

Main Methods:

  • Ab initio simulations to predict Ni ion states and dynamics.
  • X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) at the Ni L3,2-edge.
  • Resonant inelastic X-ray scattering (RIXS) and charge-transfer multiplet (CTM) calculations.

Main Results:

  • Simulations predicted Ni ions disproportionating into three dynamically interconverting states with temperature-dependent populations.
  • Experimental techniques confirmed this dynamic disproportionation model.
  • CTM calculations successfully reproduced all experimental features, validating the proposed model.

Conclusions:

  • A dynamic disproportionation model unifies understanding of LiNiO2 properties, including magnetic, electronic, and defect behavior.
  • This research provides crucial insights into nickelate materials for energy storage, catalysis, and superconductivity.
  • Understanding Ni ion behavior is key for optimizing nickelate functionalities.