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Updated: Dec 27, 2025

Atomically Defined Templates for Epitaxial Growth of Complex Oxide Thin Films
Published on: December 4, 2014
Hidden Subsurface Reconstruction and Its Atomic Origins in Layered Oxide Cathodes
Linze Li1, Ethan C Self2, Devendrasinh Darbar2,3
1Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, 902 Battelle Boulevard, Richland, Washington 99354, United States.
Structural transformations in layered oxide cathodes surprisingly begin below the surface, not at the outermost layer. This subsurface initiation is linked to atomic changes and composition gradients, offering new insights for Li-ion battery materials.
Area of Science:
- Solid-state materials science
- Surface science
- Materials chemistry
Background:
- Structural transformations near surfaces are crucial for applications like catalysis, memory, and energy storage.
- Traditionally, these transformations were thought to originate from the outermost atomic layers.
Purpose of the Study:
- To investigate the initial stages of the layered-to-spinel-like structural transformation in layered oxide cathodes for Li-ion batteries.
- To determine the precise location where this transformation initiates at the atomic level.
Main Methods:
- Atomic-level scanning transmission electron microscopy (STEM) imaging.
- Electron energy loss spectroscopy (EELS) for compositional analysis.
Main Results:
- Observed the structural transformation initiating from subsurface layers, not the surface.
- Identified reconstructed subsurfaces with mixed layered and spinel-like structures.
- Found selective atomic partitioning and nanoscale compositional gradients at the subsurface.
Conclusions:
- The study challenges the long-standing notion of surface-initiated transformations.
- Provides fundamental, atomic-scale insights into structural transformation mechanisms in layered cathodes.
- Highlights the importance of subsurface regions in material functionalization.
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