Probing Interfaces in Complex Oxide Heterostructures via 17O Solid State NMR Spectroscopy

13 May 2020, Version 1
This content is a preprint and has not undergone peer review at the time of posting.


The determination of the atomic-scale structure of a solid–solid interface is a major outstanding problem in the physical sciences, the structure controlling many properties including stability, ionic and electronic transport, magnetism, multiferroicity and superconductivity. NMR spectroscopy is sensitive to local structure but is not typically sufficiently sensitive or selective to observe solid–solid interfaces. In this work, CeO2–SrTiO3 vertically aligned nanocomposite (VAN) thin films are studied and, by combining selective isotopic enrichment with a lift-off technique to remove the substrate, the 17O NMR signal from single atomic layer interfaces can clearly be seen. The interfacial structure is solved by calculating the NMR parameters using density functional theory combined with random structure searching. By performing the isotopic enrichment at variable temperatures, the superior oxide-ion conductivity of the VAN films compared to the bulk materials is shown to arise in part from enhanced oxygen mobility at this interface; oxygen motion at the interface is further identified from 17O relaxometry experiments. These results highlight the information that can be obtained on interfacial structure and dynamics with solid-state NMR spectroscopy, in this and other nanostructured systems, our methodology being generally applicable to overcome sensitivity limitations in thin-film studies.


VAN films
thin films
Vertically aligned nanocomposites
Solid State NMR Spectroscopy
17O-NMR spectroscopy
oxide-ion conductivity
oxygen diffusion
Random structure searching
NMR Spectroscopy

Supplementary materials

Lift off 17O NMR SI


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