Capturing the hidden short-range order in amorphous oxide interfaces that directs quasi-epitaxial thin-film growth
Abstract
As solid-state device architectures become increasingly complex, buried interfaces play a critical role in determining thin-film texture, morphology, and defect formation. However, resolving the structural features that control growth on nominally amorphous interlayers remains challenging because it requires three-dimensional sensitivity at high spatial resolution. Here, we combine four-dimensional scanning transmission electron microscopy, fluctuation electron microscopy, and multislice electron ptychography to investigate ruthenium (Ru) thin films grown on an underlying amorphous Ta2O5 layer, a material stack relevant for next-generation electronic and spintronic devices. Although the Ta2O5 layer appears amorphous in conventional imaging, from diffraction and depth-resolved ptychographic reconstructions, nanoscale β-Ta2O5-like ordered motifs are revealed near the Ru/Ta2O5 interface. These locally ordered motifs, together with the interfacial morphology, guide the orientation of the Ru layer and produce a textured, quasi-epitaxial film. The curved and atomically rough interface further induces depth-dependent strain gradients and promotes planar defect formation within the Ru layer. Collectively, these results demonstrate that hidden short-range order within nominally amorphous oxides can direct the growth of metallic thin films, providing a framework for engineering buried interfaces in advanced electronic and spintronic material stacks.
Dataset DOI: 10.5061/dryad.w9ghx3g61
Description of the data and file structure
This dataset (dryad.zip) contains the files used for multislice electron ptychography reconstruction associated with Figure 4a-e of the main manuscript. The dataset includes:
- Four-dimensional scanning transmission electron microscopy (4D-STEM) datasets in .raw format
- EMPAD acquisition parameters and metadata in .json format
- Reconstruction configurations and processing parameters in .yaml format
- Ptychographic reconstruction outputs in .h5 format
Files and variables
File: dryad.zip
Description:
The .raw file contains a 4D-STEM dataset consisting of a two-dimensional real-space probe scan, with a two-dimensional diffraction pattern recorded at each scan position. The raw datasets can be viewed or processed using software such as the 4D-STEM Explorer application for macOS, the EMPAD-G2 Raw Reader package, or raw-data import plugins for Fiji. The files can also be accessed using custom Python scripts.
The .json file contains the acquisition parameters and metadata recorded by the EMPAD detector system during 4D-STEM data acquisition.
The .yaml file contains the reconstruction recipes used for multislice electron ptychography, including the parameters and settings.
The .h5 file contains the outputs of ptychographic reconstruction generated using Phaser, including the reconstructed object, probe, refined scan positions, diagnostic outputs, and reconstruction metadata. The principal variables are described below. More detailed information about the reconstruction output format is available in the Phaser documentation.
Variables in .h5 file:
1) Object: Reconstructed complex object transmission function stored in object/data. For multislice reconstructions, this dataset contains a series of depth-resolved object slices. Information describing the slice thickness and spatial sampling is also included.
2) Probe: Reconstructed complex incident electron wavefield stored in probe/data. When a mixed-state probe representation is used, the first dimension represents the different incoherent probe modes.
3) Scan: Final refined probe scan positions stored in scan.
4) Progress: Reconstruction diagnostics stored in progress, including convergence metrics, detector-error values, and the corresponding reconstruction iterations.
5) Iter: Reconstruction iteration information, including the engine number, engine iteration, and total iteration number.
Code/software
Performed using the Phaser package (https://doi.org/10.1038/s41524-026-01956-8)
