Perovskites are promising functional materials for their optoelectronic properties and anion migration plays a key role in their functional performance [1-3]. By using in-situ (S)TEM mechanical and electrical testing in conjunction with 4D-STEM [4,5], we directly observed/probed anion migration in perovskites at atomic resolution (see Figure 1). Here, we studied the mechanism for the anion migration in perovskites such as (PbZr)TiO3 and BaTiO3, which is induced under the mechnaicl/electrical loading. To avoid the influence of the electron beam, we carried out the in-situ (S)TEM study at 60kv with low dose. And to avoid the possible strong size effect and the substrate (interface) influence, we prepared free-standing sub-micrometer single-crystalline structures to perform the experiments. Corresponding EDS and EELS examinations were performed to measure the local chemical change with applied stress and electrical currents. Our observations revealed the coexistence of multiple phase structures and hierarchical domain structures, as well as the greatly enhanced anion drifting and diffusion at the charged domain walls (Figure 2) and phase boundaries. The complex interaction between the local domain evolution and phase transition has been discussed. Based on above investigations, a model for anion migration in perovskire under mechanical/electrical loading has been presented.

Scanning transmission electron microscopy (STEM) allows for imaging, diffraction, and spectroscopy of materials on length scales ranging from microns to atoms. By using a high-speed, direct electron detector, it is now possible to record a full two-dimensional (2D) image of the diffracted electron beam at each probe position, typically a 2D grid of probe positions. These 4D-STEM datasets are rich in information, including signatures of the local structure, orientation, deformation, electromagnetic fields, and other sample-dependent properties. However, extracting this information requires complex analysis pipelines that include data wrangling, calibration, analysis, and visualization, all while maintaining robustness against imaging distortions and artifacts. In this paper, we present py4DSTEM, an analysis toolkit for measuring material properties from 4D-STEM datasets, written in the Python language and released with an open-source license. We describe the algorithmic steps for dataset calibration and various 4D-STEM property measurements in detail and present results from several experimental datasets. We also implement a simple and universal file format appropriate for electron microscopy data in py4DSTEM, which uses the open-source HDF5 standard. We hope this tool will benefit the research community and help improve the standards for data and computational methods in electron microscopy, and we invite the community to contribute to this ongoing project.

One of the primary uses for transmission electron microscopy (TEM) is to measure diffraction pattern images in order to determine a crystal structure and orientation. In nanobeam electron diffraction (NBED), we scan a moderately converged electron probe over the sample to acquire thousands or even millions of sequential diffraction images, a technique that is especially appropriate for polycrystalline samples. However, due to the large Ewald sphere of TEM, excitation of Bragg peaks can be extremely sensitive to sample tilt, varying strongly for even a few degrees of sample tilt for crystalline samples. In this paper, we present multibeam electron diffraction (MBED), where multiple probe-forming apertures are used to create multiple scanning transmission electron microscopy (STEM) probes, all of which interact with the sample simultaneously. We detail designs for MBED experiments, and a method for using a focused ion beam to produce MBED apertures. We show the efficacy of the MBED technique for crystalline orientation mapping using both simulations and proof-of-principle experiments. We also show how the angular information in MBED can be used to perform 3D tomographic reconstruction of samples without needing to tilt or scan the sample multiple times. Finally, we also discuss future opportunities for the MBED method.