Scanning Convergent-beam Electron Diffraction Research Articles

Revealing the Distribution of Lithium Compounds in Lithium Dendrites by Four-Dimensional Electron Microscopy Analysis.

Characterizing the microstructure of radiation- and chemical-sensitive lithium dendrites and its solid electrolyte interphase (SEI) is an important task when investigating the performance and reliability of lithium-ion batteries. Widely used methods, such as cryogenic high-resolution transmission electron microscopy as well as related spectroscopy, are able to reveal the local structure at nanometer and atomic scale; however, these methods are unable to show the distribution of various crystal phases along the dendrite in a large field of view. In this work, two types of four-dimensional electron microscopy diffractive imaging methods, i.e., scanning electron nanodiffraction (SEND) and scanning convergent beam electron diffraction (SCBED), are employed to show a new pathway on characterizing the sensitive lithium dendrite samples at room temperature and in a large field of view. Combining with the non-negative matrix factorization (NMF) algorithm, orientations of different lithium metal grains along the lithium dendrite as well as different lithium compounds in the SEI layer are clearly identified.

A data-driven cross-scale polarization states recognition method based on scanning convergent beam electron diffraction in ferroelectric ceramic

Ferroelectric materials showing piezoelectricity, pyroelectricity and other functional properties have been found a variety of applications in electrical and electronic devices. These properties highly rely on polarization states in multi-scale structures, including ferroelectric domains mainly in mesoscopic scale, domain walls in microscopic scale and so on. However, it is still lack of effective method to characterize multi-scale polarization states simultaneously in ferroelectric materials. Here, we proposed a data-driven cross-scale polarization state recognition method based on scanning convergent beam electron diffraction (SCBED) to characterize the complicated polarization states in a PbZr0.4Ti0.6O3 ceramic. This method employed a deep learning model to interpret the extensive dataset of CBED patterns generated during the scanning process and further validated by atomic resolution transmission electron microscope (ARTEM). The data-driven SCBED method provided a novel strategy for characterizing and interpreting the complicated cross-scale structure frame in ferroelectric materials.

Local negative permittivity and topological phase transition in polar skyrmions.

Topological solitons such as magnetic skyrmions have drawn attention as stable quasi-particle-like objects. The recent discovery of polar vortices and skyrmions in ferroelectric oxide superlattices has opened up new vistas to explore topology, emergent phenomena and approaches for manipulating such features with electric fields. Using macroscopic dielectric measurements, coupled with direct scanning convergent beam electron diffraction imaging on the atomic scale, theoretical phase-field simulations and second-principles calculations, we demonstrate that polar skyrmions in (PbTiO3)n/(SrTiO3)n superlattices are distinguished by a sheath of negative permittivity at the periphery of each skyrmion. This enhances the effective dielectric permittivity compared with the individual SrTiO3 and PbTiO3 layers. Moreover, the response of these topologically protected structures to electric field and temperature shows a reversible phase transition from the skyrmion state to a trivial uniform ferroelectric state, accompanied by large tunability of the dielectric permittivity. Pulsed switching measurements show a time-dependent evolution and recovery of the skyrmion state (and macroscopic dielectric response). The interrelationship between topological and dielectric properties presents an opportunity to simultaneously manipulate both by a single, and easily controlled, stimulus, the applied electric field.

Scanning Convergent Beam Electron Diffraction (CBED), the Essential Questions of Why, What and How?

Scanning Convergent Beam Electron Diffraction (CBED), the Essential Questions of Why, What and How?

Nanoscale symmetry fluctuations in ferroelectric barium titanate, BaTiO3.

Crystal charge density is a ground-state electronic property. In ferroelectrics, charge is strongly influenced by lattice and vice versa, leading to a range of interesting temperature-dependent physical properties. However, experimental determination of charge in ferroelectrics is challenging because of the formation of ferroelectric domains. Demonstrated here is the scanning convergent-beam electron diffraction (SCBED) technique that can be simultaneously used for imaging ferroelectric domains and identifying crystal symmetry and its fluctuations. Results from SCBED confirm the acentric tetragonal, orthorhombic and rhombohedral symmetry for the ferroelectric phases of BaTiO3. However, the symmetry is not homogeneous; regions of a few tens of nanometres retaining almost perfect symmetry are interspersed in regions of lower symmetry. While the observed highest symmetry is consistent with the displacive model of ferroelectric phase transitions in BaTiO3, the observed nanoscale symmetry fluctuations are consistent with the predictions of the order-disorder phase-transition mechanism.

Lattice-Rotation Vortex at the Charged Monoclinic Domain Boundary in a Relaxor Ferroelectric Crystal.

We present evidence of lattice-rotation vortices having an average radius of ∼7 nm at the ferroelectric domain boundary of (1-x)Pb(Zn_{1/3}Nb_{2/3})O_{3}-xPbTiO_{3} (x=0.08). Maps of crystal orientations and domain symmetry breaking are obtained using scanning convergent beam electron diffraction, which show fractional rotation vortices near the 50° monoclinic domain walls. The merging of 2D and 1D topological defects is consistent with inhomogeneous boundary charge and expected to have a large impact on the domain-switching mechanisms in relaxor ferroelectric crystals and ferroelectric devices.

Non-spectroscopic composition measurements of SrTiO3-La0.7Sr0.3MnO3 multilayers using scanning convergent beam electron diffraction

The local atomic structure of a crystalline sample aligned along a zone axis can be probed with a focused electron probe, which produces a convergent beam electron diffraction pattern. The introduction of high speed direct electron detectors has allowed for experiments that can record a full diffraction pattern image at thousands of probe positions on a sample. By incoherently summing these patterns over crystalline unit cells, we demonstrate that in addition to crystal structure and thickness, we can also estimate the local composition of a perovskite superlattice sample. This is achieved by matching the summed patterns to a library of simulated diffraction patterns. This technique allows for atomic-scale chemical measurements without requiring a spectrometer or hardware aberration correction.

Determination of 60° polarization nanodomains in a relaxor-based ferroelectric single crystal

Here, we report a determination of monoclinic nanodomains in PMN-xPT with x = 31%PT by using scanning convergent beam electron diffraction (SCBED). We show the presence of 60 ± α degree nanodomains with Cm-like symmetry as well as significant variations (α) in local polarization directions across lengths of ∼10 nm. The principle of our technique is general and can be applied for the determination of polarization domains in other ferroelectric materials of different symmetry.