Three-dimensional (3D) tomographic imaging of the structural, chemical, and physical properties of a material provides key knowledge that links the structure of a material to both its processing and structure that is central to studies across a broad spectrum of materials. For many decades, tomography using x-rays or electrons has proven to be an essential 3D characterization tool. In recent years, advances in technology have significantly pushed the envelope of these techniques in many respects, enabling new imaging capabilities at the nanometer and atomic scale. This article highlights several such developments in nanoscale x-ray and electron tomography. The five articles that appear in this issue of MRS Bulletin discuss research frontiers that include multimodal x-ray tomography at the nanoscale, x-ray spectroscopic tomography, dark-field x-ray microscopy, electron nanotomography for functional nanomaterials, and atomistic imaging by electron tomography. These articles give a holistic view of the status of these techniques and promising future directions, as well highlighting their applications for scientific problems.

The available x-ray brightness from accelerator-based light sources has been increasing at a rate faster than Moore’s Law. This is enabling new developments in x-ray tomography, using nanoscale x-ray beams on materials ranging in size from micrometers to centimeters. With scanning, one can record x-ray diffraction patterns to view nanoscale structure beyond the optic resolution, or fluorescence signals to study elemental distributions in three dimensions. These approaches are being used in various applications, for example, to study the redistribution of intrinsic metals in biological cells and tissues during biological processes, to compare as-fabricated versus as-designed integrated circuits, and to see the domain structure of soft ferromagnetic materials. While some applications face challenges, including radiation dose, new developments in sparse sampling and reconstruction algorithms, along with a new generation of diffraction-limited storage rings, offer exciting opportunities for materials research.

Dark-field x-ray microscopy is intended for the acquisition of three -dimensional (3D) movies of the nanostructure (grains, domains, and dislocations) and the associated local strain within bulk materials. It is analogous to dark-field electron microscopy in that an objective lens magnifies diffracting features of the sample. The use of high-energy synchrotron x-rays, however, means that these microstructural features can be large and deeply embedded. The spatial and angular resolution is on the order of 100 nm and 0.001°, respectively, and full maps can be recorded in seconds to minutes. Four applications of the technique are presented—domain switching in ferroelectrics, processing of metals, microstructural characterization of biominerals, and visualization of dislocations. The ability to directly characterize complex, multiscale phenomena in situ—and in 3D—is a key step toward formulating and validating multiscale models that account for the entire heterogeneity of materials.

At the forefront of developments in synchrotron x-ray microscopy, nanoscale-resolution high-dimensional spectrotomography under controlled sample environments has been demonstrated. Such cutting-edge experimental capability has been broadly applied to scientific studies in the field of energy materials science, where the dynamically evolving structural and chemical defects play a vital role in the functionality. In this article, we review novel developments of this technique from both experimental and data/information mining perspectives. Using studies on lithium-ion battery electrode materials as examples, we highlight the rich information in the high-dimensional and high-resolution x-ray tomographic data, which can be used to interpret the complicated thermal-electro-chemo-mechanical interplay that occurs under the operating conditions and collectively determines battery performance. We also discuss the frontier challenges in this field and our perspectives of the future directions in the context of projected major developments in the landscape of large-scale x-ray facilities across the globe.

Atomic electron tomography (AET) has become a powerful tool for atomic-scale structural characterization in three and four dimensions. It provides the ability to correlate structures and properties of materials at the single-atom level. With recent advances in data acquisition methods, iterative three-dimensional (3D) reconstruction algorithms, and post-processing methods, AET can now determine 3D atomic coordinates and chemical species with sub-Angstrom precision, and reveal their atomic-scale time evolution during dynamical processes. Here, we review the recent experimental and algorithmic developments of AET and highlight several groundbreaking experiments, which include pinpointing the 3D atom positions and chemical order/disorder in technologically relevant materials and capturing how atoms rearrange during early nucleation at four-dimensional atomic resolution.

Modern nanomaterials contain complexity that spans all three dimensions—from multigate semiconductors to clean energy nanocatalysts to complex block copolymers. For nanoscale characterization, it has been a long-standing goal to observe and quantify the three-dimensional (3D) structure—not just surfaces, but the entire internal volume and the chemical arrangement. Electron tomography estimates the complete 3D structure of nanomaterials from a series of two-dimensional projections taken across many viewing angles. Since its first introduction in 1968, electron tomography has progressed substantially in resolution, dose, and chemical sensitivity. In particular, scanning transmission electron microscope tomography has greatly enhanced the study of 3D nanomaterials by providing quantifiable internal morphology and spectroscopic detection of elements. Combined with recent innovations in computational reconstruction algorithms and 3D visualization tools, scientists can interactively dissect volumetric representations and extract meaningful statistics of specimens. This article highlights the maturing field of electron tomography and the widening scientific applications that utilize 3D structural, chemical, and functional imaging at the nanometer and subnanometer length scales.