Atomically resolved imaging of materials enabled by the advent of aberration-corrected scanning transmission electron microscopy (STEM) has become a mainstay of modern materials science. However, much of the wealth of quantitative information contained in the fine details of atomic structure or spectra remains largely unexplored. In this article, we discuss new opportunities enabled by physics-informed big data and machine learning technologies to extract physical information from static and dynamic STEM images, ranging from statistical thermodynamics of alloys to kinetics of solid-state reactions at a single defect level. The synergy of deep-learning image analytics and real-time feedback further allows harnessing beam-induced atomic and bond dynamics to enable direct atom-by-atom fabrication. Examples of direct atomic motion over mesoscopic distances, engineered doping at selected lattice sites, and assembly of multiatomic structures are reviewed. These advances position the scanning transmission electron microscope to transition from a mere imaging tool toward a complete nanoscale laboratory for exploring electronic, phonon, and quantum phenomena in atomically engineered structures.

Ferroelectric single-crystal-architecture-in-glass is a new class of metamaterials that would enable active integrated optics if the ferroelectric behavior is preserved within the confines of glass. We demonstrate using lithium niobate crystals fabricated in lithium niobosilicate glass by femtosecond laser irradiation that not only such behavior is preserved, the ferroelectric domains can be engineered with a DC bias. A piezoresponse force microscope is used to characterize the piezoelectric and ferroelectric behavior. The piezoresponse correlates with the orientation of the crystal lattice as expected for unconfined crystal, and a complex micro- and nano-scale ferroelectric domain structure of the as-grown crystals is revealed.

Scanning transmission electron microscopy (STEM) has become the main stay for materials characterization on atomic level, with applications ranging from visualization of localized and extended defects to mapping order parameter fields. In recent years, attention has focused on the potential of STEM to explore beam induced chemical processes and especially manipulating atomic motion, enabling atom-by-atom fabrication. These applications, as well as traditional imaging of beam sensitive materials, necessitate increasing the dynamic range of STEM in imaging and manipulation modes, and increasing the absolute scanning speed which can be achieved by combining sparse sensing methods with nonrectangular scanning trajectories. Here we have developed a general method for real-time reconstruction of sparsely sampled images from high-speed, noninvasive and diverse scanning pathways, including spiral scan and Lissajous scan. This approach is demonstrated on both the synthetic data and experimental STEM data on the beam sensitive material graphene. This work opens the door for comprehensive investigation and optimal design of dose efficient scanning strategies and real-time adaptive inference and control of e-beam induced atomic fabrication.

New developments in manufacturing and automation, from three-dimensional printing to the “Internet of things,” signify dramatic changes in our society. The push toward quantum materials is driving device fabrication toward atomic precision. Recent results suggest that scanning transmission electron microscopy (STEM) with sub-angstrom scale beams could offer a solution. However, a detailed theoretical understanding of the interaction of the electron beam with solids is needed to form a basis for new technology. This article summarizes the existing literature on electron-beam interactions with solids with a focus on irreversible transformation. We further suggest that the theoretical framework of a two-temperature model developed for fast ion damage in solids could be applicable to predicting the effects of fast electrons. Recent results from STEM-directed epitaxial growth on crystalline–amorphous interfaces are discussed in detail. Finally, perspectives on the development of this field in the near future are offered.

The two current reigning paradigms enabling nanotechnology are scanning probe microscopy and molecular machine devices that date back to seminal experiments by Eigler and visionary work by Drexler, respectively. The nanoscience and nanotechnology community is seeing the emergence of a third paradigm—the use of the atomically focused beam of a scanning transmission electron microscope (STEM) to control and direct matter on the atomic scale. Beam-induced modifications involving one atom or a small group of atoms can be induced and monitored in real time with atomic resolution. Combined with the development of beam-control electronics, big data acquisition, and analytical tools such as artificial intelligence-based feedback systems, electron and ion microscopies are at the brink of a transition from purely imaging tools to tools capable of creating structures with atomic precision and high throughput. In this issue of MRS Bulletin, we present recent advances in electron- and ion-beam-based atomic fabrication on surfaces, in layered materials, and finally in three dimensions—the ultimate dream and possibly the final frontier of nanoscience.