Spatial hierarchy of microstructure is a defining characteristic of many practical materials systems. Elements of this hierarchy are often realized through nonequilibrium synthesis and process routes, leading to metastable structures that confer specific functionality and enhanced performance. The key to accelerating understanding and developing new and improved materials lies in quantifying microstructure in an unambiguous digital format, employing both physical models and data science methods to explore cause-and-effect relations between structure and properties and relations between composition-dependent process path history and hierarchical microstructure. Given the current state of predictive multiscale modeling, the uncertainties are simply too high to provide necessary decision support in isolation from experiments. Hence, combining experiments and computational modeling with materials data science and informatics provides the only practical path forward in replacing the historical paradigm of empirical materials development. The articles in this issue focus on microstructure informatics, which is relatively less well explored than the use of first-principles combinatorial methods applied to search the space of stable compounds, small molecules, and interface structures.

Frequently, fundamental scientific and technological issues are related to the chemical structure of a material at the nanometer or even atomistic length scales. This includes, but is not limited to, internal interfaces of complex topology as they appear, for example, in current energy-harvesting applications or advanced microelectronics. Scientific understanding of the underlying physics and chemistry requires advanced characterization tools that provide critical three-dimensional information at the subnanometer length scale. Atom probe tomography (APT) meets such requirements. Today, with remarkable progress in instrumentation and sample preparation, APT has become a very versatile tool to address fundamental questions of materials science. In this issue of MRS Bulletin, the APT technique is introduced, with a particular focus on recent developments and the broadening range of studied material classes and applications.

Ultrafast laser synthesis and processing of materials is a burgeoning field that is still in its infancy. This article and the theme articles in this issue review recent developments in the fundamental physics of ultrafast laser–solid interactions as well as the state of our understanding of ultrafast laser-driven surface morphology, modification of transparent media, 3D photo-polymerization and additive fabrication, spallation of graphene, and biological interactions. Also reviewed is the current state of emerging commercial high average power lasers, central to the widespread adoption of ultrafast laser synthesis and processing of materials. It is remarkable that ultrafast lasers with 20 to 600 femtosecond pulse duration can have such a dramatic impact on materials. As we learn more about the fundamental mechanisms that drive the ultrafast laser-material response, even more applications are anticipated to emerge. This revolutionary approach to materials synthesis and processing has already spawned several commercial technologies and promises to create many more in the near future.

Mechanisms of dislocation generation and methods of crystal growth are two historically rich areas of scientific study. These two fields converge in the area of metamorphic epitaxial materials, where the goal is to produce high-performance devices that contain high densities of crystal defects in regions of the engineered material away from the active areas. Metamorphic epitaxy is a form of thin-film growth, where the lattice structure of the layer and substrate are mismatched, and its defining characteristic is that any elastic strain in the overlayer has been relaxed by the deliberate introduction of dislocations at the film–substrate interface. Metamorphic growth enables novel combinations of relaxed single-crystal materials to realize novel functionality and performance in numerous technological areas, including lasers, photovoltaics, transistors, and quantum computing. Many of the devices described in this issue are impossible to realize using the traditional approach of avoiding dislocation generation; instead, they rely on metamorphic epitaxy to attain high performance.

Three-dimensional (3D) printing of metallic materials involves the layerwise consolidation of feedstock materials in the form of powder, wire, or sheet using various energy sources to form complex shapes. The past two decades have witnessed significant advances in the field, in terms of both technologies and materials for metal 3D printing. This has led to widespread exploration and adoption of the technologies across industry, academia, and R&D organizations. This article presents an overview of the field of metal 3D printing. A brief history of metal 3D printing is followed by an overview of metal 3D printing methods and metallic material systems used in these methods. Microstructure and properties, and their relationship to process parameters are discussed next, followed by current challenges and qualification issues. The article concludes with future trends and a brief description of the invited articles included in this special issue.

Hierarchical design draws inspiration from analysis of biological materials and has opened new possibilities for enhancing performance and enabling new functionalities and extraordinary properties. With the development of nanotechnology, the necessary technological requirements for the manufacturing of hierarchical materials are advancing at a fast pace, opening new challenges and opportunities. This article presents an overview of possible applications of and perspectives on hierarchical materials.

Twins are domain crystals inside their parent crystals, where they share some of the same crystal lattice points in a symmetrical manner. The formation and growth of twins result in substantial evolution of microstructures and properties in a large variety of metallic materials. Twin boundaries that separate two crystals effectively strengthen the material by impeding mobile dislocations, and increase the ductility and work-hardening capability of metallic materials. The articles in this issue of MRS Bulletin overview the synthesis and mechanical behavior of nanotwinned metallic materials, as well as plasticity dominated by mechanical twinning.

Three-dimensional (3D) tomography using electrons and x-rays has pushed and expanded our understanding of the micro- and nanoscale spatial organization of inorganic, organic, and biological materials. While a significant impact on the field of materials science has already been realized from tomography applications, new advanced methods are quickly expanding the versatility of this approach to better link structure, composition, and function of complex 3D assemblies across multiple scales. In this article, we highlight several frontiers where new developments in tomography are empowering new science across biology, chemistry, and physics. The five articles that appear in this issue of MRS Bulletin describe some of these latest developments in detail, including analytical electron tomography, atomic resolution electron tomography, advanced recording schemes in scanning transmission electron microscopy (STEM) tomography, cryo-STEM tomography of whole cells, and multiscale correlative tomography.

Synchrotron radiation has evolved tremendously in recent decades in sources, instrumentation, and applications in materials studies. This article provides background and an introduction to the state of the art of synchrotron research as it relates to materials research, including an overview of the articles in this MRS Bulletin issue, which focus on Laue microdiffraction, high-energy x-ray diffraction on battery materials, synchrotron radiation in high-pressure research, x-ray dark-field microscopy, and x-ray absorption spectroscopy applied to energy research. The modern approach of displaying diffraction data in reciprocal-space units and the distinction between spectroscopy and diffraction are summarized. Applications and technologies are continuously developing toward technical and optical limits, combining multiple methods for an even brighter future for this field. It is now time for expert groups to begin applying multiple and different kinds of quantum beams, such as neutrons, muons, electrons, and ions, complementary to synchrotron radiation for more efficient and effective characterization of materials.

Conventional photolithography is an effective patterning technique that has enabled modern electronics and advanced micro- and nanoscale devices. However, it has limitations, including high cost, limited resolution, and poor compatibility with unconventional materials that may be soft, nonplanar, or difficult to process. There is active research ongoing to develop unconventional patterning methods such as self-organization and self-folding. Self-organization harnesses various driving forces to produce patterns without external intervention and includes methods such as self-assembly of block copolymers, capillary-driven assembly of micro-/nanoscale structures, and thin-film instabilities. Self-folding (origami)—and its cousin, kirigami—harnesses patterning and materials strategies to convert planar substrates into three-dimensional shapes in response to external stimuli. These multidisciplinary approaches open many engineering opportunities by providing new and versatile material functionalities. This article overviews the field and the topics covered in the articles in this issue of MRS Bulletin, highlighting recent progress in patterning approaches based on self-organization and self-folding.

Metal–organic frameworks (MOFs), with their crystalline nanoporous three-dimensional structures, have emerged as unique multifunctional materials that combine high porosity with catalytic, photophysical, or other properties to reveal new fundamental science and applications. Because MOFs are composed of organic molecules linking metal centers in ways that are not usually conducive to the formation of free-charge carriers or low-energy charge-transport pathways, they are typically insulators. Accordingly, applications so far have harnessed the unique structural properties and porosity of MOFs, which depend only to a small extent on the ability to manipulate their electronic structure. An exciting new area has emerged due to the recent demonstration of MOFs with controlled electronic and optical properties, which is enabling new fundamental science and opens up the possibility of applications in electronics and photonics. This article presents an overview of the fundamental science issues related to controlling electronic and optical properties of MOFs, and how research groups worldwide have been exploring such properties for electronics, thermoelectrics, photophysics, and charge storage.

Nucleation is the first step in the formation of many materials; understanding its microscopic dynamics is crucial for improving synthesis of existing materials and predicting under what conditions novel materials will form. The simple picture of nucleation that prevailed for more than a century does not account for complex nucleation pathways observed in recent years in experiments and simulations. A more general framework is needed to explain reported phenomena; such a framework must account for the peaks and valleys in the free-energy landscape across which nucleation takes place and for the microscopic dynamic factors that dictate how a system explores this landscape. The articles of this issue illustrate and describe the many complex nucleation pathways seen across a range of material systems.

Short pulse laser irradiation has the ability to bring a material into a state of strong electronic, thermal, phase, and mechanical nonequilibrium and trigger a sequence of structural transformations leading to the generation of complex multiscale surface morphologies, unusual metastable phases, and microstructures that cannot be produced by any other means. In this article, we provide an overview of recent advancements and existing challenges in the understanding of the fundamental mechanisms of short pulse laser interaction with materials, including the material response to strong electronic excitation, ultrafast redistribution and partitioning of the deposited laser energy, the peculiarities of phase transformations occurring under conditions of strong superheating/undercooling, as well as laser-induced generation of crystal defects and modification of surface microstructure.

The development of metal–organic frameworks (MOFs) as microporous electronic conductors is an exciting research frontier that has the potential to revolutionize a wide range of technologically and industrially relevant fields, from catalysis to solid-state sensing and energy-storage devices, among others. After nearly two decades of intense research on MOFs, examples of intrinsically conducting MOFs remain relatively scarce; however, enormous strides have recently been made. This article briefly reviews the current status of the field, with a focus on experimental milestones that have shed light on crucial structure–property relationships that underpin future progress. Central to our discussion are a series of design considerations, including redox-matching, donor–acceptor interactions, mixed valency, and π-interactions. Transformational opportunities exist at both fundamental and applied levels, from improved measurement techniques and theoretical understanding of conduction mechanisms to device engineering. Taken together, these developments will herald a new era in advanced functional materials.