In this review, a comprehensive overview of recent progress and achievements in defect engineering of electrode materials towards superior reaction kinetics for supercapacitors are presented. 

Defect engineering of electrode materials towards superior reaction kinetics for high-performance supercapacitors

The integration of dissimilar materials in heterostructures has long been a cornerstone of modern materials science—seminal examples are 2D materials and van der Waals heterostructures. Recently, new methods have been developed that enable the realization of ultrathin freestanding oxide films approaching the 2D limit. Oxides offer new degrees of freedom, due to the strong electronic interactions, especially the 3d orbital electrons, which give rise to rich exotic phases. Inspired by this progress, a new platform for assembling freestanding oxide thin films with different materials and orientations into artificial stacks with heterointerfaces is developed. It is shown that the oxide stacks can be tailored by controlling the stacking sequences, as well as the twist angle between the constituent layers with atomically sharp interfaces, leading to distinct moiré patterns in the transmission electron microscopy images of the full stacks. Stacking and twisting is recognized as a key degree of structural freedom in 2D materials but, until now, has never been realized for oxide materials. This approach opens unexplored avenues for fabricating artificial 3D oxide stacking heterostructures with freestanding membranes across a broad range of complex oxide crystal structures with functionalities not available in conventional 2D materials.

Stacking and Twisting of Freestanding Complex Oxide Thin Films

Decades of advancements in strategies for the calculation of atomic interactions have culminated in a class of methods known as machine-learning interatomic potentials (MLIAPs). MLIAPs dramatically widen the spectrum of materials systems that can be simulated with high physical fidelity, including their microstructural evolution and kinetics. This framework, in conjunction with cross-scale simulations and in silico microscopy, is poised to bring a paradigm shift to the field of atomistic simulations of materials. In this prospective article we summarize recent progress in the application of MLIAPs to crystal defects. Graphical abstract

/pdf/machine-learning-potentials-for-crystal-defects-s929ryvf.pdf

Machine-learning potentials for crystal defects

Abstract The potential of dislocations (line defects) in ceramics may have been greatly underrated until most recently. Promising proofs‐of‐concept have been demonstrated for dislocation‐tuned functional and mechanical properties, revealing a new research front for dislocations in ceramics for a wide range of potential applications. However, it is commonly known that ceramics are hard (difficult to deform) and brittle (easy to fracture), particularly at room temperature. It remains a great challenge to mechanically tailor dislocations in ceramics. To address this pressing bottleneck, this article discusses the mechanics‐based dislocation engineering in ceramics by examining the three fundamental factors of dislocation nucleation, multiplication, and motion. Successful experimental approaches to tune dislocation density and plastic zone size on single‐crystal strontium titanate are demonstrated. The dislocation‐based competition between plastic deformation and crack formation is discussed. The aspects of coupling external fields to manipulate dislocations are highlighted, which may hold the key to modulating the charged dislocation cores in ceramics and opening new routes for mechanical tailoring of dislocations at room temperature. Some open questions and challenges for engineering dislocations in ceramics are discussed. 

Mechanical tailoring of dislocations in ceramics at room temperature: A perspective

Dislocation-enhanced electrical conductivity in rutile TiO2 accessed by room-temperature nanoindentation

Dislocations in ionic solids are topological extended defects that modulate composition, strain, and charge over multiple length scales. As such, they provide an extra degree of freedom to tailor ionic and electronic transport beyond limits inherent in bulk doping. Heterogeneity of transport paths as well as the ability to dynamically reconfigure structure and properties through multiple stimuli lend dislocations to particular potential applications including memory, switching, non-Ohmic electronics, capacitive charge storage, and single-atom catalysis. However, isolating, understanding, and predicting causes of modified transport behavior remain a challenge. In this Perspective, we first review existing reports of dislocation-modified transport behavior in oxides, as well as synthetic strategies and multiscale characterization routes to uncover processing-structure-property relationships. We outline a vision for future research, suggesting outstanding questions, tasks, and opportunities. Advances in this field will require highly interdisciplinary, convergent computational-experimental approaches, covering orders of magnitude in length scale, and spanning fields from microscopy and machine learning to electro-chemo-mechanics and point defect chemistry to transport-by-design and advanced manufacturing.

Dislocation-Mediated Conductivity in Oxides: Progress, Challenges, and Opportunities.

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Dislocation-Mediated Conductivity in Oxides: Progress, Challenges, and Opportunities.