To utilize the intrinsic properties of 2D materials, it is important to control both interlayer interfaces and intralayer dislocations. Significant efforts have been made mostly to suppress the formation of crystalline disorders by developing advanced material growths [10][11][12] and integration techniques, [13] resulting in single-crystalline materials with atomically clean interfaces. However, structural boundaries can provide exciting control knobs to program the material properties beyond what is available in the thermodynamically most stable forms if the boundaries are fabricated controllably. Prototypical examples are the electrical doping of materials by introducing impurities [14] and optimizing device performances for targeted functionalities by forming heterojunctions. [15] Furthermore, 2D materials of van der Waals (vdW) structures arbitrarily enable the control of their atomic configurations due to the weak interlayer interactions. Therefore, various types of structural boundaries with different crystalline symmetries and band structures have been reported even in a single material platform by atomic displacements, [16,17] crystalline misorientation, [18] and distortions of chemical bonding [19,20] without the introduction of foreign materials. They have provided testbeds to discover novel electrical properties, [21] which are inaccessible in perfect crystals. However, direct applications of the material properties are elusive due to the lack of techniques to precisely control the boundaries over technologically relevant scales.In this review, we discuss about the emerging properties of structural boundaries in vdW structures and the developments of techniques to control the boundaries at the atomic scale. We focus on boundary structures caused by atomic displacements within a single-crystalline material, rather than heterogeneous boundaries with chemical complexity, which have been summarized in detail elsewhere. [22] We discuss the remaining critical issues to reproduce functional boundaries by a designer approach for the discovery of properties and applications in electronics and provide our outlook on the directions in the field.
Boundary Types and Related Properties in vdW SolidsA grain boundary is an interfacial plane that exists between two perfect crystallites. The boundaries are not randomly formed, and the resultant structures are restricted by the crystalline lattices, in which they are embedded. The structural defects emerge at the boundaries of misaligned crystalline domains, whose rotation axis most likely points to the out-of-plane Engineering the boundary structures in 2D materials provides an unprecedented opportunity to program the physical properties of the materials with extensive tunability and realize innovative devices with advanced functionalities. However, structural engineering technology is still in its infancy, and creating artificial boundary structures with high reproducibility remains difficult. In this review, various emergent properties of 2D materials with different ...