Evolution of Multidimensional DNA Origami Crystal Habits by Bottom-Up Shaping and Top-Down Cutting

The modification of the macroscopic morphology of crystals constitutes a critical procedure in the device fabrication process, as it directly influences the physical and chemical characteristics of crystals, as well as the economic benefits. However, at the optico-microscopic scale (1–100 mm), the fine processing of crystal shapes and dimensions directly in solution is often more challenging to achieve, as the scale and environment of processing are both currently situated in a blank stage of technological development. In this work, we proposed a programmable wet-chemistry approach for processing the precise shapes of micrometer crystals and demonstrated the evolution of multidimensional DNA origami crystal habits, which exhibits predefined shapes, degrees of anisotropy, or dimensions. Significantly, this approach decouples the inherent symmetry of building blocks and packing modes to crystallization, thereby eliminating the necessity for the de novo design of DNA origami building blocks and the trial-and-error attempts on the connection modes. Furthermore, we illustrated the viability of exfoliating crystals along designated crystal planes directly in solution, which allows two-dimensional (2D) crystals to possess both the structural and the morphological characteristics inherited from the three-dimensional (3D) crystals. The accurate structural design, in conjunction with the customization of multidimensional habits, theoretically offers the potential for enhancement in diverse performances of DNA crystals.