Dynamically Reconfigurable DNA Origami Crystals Driven by a Designated Path Diagram

Constructing adaptable and switchable crystal structures renders it possible to dynamically control the properties and functions of adaptive materials, thereby expanding the potential application of these structures in fields such as optics, biology, and catalysis. Recently, researchers have developed various dynamic crystals possessing phase transition abilities. However, manufacturing switchable crystals with multiple-phase-transition ability by integrating various responsive behaviors into different dimensions of a single lattice remains considerably challenging. Herein, we built a set of dynamically reconfigurable DNA origami crystals by orthogonally integrating multiple dynamic effectors into the prescribed dimensions of the octahedral DNA origami frames. Further, we independently manipulated and logically combined the dynamic behaviors of the effectors in different dimensions. The initial mother phase and three derived daughter phases were interconnected into a path diagram by six elementary paths. Furthermore, these paths could be superimposed under multiple stimulus instructions by design to obtain the desired intricate transition routes. Moreover, finer manipulations were also applied to these paths to obtain extra new phase stations for the path diagram. To conveniently detect these phase transitions, a color-based visualization strategy was developed that converted the microscopic symmetry transformation of the lattices into macroscopic color changes that could be observed via a fluorescence microscope. Hence, this strategy lays the foundation for artificially constructing biomimetic functional crystals.