Powering ≈50 µm Motion by a Molecular Event in DNA Crystals

Abstract

A major challenge in material design is to couple nanoscale molecular and supramolecular events into desired chemical, physical, and mechanical properties at the macroscopic scale. Here, a novel self‐assembled DNA crystal actuator is reported, which has reversible, directional expansion and contraction for over 50 μm in response to versatile stimuli, including temperature, ionic strength, pH, and redox potential. The macroscopic actuation is powered by cooperative dissociation or cohesion of thousands of DNA sticky ends at the designed crystal contacts. The increase in crystal porosity and cavity in the expanded state dramatically enhances the crystal capability to accommodate/encapsulate nanoparticles/proteins, while the contraction enables a “sponge squeezing” motion for releasing nanoparticles. This crystal actuator is envisioned to be useful for a wide range of applications, including powering self‐propelled robotics, sensing subtle environmental changes, constructing functional hybrid materials, and working in drug controlled‐release systems.

Engineering DNA Crystals toward Studying DNA–Guest Molecule Interactions

“…In the P 3 2 crystals, the 2 nm wide, continuous channels could accommodate up to 2 nm guest objects, including most organic compounds, peptides, oligosaccharides, small nucleic acids (aptamers, ribozymes, and DNAzymes), and small proteins. The engineered DNA crystals may also be explored for other applications such as for catalysis, − separation, − and information − and matter storage. , …”

Augmented DNA Nanoarchitectures: A Structural Library of 3D Self‐Assembling Tensegrity Triangle Variants

“…This includes the augmentation of the hexagonal phenotype of DNA tensegrity triangle arrangement through linker modulation; [8] more controllable or predictable recognition, binding, and harboring of guest macromolecules; [1a,10,19] crystallization and structural elucidation of complex DNA tiles as linkers; [24] structure elucidation of modified nucleic acids; [25] pH-responsive DNA crystallization through linked i-motif structures; [26] increased programmability of metal mediated DNA and more complex molecular electronics; [9,27] and designer crystals with electronically or magnetically active nanomaterials such as nanoparticles or carbon allotropes in asymmetric, circuit-like orientations. [16,17,28] One of the foundational goals of DNA nanotechnology is the harboring of guest macromolecules toward their structural determination. In this study, we have expanded the library of macromolecules that can be applied toward this goal, and we have further validated the systematic approach to the alteration and augmentation of DNA nanoarchitectures.…”

“…[14] Greater control over rhombohedral face size and lattice cavity size is necessary for the design and construction of nanostructures capable of being crystallized in tandem with a wider range of guest species. DNA crystals have thus far been utilized as vehicles to study and perform catalysis; [15] organize and trap nanoparticles through molecular motion; [16] template complex assemblies of organic semiconductors; [17] host a variety of fluorescent and triple helical guests; [3,18] and function as macromolecular sieves for the selective, albeit nonspecific, adsorption of proteins. [19] Yet the idea that inspired the field of structural DNA nanotechnology-to precisely orient and position guest macromolecules along DNA scaffolds for their structure determination via X-ray crystallographyhas eluded us in practice.…”

Highly Symmetric, Self‐Assembling 3D DNA Crystals with Cubic and Trigonal Lattices

“…The trigonal honeycombs shown here may possess greater compression and tensile strength than previously reported hexagons, yielding novel structural functionality. With recent advances in molecular motion, [13] organic semiconductors, [14] and more, self-assembling 3D DNA crystals have achieved a level of precision and versatility that could not have been imagined from their inception. Expanding our understanding of self-assembly pathways, mechanisms, and results can only further diversify the topological design space and subsequent applications of structural DNA nanotechnology.…”