Molecular Lithography on Silicon Wafers Guided by Porous, Extended Arrays of Small DNA Tiles.

Tile-based DNA self-assembly is a cost-effective fabrication method for large-scale nanopatterns. Herein, we report a protocol to directly assemble DNA 2D arrays on silicon wafers and then use the DNA nanostructures as molds to fabricate the corresponding nanostructures on the silicon wafers by hydrogen fluoride (HF) etching. Similar HF etching has been used with robust large DNA origami structures as templates.

Implementing Logic Gates by DNA Crystal Engineering.

DNA self-assembly computation is attractive for its potential to perform massively parallel information processing at the molecular level while at the same time maintaining its natural biocompatibility. It has been extensively studied at the individual molecule level, but not as much as ensembles in 3D. Here, the feasibility of implementing logic gates, the basic computation operations, in large ensembles: macroscopic, engineered 3D DNA crystals is demonstrated.

Divergence and Convergence: Complexity Emerges in Crystal Engineering from an 8-mer DNA.

Biology provides plenty of examples on achieving complicated structures out of minimal numbers of building blocks. In contrast, structural complexity of designed molecular systems is achieved by increasing the numbers of component molecules. In this study, the component DNA strand assembles into a highly complex crystal structure via an unusual path of divergence and convergence.

Engineering DNA Crystals toward Studying DNA-Guest Molecule Interactions.

Sequence-selective recognition of DNA duplexes is important for a wide range of applications including regulating gene expression, drug development, and genome editing. Many small molecules can bind DNA duplexes with sequence selectivity. It remains as a challenge how to reliably and conveniently obtain the detailed structural information on DNA-molecule interactions because such information is critically needed for understanding the underlying rules of DNA-molecule interactions.

Near-Quantitative Preparation of Short Single-Stranded DNA Circles.

Small, single-stranded DNA (ssDNA) circles have many applications, such as templating rolling circle amplification (RCA), capturing microRNAs, and scaffolding DNA nanostructures. However, it is challenging to prepare such ssDNA circles, particularly when the DNA size becomes very small (e.g.

Programmable 3D Hexagonal Geometry of DNA Tensegrity Triangles.

Non-canonical interactions in DNA remain under-explored in DNA nanotechnology. Recently, many structures with non-canonical motifs have been discovered, notably a hexagonal arrangement of typically rhombohedral DNA tensegrity triangles that forms through non-canonical sticky end interactions. Here, we find a series of mechanisms to program a hexagonal arrangement using: the sticky end sequence; triangle edge torsional stress; and crystallization condition.

DNA conformational equilibrium enables continuous changing of curvatures.

Assembly of complex structures from a small set of tiles is a common theme in biology. For example, many copies of identical proteins make up polyhedron-shaped, viral capsids and tubulin can make long microtubules. This inspired the development of tile-based DNA self-assembly for nanoconstruction, particularly for structures with high symmetries.

Tomography of DNA tiles influences the kinetics of surface-mediated DNA self-assembly.

This manuscript studies the impact of extruding hairpins on two-dimensional self-assembly of DNA tiles on solid surface. Hairpins are commonly used as tomographic markers in DNA nanostructures for atomic force microscopy imaging. In this study, we have discovered that hairpins play a more active role.

Assembly of Two-Dimensional DNA Arrays Could Influence the Formation of Their Component Tiles.

Tile-based DNA self-assembly is a powerful approach for nano-constructions. In this approach, individual DNA single strands first assemble into well-defined structural tiles, which, then, further associate with each other into final nanostructures. It is a general assumption that the lower-level structures (tiles) determine the higher-level, final structures.

Programming DNA Self-Assembly by Geometry†.

This manuscript introduces geometry as a means to program the tile-based DNA self-assembly in two and three dimensions. This strategy complements the sequence-focused programmable assembly. DNA crystal assembly critically relies on intermotif, sticky-end cohesion, which requires complementarity not only in sequence but also in geometry.

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

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.

A generalizable method for the construction of MOF@polymer functional composites through surface-initiated atom transfer radical polymerization.

We report a generalizable approach to construct MOF@polymer functional composites through surface-initiated atom transfer radical polymerization (SI-ATRP). Unlike conventional SI-ATRP that requires covalent pre-anchoring of the initiating group on substrate surfaces, in our approach, a rationally designed random copolymer (RCP) macroinitiator first self-assembles on MOF surfaces through inter-chain hydrogen bond crosslinking. Subsequent polymerization in the presence of a crosslinking monomer covalently threads these polymer chains into a robust network, physically confining the MOF particle inside the polymer shell.

Adhesive bacterial amyloid nanofiber-mediated growth of metal-organic frameworks on diverse polymeric substrates.

The development of a simple, robust, and generalizable approach for spatially controlled growth of metal-organic frameworks (MOFs) on diverse polymeric substrates is of profound technological significance but remains a major challenge. Here, we reported the use of adhesive bacterial amyloid nanofibers, also known as curli nanofibers (CNFs), major protein components of bacterial biofilms, as universal and chemically/mechanically robust coatings on various polymeric substrates to achieve controlled MOF growth with improved surface coverage up to 100-fold. Notably, owing to the intrinsic adhesive attributes of CNFs, our approach is applicable for MOF growth on both 2D surfaces and 3D objects regardless of their geometric complexity.