Electrical energy storage systems such as batteries would benefit enormously from integrating all device components in three-dimensional (3-D) architectures on the nanoscale to improve their power capability without negatively impacting the device-scale energy density. However, the lack of large scale synthesis methods of 3-D architectures with precise spatial control of multiple, functional energy materials at the nanoscale remains a key issue holding back the development of such intricate device designs. To achieve fully integrated, multi-material nano-3-D architectures, next-generation nanofabrication requires departure from the traditional top-down patterning methods. Here, we present an approach to such systems based on the bottom-up synthesis of co-continuous nanohybrids with all necessary functional battery components rationally integrated in a triblock terpolymer derived core–shell double gyroid architecture. In our design three-dimensional periodically ordered, functional anode and cathode nanonetworks are separated by an ultrathin electrolyte phase within a single 3-D nanostructure. All materials are less than 20 nm in their layer dimensions, co-continuous and interpenetrating in 3-D, and extended throughout a macroscopic monolith. The electrochemical analysis of our solid-state nano-3-D Li-ion/sulfur system demonstrated battery-like characteristics with stable open circuit voltage, reversible discharge voltage and capacity, and orders of magnitude decreases in footprint area compared to two-dimensional thin layer designs.
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DNA origami: The bridge from bottom to top
Over the last decade, DNA origami has matured into one of the most powerful bottom-up nanofabrication techniques. It enables both the fabrication of nanoparticles of arbitrary two-dimensional or three-dimensional shapes, and the spatial organization of any DNA-linked nanomaterial, such as carbon nanotubes, quantum dots, or proteins at ∼5-nm resolution. While widely used within the DNA nanotechnology community, DNA origami has yet to be broadly applied in materials science and device physics, which now rely primarily on top-down nanofabrication. In this article, we first introduce DNA origami as a modular breadboard for nanomaterials and then present a brief survey of recent results demonstrating the unique capabilities created by the combination of DNA origami with existing top-down techniques. Emphasis is given to the open challenges associated with each method, and we suggest potential next steps drawing inspiration from recent work in materials science and device physics. Finally, we discuss some near-term applications made possible by the marriage of DNA origami and top-down nanofabrication.
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- Award ID(s):
- 1636364
- NSF-PAR ID:
- 10081419
- Date Published:
- Journal Name:
- MRS Bulletin
- Volume:
- 42
- Issue:
- 12
- ISSN:
- 0883-7694
- Page Range / eLocation ID:
- 943 to 950
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Wireframe DNA origami has emerged as a powerful approach to fabricating nearly arbitrary 2D and 3D geometries at the nanometer-scale. Complex scaffold and staple routing needed to design wireframe DNA origami objects, however, render fully automated, geometry-based sequence design approaches essential for their synthesis. And wireframe DNA origami structural fidelity can be limited by wireframe edges that are composed only of one or two duplexes. Here we introduce a fully automated computational approach that programs 2D wireframe origami assemblies using honeycomb edges composed of six parallel duplexes. These wireframe assemblies show enhanced structural fidelity from electron microscopy-based measurement of programmed angles compared with identical geometries programmed using dual-duplex edges. Molecular dynamics provides additional theoretical support for the enhanced structural fidelity observed. Application of our top-down sequence design procedure to a variety of complex objects demonstrates its broad utility for programmable 2D nanoscale materials.
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Abstract Hybrid RNA:DNA origami, in which a long RNA scaffold strand folds into a target nanostructure via thermal annealing with complementary DNA oligos, has only been explored to a limited extent despite its unique potential for biomedical delivery of mRNA, tertiary structure characterization of long RNAs, and fabrication of artificial ribozymes. Here, we investigate design principles of three-dimensional wireframe RNA-scaffolded origami rendered as polyhedra composed of dual-duplex edges. We computationally design, fabricate, and characterize tetrahedra folded from an EGFP-encoding messenger RNA and de Bruijn sequences, an octahedron folded with M13 transcript RNA, and an octahedron and pentagonal bipyramids folded with 23S ribosomal RNA, demonstrating the ability to make diverse polyhedral shapes with distinct structural and functional RNA scaffolds. We characterize secondary and tertiary structures using dimethyl sulfate mutational profiling and cryo-electron microscopy, revealing insight into both global and local, base-level structures of origami. Our top-down sequence design strategy enables the use of long RNAs as functional scaffolds for complex wireframe origami.
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Structural DNA nanotechnology has enabled the design and construction of complex nanoscale structures with precise geometry and programmable dynamic and mechanical properties. Recent efforts have led to major advances in the capacity to actuate shape changes of DNA origami devices and incorporate DNA origami into larger assemblies, which open the prospect of using DNA to design shape-morphing assemblies as components of micro-scale reconfigurable or sensing materials. Indeed, a few studies have constructed higher order assemblies with reconfigurable devices; however, these demonstrations have utilized structures with relatively simple motion, primarily hinges that open and close. To advance the shape changing capabilities of DNA origami assemblies, we developed a multi-component DNA origami 6-bar mechanism that can be reconfigured into various shapes and can be incorporated into larger assemblies while maintaining capabilities for a variety of shape transformations. We demonstrate the folding of the 6-bar mechanism into four different shapes and demonstrate multiple transitions between these shapes. We also studied the shape preferences of the 6-bar mechanism in competitive folding reactions to gain insight into the relative free energies of the shapes. Furthermore, we polymerized the 6-bar mechanism into tubes with various cross-sections, defined by the shape of the individual mechanism, and we demonstrate the ability to change the shape of the tube cross-section. This expansion of current single-device reconfiguration to higher order scales provides a foundation for nano to micron scale DNA nanotechnology applications such as biosensing or materials with tunable properties.more » « less
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Abstract Wireframe DNA origami assemblies can now be programmed automatically from the top-down using simple wireframe target geometries, or meshes, in 2D and 3D, using either rigid, six-helix bundle (6HB) or more compliant, two-helix bundle (DX) edges. While these assemblies have numerous applications in nanoscale materials fabrication due to their nanoscale spatial addressability and high degree of customization, no easy-to-use graphical user interface software yet exists to deploy these algorithmic approaches within a single, standalone interface. Further, top-down sequence design of 3D DX-based objects previously enabled by DAEDALUS was limited to discrete edge lengths and uniform vertex angles, limiting the scope of objects that can be designed. Here, we introduce the open-source software package ATHENA with a graphical user interface that automatically renders single-stranded DNA scaffold routing and staple strand sequences for any target wireframe DNA origami using DX or 6HB edges, including irregular, asymmetric DX-based polyhedra with variable edge lengths and vertices demonstrated experimentally, which significantly expands the set of possible 3D DNA-based assemblies that can be designed. ATHENA also enables external editing of sequences using caDNAno, demonstrated using asymmetric nanoscale positioning of gold nanoparticles, as well as providing atomic-level models for molecular dynamics, coarse-grained dynamics with oxDNA, and other computational chemistry simulation approaches.more » « less
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1557/mrs.2017.275
