Chemistries that Facilitate Nanotechnology Kim E. Sapsford,† W. Russ Algar, Lorenzo Berti, Kelly Boeneman Gemmill,‡ Brendan J. Casey,† Eunkeu Oh, Michael H. Stewart, and Igor L. Medintz*,‡ †Division of Biology, Department of Chemistry and Materials Science, Office of Science and Engineering Laboratories, U.S. Food and Drug Administration, Silver Spring, Maryland 20993, United States ‡Center for Bio/Molecular Science and Engineering Code 6900 and Division of Optical Sciences Code 5611, U.S. Naval Research Laboratory, Washington, D.C. 20375, United States College of Science, George Mason University, 4400 University Drive, Fairfax, Virginia 22030, United States Department of Biochemistry and Molecular Medicine, University of California, Davis, School of Medicine, Sacramento, California 95817, United States Sotera Defense Solutions, Crofton, Maryland 21114, United States

Functionalizing nanoparticles with biological molecules: developing chemistries that facilitate nanotechnology.

The field of supramolecular chemistry focuses on the non-covalent interactions between molecules that give rise to molecular recognition and self-assembly processes. Since most non-covalent interactions are relatively weak and form and break without significant activation barriers, many supramolecular systems are under thermodynamic control. Hence, traditionally, supramolecular chemistry has focused predominantly on systems at equilibrium. However, more recently, self-assembly processes that are governed by kinetics, where the outcome of the assembly process is dictated by the assembly pathway rather than the free energy of the final assembled state, are becoming topical. Within the kinetic regime it is possible to distinguish between systems that reside in a kinetic trap and systems that are far from equilibrium and require a continuous supply of energy to maintain a stationary state. In particular, the latter systems have vast functional potential, as they allow, in principle, for more elaborate structural and functional diversity of self-assembled systems - indeed, life is a prime example of a far-from-equilibrium system. In this Review, we compare the different thermodynamic regimes using some selected examples and discuss some of the challenges that need to be addressed when developing new functional supramolecular systems.

Supramolecular systems chemistry

This review discusses one-dimensional supramolecular polymers that form in aqueous media. First, naturally occurring supramolecular polymers are described, in particular, amyloid fibrils, actin filaments, and microtubules. Their structural, thermodynamic, kinetic, and nanomechanical properties are highlighted, as well as their importance for the advancement of biologically inspired supramolecular polymer materials. Second, five classes of synthetic supramolecular polymers are described: systems based on (1) hydrogen-bond motifs, (2) large π-conjugated surfaces, (3) host–guest interactions, (4) peptides, and (5) DNA. We focus on recent studies that address key challenges in the field, providing mechanistic understanding, rational polymer design, important functionality, robustness, or unusual thermodynamic and kinetic properties.

Supramolecular Polymers in Aqueous Media

From Cascaded Catalytic Nucleic Acids to Enzyme–DNA Nanostructures: Controlling Reactivity, Sensing, Logic Operations, and Assembly of Complex Structures

A series of exciting phenomena that can occur in supramolecular systems away from equilibrium are reviewed. 

Systems chemistry

Effects of mutations in de novo designed synthetic amphiphilic β-sheet peptides on self-assembly of fibrils.

Patterning of nanoparticles on solid substrates is one of the main challenges of current nanotechnology applications. The use of organic molecules as templates for the deposition of the nanoparticles makes it possible to utilize simple soft lithography techniques for patterning. Peptides appear to be powerful candidates for this job due to their versatility and design flexibility. In this work, we demonstrate the use of dual-affinity peptides, which bind both to the substrate and to the deposited nanoparticles, as single-layer linkers for the creation of multi-component nanoparticle patterns via microcontact printing processes. Controlled deposition and patterning of gold colloids or carbon nanotubes (CNTs) on silicon oxide surfaces and that of silicon oxide nanoparticles on gold surfaces have been achieved by the use of the corresponding dual-affinity peptides. Furthermore, patterning of both gold colloids and CNTs on a single substrate on predefined locations has been achieved. The suggested generic approach offers great flexibility by allowing binding of any material to a substrate of choice, provided that a peptide binding segment has been engineered for each of the inorganic components. Furthermore, the diversity of possible peptide sequences allows the formation of multi-component patterns, paving the way to fabricating complex functional structures based on peptide templates.

https://iopscience.iop.org/article/10.1088/0957-4484/21/14/145305/pdf

Bioassisted multi-nanoparticle patterning using single-layer peptide templates.

Most self-replicating peptide systems are made of α-helix forming sequences. However, it has been postulated that shorter and simpler peptides may also serve as templates for replication when arranged into well-defined structures. We describe here the design and characterization of new peptides that form soluble β-sheet aggregates that serve to significantly accelerate their ligation and self-replication. We then discuss the relevance of these phenomena to early molecular evolution, in light of additional functionality associated with β-sheet assemblies.

Self-assembly and Self-replication of Short Amphiphilic β-sheet Peptides

This study addresses the question of whether chemically deposited PbS thin films grown on GaAs(111) are affected by the oppositely terminated substrate surfaces, gallium terminated GaAs(111)A and arsenic terminated GaAs(111)B. The differences in PbS film deposition pathway in both cases of substrate surface termination were investigated using X-ray photoelectron spectroscopy (XPS), Raman scattering, and contact potential difference (CPD) measurements. The morphology, microstructure, and crystallographic orientation of the films were studied using scanning electron microscopy, X-ray diffraction, and transmission electron microscopy. XPS and CPD measurements indicated that PbS films deposited on oppositely terminated GaAs(111) surfaces possessed corresponding surface terminations, with PbS(111)B obtained on GaAs(111)B and PbS(111)A on GaAs(111)A. Subsequently, different surface oxides were detected by XPS on A and B terminated PbS(111), with lead oxide obtained on PbS(111)A and PbSO3 obtained on PbS(111)B. ...

Surface Termination Control in Chemically Deposited PbS Films: Nucleation and Growth on GaAs(111)A and GaAs(111)B

The unique properties of peptides have led to their use in diverse applications in medicine and nanotechnology. In order to demonstrate their utility as multifunctional, selective, adhesion layers in electronic devices, we demonstrate here peptide mediated synthesis approach for the formation of continuous gold films on a silicon–oxide substrate. This is done using a dual affinity peptide (DAP), engineered to specifically bind to the substrate at one end, and nucleate the growth of gold at the other end. The resulting film is comprised of disk shaped crystalline gold nanoparticles (NPs) with a ratio of 3–4 gold atoms per peptide. Charge transfer between the NPs and the peptide results in positive charging of the NPs, with about 23% of the gold atoms, presumably located at the surface of the NPs, interacting strongly with the peptide side chains. The resistance of the film decreases during its growth, reaching a value of 14 kΩ □−1 upon the formation of a continuous film. Finally the ability to define pattern of the films on the surface is demonstrated using the peptide as an ink in a micro-contact printing process for the formation of a template pattern on which the gold film is grown. Taking into account the diversity of peptides that can be designed this work demonstrates the promises of the use of DAPs as adhesive templates in the fabrication of devices for diverse applications.

Peptide directed growth of gold films

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