Programmable, hierarchical assembly of DNA nanostructures with precise organisation of functional components have been demonstrated previously with tiled assembly and DNA origami. However, building organised nanostructures with random oligonucleotide strands remains as an elusive problem. Herein, a simple and general strategy, in which nanoclusters of a fullerene derivative act as stapler motifs in bringing ordered nanoscale assembly of short oligonucleotide duplexes into micrometre-sized nanowires, is described. In this approach, the fullerene derivative, by virtue of its amphiphilic structure and unique hydrophobic-hydrophilic balance, pre-assembles to form 3-5 nm sized clusters in a mixture of DMSO-phosphate buffer, which further assists the assembly of DNA strands. The optimum cluster size, availability of DNA anchoring motifs and the nature of the DNA strands controls the structure of these nanomaterials. Furthermore, horizontal conductivity measurements through conductive AFM confirmed the charge transport properties of these nanowires. The current strategy could be employed to organise random DNA duplexes and tiles into functional nanostructures, and hence, open up new avenues in DNA nanotechnology.

Programmable DNA-guided self-assembly of nanoscale functional materials is of great interest in the context of nanofabrication or nanoelectronics. Attributed to its unique sequence programmability and precisely defined dimension, DNA has been used as a template for constructing ordered one-, two-, and three-dimensional architectures with organic, inorganic, and polymeric building blocks via various self-assembly strategies. Moreover, the accessible integration capability of DNA with diverse electronics-related materials propels the field of DNA-guided assemblies toward nanoelectronic applications. In this review, we outline the development in the area of DNA-guided assemblies that are constructed from carbon nanotubes, fullerenes, polymers, metals, metal oxides, and minerals using various strategies, with the focus on the bottom-up DNA-guided conducting, semiconducting, and insulating nanomaterials applied on nanoelectronics. We also review some bottom-up and top-down hybrid methods that precisely immobilize functional DNA-guided materials on substrates with high throughput. Finally, we describe the challenges in nanofabrication and potential applications of DNA-guided assemblies in nanoelectronics.

Living systems are categorically a kinetic state of matter that exhibits complex functions and emergent behaviors. By contrast, synthetic systems are relatively simple and are typically controlled by the thermodynamic parameters. To understand this inherent difference between the biological and synthetic systems, novel approaches are of vital importance. In this regard, we have designed a three-component molecular system (a triad) by conjugating an amino acid with two functional molecules (naphthalenediimide and pyrene), which facilitates kinetically controlled self-assemblies. Herein, we describe three different molecular aggregation states of triads (entitled State I, State II, and State III) and also the dynamic pathway complexities associated with their transformations from one state to another. By meticulously employing the triads of different molecular aggregation states and the stereochemical information of the amino acid, we report emergent behaviors termed “supramolecular speciation” and “supramolecular regulation”. Further, we present a hitherto unknown emergent property in a self-assembled state under the majority-rules experiment, which has been termed “super-nonlinearity”. This work provides novel insights into complex synthetic systems having unprecedented functions and properties. Such emergent behaviors of synthetic triads that involve an interplay among complex interactions may find relevance in the context of prebiotic chemical evolution.