Two‐Dimensional Excitonic Networks Directed by DNA Templates as an Efficient Model Light‐Harvesting and Energy Transfer System

Abstract

Photosynthetic organisms organize discrete light-harvesting complexes into large-scale networks to facilitate efficient light collection and utilization. Inspired by nature, herein, synthetic DNA templates were used to direct the formation of dye aggregates with a cyanine dye, K21, into discrete branched photonic complexes, and two-dimensional (2D) excitonic networks. The DNA templates ranged from four-arm DNA tiles, � 10 nm in each arm, to 2D wireframe DNA origami nanostructures with different geometries and varying dimensions up to 100 × 100 nm. These DNAtemplated dye aggregates presented strongly coupled spectral features and delocalized exciton characteristics, enabling efficient photon collection and energy transfer. Compared to the discrete branched photonic systems templated on individual DNA tiles, the interconnected excitonic networks showed approximately a 2-fold increase in energy transfer efficiency. This bottom-up assembly strategy paves the way to create 2D excitonic systems with complex geometries and engineered energy pathways.

Lab-on-a-DNA origami: nanoengineered single-molecule platforms

“…32 More recently, DNA origami was used to create excitonic wires and networks. 22,33 DNA origami allows precise control over the geometric arrangement and energy flow through photonic materials. The DNA double helix was used to guide the assembly of the cyanine dye K21, which forms a closedpacked aggregate exhibiting strong excitonic coupling between chromophores, Fig.…”

“…33 The same strategy was used to create 2D wireframe DNA origami nanostructures for multiple excitation energy transfer pathways increasing the light collection efficiency, decreasing possible failures, and enabling a more robust and resilient system. 22 Due to the relatively straightforward chemical functionalization of DNA, energy and charge transfer between short polymers were also already studied. For example, Wang et al 35 modified DNA frames with polyaniline and poly(phenylenevinylene), which would reversibly change a fluorescence signal output upon a redox reconfiguration.…”

“… 33 The same strategy was used to create 2D wireframe DNA origami nanostructures for multiple excitation energy transfer pathways increasing the light collection efficiency, decreasing possible failures, and enabling a more robust and resilient system. 22 …”

Multifunctional Exo III-assisted scalability strategy for constructing DNA molecular logic circuits

“…1,2 Based on the principle of complementary base pairing, DNA molecules are being used in frontier areas such as neural networks, 3,4 information encryption 5,6 disease detection 7,8 and DNA storage. [9][10][11] With great potential for information transfer and processing, DNA molecules enable molecular logic circuits, [12][13][14] tiles, [15][16][17] walker machines, [18][19][20] and protein interaction. 21 Molecular logic circuits are circuits that perform basic logic operations, and they are often used to implement functions such as parity checking, 22,23 logic computations, 24,25 drug delivery 26,27 and biosensing.…”

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

“…Our findings may provide a strategy for guiding the self-assembly of DNA strands into one particular structure when there are multiple potential structures. In the applied side, the high resolution of the DNA crystals may allow structural studies of small guest molecules that can be incorporated into the DNA crystal lattices, or organize molecules in 3D with Å level precision for other applications, such as photonic devices, cascade catalysis, − and information processing and storages. − …”