DNA-templated programmable excitonic wires for micron-scale exciton transport

Zhou, Xu; Líu, Hao; Djutanta, Franky; Satyabola, Deeksha; Jiang, Shuoxing; Qi, Xiaodong; Yu, Lu; Lin, Su; Hariadi, Rizal F.; Liu, Yan; Woodbury, Neal W.; Yan, Hao

doi:10.1016/j.chempr.2022.05.017

Cited by 17 publications

(26 citation statements)

References 60 publications

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“…This long-range energy transfer along fluorophore chains emulated the natural process of light harvesting, in which the photon energy absorbed by pigments in the light-harvesting complexes is transferred to the reaction center. To mimic the well-controlled multi-chromophore complexes organized on protein scaffolds for light harvesting and energy transfer, Zhou et al reported a bioinspired excitonic system templated by DNA origami to enable the long-range exciton migration (see Figure C) . A four-helix-bundle DNA origami of 600 nm in length was used to assemble K21 dye aggregates.…”

Section: Dna-origami-enabled Nanophotonicsmentioning

confidence: 99%

Section: Dna-origami-enabled Nanophotonicsmentioning

confidence: 99%

“…To mimic the well-controlled multi-chromophore complexes organized on protein scaffolds for light harvesting and energy transfer, Zhou et al reported a bioinspired excitonic system templated by DNA origami to enable the long-range exciton migration (see Figure 31C). 491 A four-helix-bundle DNA origami of 600 nm in length was used to assemble K21 dye aggregates. These excitonic wires were coupled with energy donors and acceptors to achieve directional excitation transfer over submicron distances.…”

Section: Nanoscale Distance Control By Dna Origamimentioning

confidence: 99%

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Recent Advances in DNA Origami-Engineered Nanomaterials and Applications

et al. 2023

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DNA nanotechnology is a unique field, where physics, chemistry, biology, mathematics, engineering, and materials science can elegantly converge. Since the original proposal of Nadrian Seeman, significant advances have been achieved in the past four decades. During this glory time, the DNA origami technique developed by Paul Rothemund further pushed the field forward with a vigorous momentum, fostering a plethora of concepts, models, methodologies, and applications that were not thought of before. This review focuses on the recent progress in DNA origami-engineered nanomaterials in the past five years, outlining the exciting achievements as well as the unexplored research avenues. We believe that the spirit and assets that Seeman left for scientists will continue to bring interdisciplinary innovations and useful applications to this field in the next decade.

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Section: Dna-origami-enabled Nanophotonicsmentioning

confidence: 99%

Section: Dna-origami-enabled Nanophotonicsmentioning

confidence: 99%

Section: Nanoscale Distance Control By Dna Origamimentioning

confidence: 99%

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Recent Advances in DNA Origami-Engineered Nanomaterials and Applications

et al. 2023

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“…DNA nanotechnology [11] offers a high level of flexibility to engineer these synthetic templates with programmable dimensions, shapes, and geometries, as well as chemical addressability, to direct the assembly of excitonic wires [10d, 12] and simple circuits [10b] . For example, DNA origami‐based one‐dimensional (1D) bundles have been shown to act as templates in the formation of strongly coupled aggregates of the cyanine dye, K21, which mediates efficient energy transfer along a defined 1D track up to 500 nm [10h] …”

Section: Introductionmentioning

confidence: 99%

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

et al. 2022

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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.

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“…In turn, this lack of control has limited the efficiency and reproducibility of experiments and applications. For example, a variety of photonic wires and 3D molecular networks have been assembled in DNA origami to gather and transmit photonic energy, [21][22][23]27,41 but their efficiency is never going to match the natural light harvesting complexes without control over the orientation of the composing molecules. Several strategies to incorporate small molecules in a DNA origami have been explored, with most of the work carried out with organic fluorophores.…”

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confidence: 99%

DNA Self-Assembly of Single Molecules with Deterministic Position and Orientation

et al. 2022

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An ideal nanofabrication method should allow the organization of nanoparticles and molecules with nanometric positional precision, stoichiometric control, and well-defined orientation. The DNA origami technique has evolved into a highly versatile bottom-up nanofabrication methodology that fulfils almost all of these features. It enables the nanometric positioning of molecules and nanoparticles with stoichiometric control, and even the orientation of asymmetrical nanoparticles along predefined directions. However, orienting individual molecules has been a standing challenge. Here, we show how single molecules, namely, Cy5 and Cy3 fluorophores, can be incorporated in a DNA origami with controlled orientation by doubly linking them to oligonucleotide strands that are hybridized while leaving unpaired bases in the scaffold. Increasing the number of bases unpaired induces a stretching of the fluorophore linkers, reducing its mobility freedom, and leaves more space for the fluorophore to accommodate and find different sites for interaction with the DNA. Particularly, we explore the effects of leaving 0, 2, 4, 6, and 8 bases unpaired and find extreme orientations for 0 and 8 unpaired bases, corresponding to the molecules being perpendicular and parallel to the DNA double-helix, respectively. We foresee that these results will expand the application field of DNA origami toward the fabrication of nanodevices involving a wide range of orientation-dependent molecular interactions, such as energy transfer, intermolecular electron transport, catalysis, exciton delocalization, or the electromagnetic coupling of a molecule to specific resonant nanoantenna modes.

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DNA-templated programmable excitonic wires for micron-scale exciton transport

Cited by 17 publications

References 60 publications

Recent Advances in DNA Origami-Engineered Nanomaterials and Applications

Recent Advances in DNA Origami-Engineered Nanomaterials and Applications

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

DNA Self-Assembly of Single Molecules with Deterministic Position and Orientation

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