期刊
CHEM
卷 7, 期 3, 页码 752-773出版社
CELL PRESS
DOI: 10.1016/j.chempr.2020.12.020
关键词
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资金
- US Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) [DE-SC001999]
- DOE, Office of Science, BES [DE-SC001999]
- National Science Foundation (NSF) RAISE TAQS [1839155]
- US Army Research Office [W911NF-19-2-0026]
- NSF RAISE TAQS [1839155]
- Office of Naval Research [N00014-17-1-2609, N00014-13-1-0664, N00014-15-1-2830]
- Swiss Nation Foundation [200020_188468]
- NSF Graduate Research Fellowship
- NSERC Postgraduate Scholarship
- Beckman Young Investigator award
- Sloan Research Fellowship in Chemistry
- CIFAR Global Scholar award
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1839155] Funding Source: National Science Foundation
This study introduces a DNA-based platform for constructing tunable excitonic systems, allowing independent control over the coupling among the chromophores and between the chromophores and the environment. It demonstrates that the coupling between the chromophores and the environment can enhance exciton transport efficiency, pointing towards the development of designer nanophotonic devices.
Control over excitons enables electronic energy to be harnessed and transported for light harvesting and molecular electronics. Such control requires nanoscale precision over the molecular components. Natural light-harvesting systems achieve this precision through sophisticated protein machinery, which is challenging to replicate synthetically. Here, we introduce a DNA-based platform that spatially organizes cyanine chromophores to construct tunable excitonic systems. We synthesized DNA-chromophore nanostructures and characterized them with ensemble ultrafast and single-molecule spectroscopy and structure-based modeling. This synthetic approach facilitated independent control over the coupling among the chromophores and between the chromophores and the environment. We demonstrated that the coupling between the chromophores and the environment could enhance exciton transport efficiency, highlighting the key role of the environment in driving exciton dynamics. Control over excitons, as reported here, offers a path toward the development of designer nanophotonic devices.
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