期刊
COMMUNICATIONS CHEMISTRY
卷 4, 期 1, 页码 -出版社
NATURE PORTFOLIO
DOI: 10.1038/s42004-021-00456-8
关键词
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资金
- U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Division of Materials Science and Engineering through the Established Program to Stimulate Competitive Research (EPSCoR) [DE-SC0020089]
- Department of the Navy, Office of Naval Research (ONR) under ONR [N00014-19-1-2615]
- Institutional Development Awards (IDeA) from the National Institute of General Medical Sciences [P20GM103408]
- National Institutes of Health [P20GM109095]
- National Science Foundation [0619793, 0923535]
- MJ Murdock Charitable Trust
- Idaho State Board of Education
- National Science Foundation NSF MRI award [0923541]
- DOE, Idaho National Laboratory, Laboratory Directed Research and Development project [154754]
- Directorate For Engineering
- Div Of Electrical, Commun & Cyber Sys [0923541] Funding Source: National Science Foundation
Molecular excitons play a crucial role in various fields such as light harvesting and organic electronics, with their structure and dynamics being influenced by molecular packing. The addition of rotaxane rings to squaraine dyes templated with DNA can result in an oblique packing arrangement with improved optical properties. This method may be beneficial for optimizing excitonic materials for applications ranging from solar energy conversion to quantum information science.
Molecular excitons play a central role in natural and artificial light harvesting, organic electronics, and nanoscale computing. The structure and dynamics of molecular excitons, critical to each application, are sensitively governed by molecular packing. Deoxyribonucleic acid (DNA) templating is a powerful approach that enables controlled aggregation via sub-nanometer positioning of molecular dyes. However, finer sub-Angstrom control of dye packing is needed to tailor excitonic properties for specific applications. Here, we show that adding rotaxane rings to squaraine dyes templated with DNA promotes an elusive oblique packing arrangement with highly desirable optical properties. Specifically, dimers of these squaraine:rotaxanes exhibit an absorption spectrum with near-equal intensity excitonically split absorption bands. Theoretical analysis indicates that the transitions are mostly electronic in nature and only have similar intensities over a narrow range of packing angles. Compared with squaraine dimers, squaraine:rotaxane dimers also exhibit extended excited-state lifetimes and less structural heterogeneity. The approach proposed here may be generally useful for optimizing excitonic materials for a variety of applications ranging from solar energy conversion to quantum information science. DNA templating is a useful strategy to control the positioning and aggregation of molecular dyes on a sub-nanometer scale, but sub-angstrom control is desirable for the precise tailoring of excitonic properties. Here, the authors show that templating squaraine dyes functionalized with rotaxane rings promotes an elusive oblique packing arrangement and extended excited-state lifetimes.
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