Solvent independent symmetry-breaking charge separation in terrylenediimide guanine-quadruplex nanoparticles [electronic resource]
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| Format: | Government Document Electronic eBook |
| Language: | English |
| Published: |
Washington, D.C. : Oak Ridge, Tenn. :
United States. Department of Energy. Office of Science ; Distributed by the Office of Scientific and Technical Information, U.S. Department of Energy,
2020.
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| Abstract: | G-quadruplex assemblies are a promising tool for self-assembling ?-stacked chromophore arrays to better understand their photophysics. We have shown that coupling a single guanine moiety to terrylenediimide (TDI) produces a structure (GTDI) that self-assembles in tetrahydrofuran (THF) into a nearly monodisperse guanine-quadruplex structure having 16 ?-stacked layers (GTDI<sub>4</sub>)<sub>16</sub>. The TDI surfaces were determined to have a high degree of cofacial overlap and underwent quantitative symmetry-breaking charge separation (SB-CS) upon photoexcitation. Here, we more deeply examine the relationship between solvent and aggregate formation and develop insights into structure?function relationships over a variety of solvent polarities and hydrogen-bonding capabilities. At high concentrations, GTDI assembles into guanine-quadruplex structures (GTDI<sub>4</sub>)<sub>16</sub> in THF and toluene, as well as (GTDI<sub>4</sub>)<sub>9</sub> in pyridine and benzonitrile. Here, transient absorption spectroscopy shows that SB-CS occurs in all solvents, regardless of their static dielectric constants, but the SB-CS yield is determined by structure. Solvent polarity independent SB-CS generation is also observed in GTDI films, where there is a complete absence of solvent. |
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| Item Description: | Published through Scitech Connect. 11/28/2020. "Journal ID: ISSN 0021-9606." "Other: 168681." ": US2212344." Powers-Riggs, Natalia E. ; Zuo, Xiaobing ; Young, Ryan M. ; Wasielewski, Michael R. ; NSF Graduate Research Fellowship. |
| Physical Description: | Size: Article No. 204302 : digital, PDF file. |