期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 141, 期 44, 页码 17512-17516出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b10108
关键词
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资金
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-FG02-99ER14999]
- NSF [DGE-1324585]
- DOE Office of Science, Argonne National Laboratory [DE-AC02-06CH11357]
Guanine-quadruplex (G-quadruplex) assemblies provide a useful platform for studying the spatial, structural, and photophysical effects of intermolecular interactions. Coupling a single guanine moiety to terrylenediimide (TDI)-a chromophore with a large extended pi-surface-produces a structure (GTDI) that assembles in plate-like tetramers, with the potential of undergoing tunable pi-stacking. At high concentrations (3 x 10(-3) M), GTDI self-assembles into a nearly monodisperse G-quadruplex structure of 16 layers, with strong p-overlap between TDI moieties, observed by small- and wide-angle X-ray scattering. Transient absorption spectroscopy reveals that excitation of TDI in the G-quadruplex results in symmetry-breaking charge separation to form ion pairs within the structure, owing to the strong pi-overlap enforced by the hydrogen-bonding. These assemblies yield important insights into the interplay of noncovalent interactions in the assembly of ordered chromophoric arrays.
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