Fluorescence Dynamics of Chlorophyll Trefoils in the Solid State Studied by Single-Molecule Fluorescence Spectroscopy

被引:31
作者
Lee, Ji-Eun [3 ,4 ]
Yang, Jaesung [3 ,4 ]
Gunderson, Victoria L. [1 ,2 ]
Wasielewski, Michael R. [1 ,2 ]
Kim, Dongho [3 ,4 ]
机构
[1] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
[2] Northwestern Univ, Argonne NW Solar Energy Res Ctr, Evanston, IL 60208 USA
[3] Yonsei Univ, Spect Lab Funct Elect Syst, Seoul 120749, South Korea
[4] Yonsei Univ, Dept Chem, Seoul 120749, South Korea
关键词
ENERGY MIGRATION PROCESSES; CYCLIC PORPHYRIN ARRAYS; ELECTRON-TRANSFER; MULTICHROMOPHORIC DENDRIMERS; PHOTOPHYSICAL PROPERTIES; LINKED PORPHYRIN; CHARGE-TRANSFER; DIMERS; LEVEL;
D O I
10.1021/jz900193c
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
We have comparatively investigated the single-molecule-photophysical properties of two chlorophyll trefoils that feature distinctive electronic couplings induced by differences in linkage: one is an ethynyl-linked chlorophyll trefoil (1) in which relatively short and rigid linkage between the chromophores promotes effective electronic coupling, and the other is a phenyl ethynyl-linked chlorophyll trefoil (2) in which the phenyl addition induces an orthogonal geometry impeding pi-conjugation and provides a longer interchlorophyll distance reducing through space interaction. By recording single molecule fluorescence intensity trajectories and their corresponding lifetimes, we observed one-step photobleaching behaviors, less frequent on off behaviors, a narrower fluorescence lifetime distribution, and higher photostability in 1 as compared with 2. These results indicate that the performance of molecular photosynthetic systems in the solid state is strongly associated with electronic couplings and; thus, give insight into the construction of well-functioning artificial photosynthetic systems.
引用
收藏
页码:284 / 289
页数:6
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