共 91 条
Efficient light harvesting in dye-endcapped conjugated polymers probed by single molecule spectroscopy
被引:76
作者:

Becker, Klaus
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Univ Munich, Phys Dept, Photon & Optoelect Grp, D-80799 Munich, Germany Univ Munich, Phys Dept, Photon & Optoelect Grp, D-80799 Munich, Germany

Lupton, John M.
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Univ Munich, Phys Dept, Photon & Optoelect Grp, D-80799 Munich, Germany Univ Munich, Phys Dept, Photon & Optoelect Grp, D-80799 Munich, Germany
机构:
[1] Univ Munich, Phys Dept, Photon & Optoelect Grp, D-80799 Munich, Germany
关键词:
D O I:
10.1021/ja0609405
中图分类号:
O6 [化学];
学科分类号:
0703 ;
摘要:
The development of sophisticated microscopic models of energy transfer in linear multichromophoric systems such as conjugated polymers is rarely matched by suitable experimental studies on the microscopic level. To assess the roles of structural, temporal, and energetic disorder in energy transfer, single molecule spectroscopic investigations of the elementary processes leading to energetic relaxation in conjugated polymers are desirable. We present a detailed study of energy transfer processes occurring in dye-endcapped conjugated polymer molecules on the single molecule level. These processes are mostly masked in ensemble investigations. Highly efficient intramolecular energy transfer along a single polyindenofluorene chain to a perylene endcap occurs in many instances and is resolved in real time. We further consider the spectral emission characteristics of the single molecule, the polarization anisotropy which reveals the chain conformation, the fluorescence intermittency, and the temperature dependence and conclude that the efficiency of energy transfer in the ensemble is controlled by the statistics of the individual molecules. The weak thermal activation of energy transfer indicates the involvement of vibrational modes in interchromophoric coupling. Whereas backbone-endcap coupling is strong, the rate-limiting step for intramolecular energy transfer is the migration along the backbone. The results are particularly relevant to understanding undesired exciton trapping on fluorenone defects in polyfluorenes.
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页码:6468 / 6479
页数:12
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