期刊
ACS NANO
卷 10, 期 6, 页码 5933-5940出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.6b01265
关键词
porphyrin nanoring; biomimetics; ultrafast spectroscopy; energy transfer
类别
资金
- European Research Council [320969]
- EPSRC
- Royal Thai Government Scholarship
- Engineering and Physical Sciences Research Council [EP/M016110/1, EP/J007161/1] Funding Source: researchfish
- EPSRC [EP/J007161/1, EP/M016110/1] Funding Source: UKRI
Supramolecular antenna-ring complexes are of great interest due to their presence in natural light harvesting complexes. While such systems are known to provide benefits through robust and efficient energy funneling, the relationship between molecular structure, strain (governed by nuclear coordinates and motion), and energy dynamics (arising from electronic behavior) is highly complex. We present a synthetic antenna-nanoring system based on a series of conjugated porphyrin chromophores ideally suited to explore such effects. By systematically varying the size of the acceptor nanoring, we reveal the interplay between antenna-nanoring binding, local strain, and energy dynamics on the picosecond time scale. Binding of the antenna unit creates a local strain in the nanoring, and this strain was measured as a function of the size of the nanoring, by UV vis-NIR titration, providing information on the conformational flexibility of the system. Strikingly, the energy-transfer rate is independent of nanoring size, indicating the existence of strain-localized acceptor states, spread over about six porphyrin units, arising from the noncovalent antenna-nanoring association.
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