Excitonic and vibrational coherence in artificial photosynthetic systems studied by negative-time ultrafast laser spectroscopy
文献情報
Dongjia Han, Bing Xue, Juan Du, Tomohiro Miyatake, Hitoshi Tamiaki, Xin Xing, Wei Yuan, Yanyan Li
Quantum coherences between excitonic states are believed to have a substantial impact on excitation energy transfer in photosynthetic systems. Here, the excitonic and vibrational coherence relaxation dynamics of artificially synthetic chlorosomes are studied by a sub 7 fs negative-time-delay laser spectroscopy at room temperature. The results provide direct evidence for the quantum coherence of the excitonic dephasing time of 23 ± 1 fs at physiologically relevant temperatures, which is significant in the initial step of energy transfer in chlorosome or chlorosome-like photosynthetic systems. Meanwhile, coherent molecular vibrations in the excited state are also detected without the effect of wave-packet motion in the ground state, which shows that the excited state wave-packet motion contributes greatly to the vibrational modes of ∼150 and ∼1340 cm−1 in artificial chlorosome systems.
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