Does Coherence Enhance Transport in Photosynthesis?
Does Coherence Enhance Transport in Photosynthesis?
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DOI：
10.1021/jz301872b
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发表时间：
2013-02-07
影响因子：
5.7
通讯作者：
Rahimi-Keshari, Saleh
中科院分区：
文献类型：
--
作者：
Kassal, Ivan;Yuen-Zhou, Joel;Rahimi-Keshari, Saleh
最近在光合复合物的相干性的观察导致了量子效应是否可以在体内发生的问题，而不是在飞秒激光脉冲，但在非相干的阳光和稳定状态下，如果是这样的话，相干性是否解释了高激子传输效率。我们介绍了状态相干性和过程相干性之间的区别，并表明尽管一些光合作用途径是部分相干过程，但自然界中的光合作用是通过稳态进行的。这种区别使我们能够排除几种机制的运输增强阳光。特别是，尽管它们对于理解激子输运是至关重要的，但无论是波状运动还是微观相干性，本身都不能提高效率。相比之下，两种部分连贯的机制--ENAQT和超级转移--即使在阳光下也可以增强传输，从而构成优化人工阳光收集的主题。最后，我们阐明了超快光谱学在理解非相干过程中的重要性。
Recent observations of coherence in photosynthetic complexes have led to the question of whether quantum effects can occur in vivo, not under femtosecond laser pulses but in incoherent sunlight and at steady state, and, if so, whether the coherence explains the high exciton transfer efficiency. We introduce the distinction between state coherence and process coherence and show that although some photosynthetic pathways are partially coherent processes, photosynthesis in nature proceeds through stationary states. This distinction allows us to rule out several mechanisms of transport enhancement in sunlight. In particular, although they are crucial for understanding exciton transport, neither wavelike motion nor microscopic coherence, on their own, enhance the efficiency. By contrast, two partially coherent mechanisms-ENAQT and supertransfer-can enhance transport even in sunlight and thus constitute motifs for the optimization of artificial sunlight harvesting. Finally, we clarify the importance of ultrafast spectroscopy in understanding incoherent processes.