Tempelaar Roel, Jansen Thomas L C, Knoester Jasper
Zernike Institute for Advanced Materials, University of Groningen , Nijenborgh 4, 9747 AG Groningen, The Netherlands.
J Phys Chem B. 2014 Nov 13;118(45):12865-72. doi: 10.1021/jp510074q. Epub 2014 Nov 3.
In biological light harvesting, solar energy is captured by photosynthetic antennae for subsequent storage into chemical bonds. The remarkable efficiency reached in transferring the energy between the collection and storage events recently has been attributed to long-lived electronic coherence present in such antennae systems. We present numerical simulations indicating that the spectroscopic transients that supported this hypothesis are not induced by electronic coherence but instead are caused by vibrational (nuclear) motion in the electronic ground state potential. Besides emphasizing the significance of such nuclear modes, our findings stimulate a reconsideration of the role of electronic coherence in promoting energy transfer in natural photosynthesis. Furthermore, they require us to rethink how energy transfer efficiency is reflected in spectral signals.
在生物光捕获过程中,太阳能被光合天线捕获,随后存储到化学键中。近来,在能量收集与存储过程之间传递能量所达到的卓越效率,被归因于此类天线系统中存在的长寿命电子相干性。我们给出的数值模拟表明,支持这一假设的光谱瞬态并非由电子相干性引起,而是由电子基态势能中的振动(核)运动导致。除了强调此类核模式的重要性之外,我们的发现促使人们重新思考电子相干性在促进自然光合作用中能量传递方面的作用。此外,这些发现要求我们重新思考能量传递效率如何在光谱信号中体现。