Smyth Cathal, Oblinsky Daniel G, Scholes Gregory D
Department of Physics, University of Toronto, Toronto, Canada.
Department of Chemistry, Princeton University, Washington Rd, Princeton, NJ 08544, USA.
Phys Chem Chem Phys. 2015 Dec 14;17(46):30805-16. doi: 10.1039/c5cp00295h.
Until recently, no analytical measure of many-body delocalization in open systems had been developed, yet such a measure enables characterization of how molecular excitons delocalize in photosynthetic light-harvesting complexes, and in turn helps us understand quantum coherent aspects of electronic energy transfer. In this paper we apply these measures to a model peripheral light-harvesting complex, LH2 from Rhodopseudomonas acidophila. We find how many chromophores collectively contribute to the "delocalization length" of an excitation within LH2 and how the coherent delocalization is distributed spatially. We also investigate to what extent this delocalization length is effective, by examining the impact of bipartite and multipartite entanglement in inter-ring energy transfer in LH2.
直到最近,还没有开发出用于开放系统中多体离域的分析方法,然而这样一种方法能够表征分子激子在光合捕光复合物中如何离域,进而帮助我们理解电子能量转移的量子相干方面。在本文中,我们将这些方法应用于一个模型外周捕光复合物,即嗜酸红假单胞菌的LH2。我们发现有多少发色团共同对LH2内激发的“离域长度”做出贡献,以及相干离域在空间上是如何分布的。我们还通过研究LH2中环间能量转移中的二分和多分纠缠的影响,来探究这种离域长度在多大程度上是有效的。