Department of Chemistry and The James Franck Institute, The University of Chicago, Chicago, Illinois 60637, USA.
J Chem Phys. 2012 Aug 21;137(7):074117. doi: 10.1063/1.4746244.
Research into the efficiency of photosynthetic light harvesting has focused on two factors: (1) entanglement of chromophores, and (2) environmental noise. While chromophores are conjugated π-bonding molecules with strongly correlated electrons, previous models have treated this correlation implicitly without a mathematical variable to gauge correlation-enhanced efficiency. Here we generalize the single-electron/exciton models to a multi-electron/exciton model that explicitly shows the effects of enhanced electron correlation within chromophores on the efficiency of energy transfer. The model provides more detailed insight into the interplay of electron correlation within chromophores and electron entanglement between chromophores. Exploiting this interplay is assisting in the design of new energy-efficient materials, which are just beginning to emerge.
（1）发色团的纠缠，以及（2）环境噪声。虽然发色团是具有强烈相关电子的共轭π键分子，但以前的模型都是隐含地处理这种相关性，而没有用数学变量来衡量相关增强的效率。在这里，我们将单电子/激子模型推广到多电子/激子模型，该模型明确显示了发色团内增强的电子相关对能量转移效率的影响。该模型更详细地揭示了发色团内电子相关和发色团间电子纠缠的相互作用。利用这种相互作用有助于设计新的节能材料，这些材料才刚刚开始出现。
