Feng Jin, Tseng Chi-Wei, Chen Tingwei, Leng Xia, Yin Huabing, Cheng Yuan-Chung, Rohlfing Michael, Ma Yuchen
School of Chemistry and Chemical Engineering, Shandong University, Jinan, 250100, China.
Department of Chemistry and Center for Quantum Science and Engineering, National Taiwan University, Taipei, 106, Taiwan.
Nat Commun. 2017 Jul 10;8(1):71. doi: 10.1038/s41467-017-00120-7.
It is unclear whether there is an intermediate dark state between the S and S states of carotenoids. Previous two-dimensional electronic spectroscopy measurements support its existence and its involvement in the energy transfer from carotenoids to chlorophylls, but there is still considerable debate on the origin of this dark state and how it regulates the energy transfer process. Here we use ab initio calculations on excited-state dynamics and simulated two-dimensional electronic spectrum of carotenoids from purple bacteria to provide evidence supporting that the dark state may be assigned to a new A state. Our calculations also indicate that groups on the conjugation backbone of carotenoids may substantially affect the excited-state levels and the energy transfer process. These results contribute to a better understanding of carotenoid excited states.Carotenoids harvest energy from light and transfer it to chlorophylls during photosynthesis. Here, Feng et al. perform ab initio calculations on excited-state dynamics and simulated 2D electronic spectrum of carotenoids, supporting the existence of a new excited state in carotenoids.
类胡萝卜素的S态和S态之间是否存在中间暗态尚不清楚。此前的二维电子光谱测量结果支持其存在以及它在从类胡萝卜素到叶绿素的能量转移中的作用，但关于这种暗态的起源以及它如何调节能量转移过程仍存在相当大的争议。在这里，我们对来自紫色细菌的类胡萝卜素的激发态动力学进行从头算计算，并模拟其二维电子光谱，以提供证据支持暗态可能被归为一种新的A态。我们的计算还表明，类胡萝卜素共轭主链上的基团可能会显著影响激发态能级和能量转移过程。这些结果有助于更好地理解类胡萝卜素的激发态。类胡萝卜素在光合作用过程中从光中获取能量并将其转移到叶绿素中。在这里，冯等人对类胡萝卜素的激发态动力学进行了从头算计算，并模拟了其二维电子光谱，支持了类胡萝卜素中一种新激发态的存在。
