The role of mixed vibronic Q(y)-Q(x) states in green light absorption of light-harvesting complex II.
The role of mixed vibronic Q(y)-Q(x) states in green light absorption of light-harvesting complex II.
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DOI：
10.1038/s41467-020-19800-y
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发表时间：
2020-11-26
影响因子：
16.6
通讯作者：
Fleming GR
中科院分区：
文献类型：
--
作者：
Arsenault EA;Yoneda Y;Iwai M;Niyogi KK;Fleming GR
长期以来，绿光对推动自然光合作用的重要性一直被低估，然而，在强光照下，绿光实际上比红光更有效地推动光合作用。这种绿光被由叶绿素(Chl)-Chl相互作用产生的混合振动Qy-Qx态所吸收，尽管对这些态几乎一无所知。本文采用偏振相关的二维电子振动光谱研究了光收集配合物II的混合振动Qy-Qx态的起源和动力学。我们证明了该区域的状态主要由Chl b产生，并证明了如何区分Qy与Qx特征的振动程度。我们发现主要是Chl b Qy和Chl b Qx特征的态的动力学是明显不同的，因为在Qx状态中激发持续的时间明显更长，并且Qx动力学中存在振荡成分，这是讨论的。我们的研究结果证明了电子-核混合在有效光收集中的核心作用以及Chl a和Chl b的不同功能。太阳光谱的绿色成分可以有效地驱动自然光合作用，但由于所涉及的激发态的复杂性，这一过程很少被研究。在这里，作者利用偏振相关的二维电子振动光谱来定义光捕获复合物II中这些状态的起源和动力学。
The importance of green light for driving natural photosynthesis has long been underappreciated, however, under the presence of strong illumination, green light actually drives photosynthesis more efficiently than red light. This green light is absorbed by mixed vibronic Qy-Qx states, arising from chlorophyll (Chl)-Chl interactions, although almost nothing is known about these states. Here, we employ polarization-dependent two-dimensional electronic-vibrational spectroscopy to study the origin and dynamics of the mixed vibronic Qy-Qx states of light-harvesting complex II. We show the states in this region dominantly arise from Chl b and demonstrate how it is possible to distinguish between the degree of vibronic Qy versus Qx character. We find that the dynamics for states of predominately Chl b Qy versus Chl b Qx character are markedly different, as excitation persists for significantly longer in the Qx states and there is an oscillatory component to the Qx dynamics, which is discussed. Our findings demonstrate the central role of electronic-nuclear mixing in efficient light-harvesting and the different functionalities of Chl a and Chl b. The green component of the solar spectrum can efficiently drive natural photosynthesis, but the process has been little investigated due to the complexity of the excited states involved. Here the authors utilize polarization-dependent two-dimensional electronic-vibrational spectroscopy to define the origin and dynamics of these states in light-harvesting complex II.
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影响因子：
3.3
作者：
Agarwal, R;Krueger, BP;Fleming, GR
通讯作者：
Fleming, GR
影响因子：
7.4
作者：
Blankenship, Robert E.
通讯作者：
Blankenship, Robert E.
影响因子：
3.7
作者：
GARLASCHI, FM;ZUCCHELLI, G;JENNINGS, RC
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3.3
作者：
Novoderezhkin, VI;Palacios, MA;van Grondelle, R
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van Grondelle, R
影响因子：
1.4
作者：
GOUTERMAN, M
通讯作者：
GOUTERMAN, M