Impact of Single-Point Mutations on the Excitonic Structure and Dynamics in a Fenna-Matthews-Olson Complex.

Impact of Single-Point Mutations on the Excitonic Structure and Dynamics in a Fenna-Matthews-Olson Complex.
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单点突变对 Fenna-Matthews-Olson 复合体激子结构和动力学的影响。

DOI:
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发表时间:
2018
影响因子:
5.7
通讯作者:
R. Jankowiak
R. Jankowiak
中科院分区:
化学2区
文献类型:
--
作者:
A. Khmelnitskiy;T. Reinot;R. Jankowiak

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烧孔 (HB) 光谱和建模研究揭示了温热绿杆菌 FMO 三聚体的几种突变体的激子结构和动力学的显着变化。当细菌叶绿素 (BChl) 1(V152N 突变体)或 BChl 6 (W184F) 附近发生突变时,高能激子的激发态衰减时间 (T1) 会显着改变。 V152N 和 W184F 突变体中最高能量激子的(平均)T1 时间较长,表明 BChls 1 和 6 的位点能量(据信在接收基板 BChls 的激发中发挥重要作用)可能在确保野生型 FMO 中观察到的飞秒(fs)能量弛豫中发挥关键作用。 HB 光谱优先显示较慢的 T1 时间(平均约 1 ps),因为 fs 时间由于极低的 HB 量子产率而禁止 HB。讨论了单体之间不相关(不相干)的激发能量转移时间、激子态的组成以及平均、频率相关的激发态衰减时间(T1)。
Hole burning (HB) spectroscopy and modeling studies reveal significant changes in the excitonic structure and dynamics in several mutants of the FMO trimer from the Chlorobaculum tepidum. The excited-state decay times ( T1) of the high-energy excitons are significantly modified when mutation occurs near bacteriochlorophyll (BChl) 1 (V152N mutant) or BChl 6 (W184F). Longer (averaged) T1 times of highest-energy excitons in V152N and W184F mutants suggest that site energies of BChls 1 and 6, believed to play an important role in receiving excitation from the baseplate BChls, likely play a critical role to ensure the femtosecond (fs) energy relaxation observed in wild-type FMO. HB spectroscopy reveals preferentially slower T1 times (about 1 ps on average) because fs times prohibit HB due to an extremely low HB quantum yield. Uncorrelated (incoherent) excitation energy transfer times between monomers, the composition of exciton states, and average, frequency-dependent, excited-state decay times ( T1) are discussed.
DOI: 10.1021/jz2007676
发表时间: 2011-06-30
期刊: The journal of physical chemistry letters
影响因子: --
作者:
Olbrich C;Strümpfer J;Schulten K;Kleinekathöfer U
通讯作者: Kleinekathöfer U
Fenna-Matthews-Olson 复合体的从头算光谱学。
DOI: 10.1021/jz402000c
发表时间: 2013
期刊: The journal of physical chemistry letters
影响因子: --
作者:
Cole DJ
通讯作者: Cole DJ
DOI: 10.1073/pnas.1702261114
发表时间: 2017-08-08
影响因子: 11.1
作者:
Duan, Hong-Guang;Prokhorenko, Valentyn I.;Miller, R. J. Dwayne
通讯作者: Miller, R. J. Dwayne