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Impact of Single-Point Mutations on the Excitonic Structure and Dynamics in a Fenna–Matthews–Olson Complex
The Journal of Physical Chemistry Letters ( IF 5.7 ) Pub Date : 2018-06-04 00:00:00 , DOI: 10.1021/acs.jpclett.8b01396
Anton Khmelnitskiy , Tonu Reinot , Ryszard Jankowiak

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.

中文翻译:

单点突变对芬娜-马修斯-奥尔森复合体的激子结构和动力学的影响

孔燃烧(HB)光谱学和模型研究表明,来自温热Chlorobaculum pidpidum的FMO三聚体的几个突变体的激子结构和动力学发生了显着变化当突变发生在细菌叶绿素(BChl)1(V152N突变体)或BChl 6(W184F)附近时,高能激子的激发态衰减时间(T 1)会显着改变。V152N和W184F突变体中最高能量激子的更长(平均)T 1倍更长,这表明BChls 1和6的位点能量被认为在接受基板BChls的激发中起重要作用,可能对确保飞秒起关键作用。 (fs)在野生型FMO中观察到的能量松弛。HB光谱显示T优先慢1倍(平均约1 ps),因为fs时间由于HB量子产率极低而禁止HB。讨论了单体之间不相关(不相干)的激发能传递时间,激子态的组成以及平均,频率相关的激发态衰减时间(T 1)。
更新日期:2018-06-04
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