4.8 Article

New Insights into the Mechanism of Uphill Excitation Energy Transfer from Core Antenna to Reaction Center in Purple Photosynthetic Bacteria

期刊

JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 9, 期 12, 页码 3278-3284

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.8b01197

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资金

  1. Natural Science Foundation of China (NSFC) [21673288]
  2. JSPS KAKENHI [JP16H04174]
  3. JSPS Research Fellowship

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The uphill excitation energy transfer (EET) from the core antenna (LH1) to the reaction center (RC) of purple photosynthetic bacteria was investigated at room temperature by comparing the native LH1-RC from Thermochromatium (Tch.) tepidum with the hybrid LH1-RC from a mutant strain of Rhodobacter (Rba.) sphaeroides. The latter protein with chimeric Tch-LH1 and Rba-RC exhibits a substantially larger RC-to-LH1 energy difference (Delta E = 630 cm(-1)) of 3-fold thermal energy (3k(B)T). The spectroscopic and kinetics results are discussed on the basis of the newly reported high-resolution structures of Tch. tepidum LH1-RC, which allow us to propose the existence of a passage formed by LH1 BChls that facilitates the LH1 -> RC EET. The semilogarithmic plot of the EET rate against Delta E was found to be linear over a broad range of Delta E, which consolidates the mechanism of thermal activation as promoted by the spectral overlap between the LH1 fluorescence and the special pair absorption of RC.

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