Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 9, Issue 8, Pages 1827-1832Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.8b00108
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Funding
- European Research Council (PHOTPROT) [267333]
- TOP-grant from Foundation of Chemical Science part of NWO [700.58.305]
- Netherlands Royal Academy of Sciences (KNAW)
- Biotechnology and Biological Sciences Research Council of the U.K. [BB/I022570/1]
- BBSRC [BB/I022570/1] Funding Source: UKRI
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Two-dimensional electronic spectroscopy was applied to a variant of the reaction center (RC) of purple bacterium Rhodobacter sphaeroides lacking the primary acceptor ubiquinone in order to understand the ultrafast separation and transfer of charge between the bacteriochlorin cofactors. For the first time, characteristic 2D spectra were obtained for the participating excited and charge-transfer states, and the electron-transfer cascade (including two different channels, the P* and B* channels) was fully mapped. By analyzing quantum beats using 2D frequency maps, excited-state vibrational modes at 153 and 33 cm(-1) were identified. We speculate that these modes couple to the charge separation (CS) process and collectively optimize the CS and are responsible for the superhigh efficiency.
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