Abstract
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.
| Original language | English |
|---|---|
| Pages (from-to) | 1827-1832 |
| Number of pages | 6 |
| Journal | Journal of Physical Chemistry Letters |
| Volume | 9 |
| Issue number | 8 |
| Early online date | 27 Mar 2018 |
| DOIs | |
| Publication status | Published - Apr 2018 |
Funding
F.M., E.R., and R.v.G. were supported by an Advanced Investigator grant from the European Research Council (No. 267333, PHOTPROT) and the TOP-grant (700.58.305) from the Foundation of Chemical Science part of NWO. R.v.G. gratefully acknowledges his Academy Professor grant from The Netherlands Royal Academy of Sciences (KNAW). M.R.J acknowledges support from the Biotechnology and Biological Sciences Research Council of the U.K. (Project BB/I022570/ 1).
| Funders | Funder number |
|---|---|
| Foundation of Chemical Science | |
| Koninklijke Nederlandse Akademie van Wetenschappen (KNAW) | |
| Seventh Framework Programme | 267333 |
| Biotechnology and Biological Sciences Research Council | BB/I022570/ 1 |
| European Research Council | 700.58.305 |
| Koninklijke Nederlandse Akademie van Wetenschappen (KNAW) | |
| Nederlandse Organisatie voor Wetenschappelijk Onderzoek |
