Abstract
The transfer of electronic charge in the reaction center of Photosystem II is one of the key building blocks of the conversion of sunlight energy into chemical energy within the cascade of the photosynthetic reactions. Since the charge transfer dynamics is mixed with the energy transfer dynamics, an effective tool for the direct resolution of charge separation in the reaction center is still missing. Here, we use experimental two-dimensional optical photon echo spectroscopy in combination with the theoretical calculation to resolve its signature. A global fitting analysis allows us to clearly and directly identify a decay pathway associated to the primary charge separation. In particular, it can be distinguished from regular energy transfer and occurs on a time scale of 1.5 ps under ambient conditions. This technique provides a general tool to identify charge separation signatures from the energy transport in two-dimensional optical spectroscopy.
| Original language | English |
|---|---|
| Article number | 12347 |
| Journal | Scientific Reports |
| Volume | 7 |
| Issue number | 1 |
| DOIs | |
| Publication status | Published - 1 Dec 2017 |
Funding
We thank Sumithra Kannan for her help with the purification at the early stage of this project. We acknowledge financial support by the Max Planck Society and the Hamburg Centre for Ultrafast Imaging (CUI) within the German Excellence Initiative supported by the Deutsche Forschungsgemeinschaft. H-G.D. acknowledges generous financial support by the Joachim-Hertz-Stiftung Hamburg. R.C. and E.W. supported by the Netherlands Organization for Scientific Research (NWO), life and Earth Science division (ALW) via a Vici grant to R.C.
| Funders | Funder number |
|---|---|
| CUI | |
| Hamburg Centre for Ultrafast Imaging | |
| Joachim-Hertz-Stiftung Hamburg | |
| Earth Sciences Division | |
| Deutsche Forschungsgemeinschaft | |
| Nederlandse Organisatie voor Wetenschappelijk Onderzoek | |
| Max-Planck-Gesellschaft |
