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The energy conversion of oxygenic photosynthesis is triggered by primary charge separation in proteins at the photosystem II reaction center. Here, we investigate the impacts of the protein environment and intramolecular vibrations on primary charge separation at the photosystem II reaction center. This is accomplished by combining the quantum dynamic theories of condensed phase electron transfer with quantum chemical calculations to evaluate the vibrational Huang-Rhys factors of chlorophyll and pheophytin molecules. We report that individual vibrational modes play a minor role in promoting the charge separation, contrary to the discussion in recent publications. Nevertheless, these small contributions accumulate to considerably influence the charge separation rate, resulting in sub-picosecond charge separation almost independent of the driving force and temperature. We suggest that the intramolecular vibrations complement the robustness of the charge separation in the photosystem II reaction center against the inherently large static disorder of the involved electronic energies.
The photosystem II reaction centre is the photosynthetic complex responsible for oxygen production on Earth. Its water splitting function is particularly favoured by the formation of a stable charge separated state via a pathway that starts at an acc
Photosystem II is crucial for life on Earth as it provides oxygen as a result of photoinduced electron transfer and water splitting reactions. The excited state dynamics of the photosystem II-reaction center (PSII-RC) has been a matter of vivid debat
Density-functional tight binding (DFTB) has become a popular form of approximate density-functional theory (DFT) based upon a minimal valence basis set and neglect of all but two center integrals. We report the results of our tests of a recent long-r
The H + D_2^+(v=0,1 and 2) charge transfer reaction is studied using an accurate wave packet method, using recently proposed coupled diabatic potential energy surfaces. The state-to-state cross section is obtained for three different channels: non-re
We extract the dynamics implicit in an algebraic fitted model Hamiltonian for the hydrogen chromophores vibrational motion in the molecule $CF_3CHFI$. The original model has 4 degrees of freedom, three positions and one representing interbond couplin