2013
DOI: 10.1021/bi400144e
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Split Electron Paramagnetic Resonance Signal Induction in Photosystem II Suggests Two Binding Sites in the S2 State for the Substrate Analogue Methanol

Abstract: Illuminating a photosystem II sample at low temperatures (here 5-10 K) yields so-called split signals detectable with continuous wave-electron paramagnetic resonance (CW-EPR). These signals reflect the oxidized, deprotonated radical of D1-Tyr161 (YZ(•)) in a magnetic interaction with the CaMn4 cluster in a particular S state. The intensity of the split EPR signals are affected by the addition of the water substrate analogue methanol. This was previously shown by the induction of split EPR signals from the S1, … Show more

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Cited by 9 publications
(22 citation statements)
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“…A hypothesis regarding the presence of two methanol binding sites was previously advanced by Sjöholm et al to account for the different methanol concentration dependence in the induction of “split” EPR signals of the OEC, that is, of states that contain a tyrosyl radical interacting with the manganese cluster. 63 The postulated interaction modes (direct binding of methanol to Mn1 and/or Mn4) can no longer be considered viable, so it might be worth revisiting that analysis in light of the present results and of the required occupation of the W6 site.…”
Section: Resultsmentioning
confidence: 84%
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“…A hypothesis regarding the presence of two methanol binding sites was previously advanced by Sjöholm et al to account for the different methanol concentration dependence in the induction of “split” EPR signals of the OEC, that is, of states that contain a tyrosyl radical interacting with the manganese cluster. 63 The postulated interaction modes (direct binding of methanol to Mn1 and/or Mn4) can no longer be considered viable, so it might be worth revisiting that analysis in light of the present results and of the required occupation of the W6 site.…”
Section: Resultsmentioning
confidence: 84%
“…73,132,142144 In this case, the influence of MeOH on proton release from W1 would be a second-order effect, acting through perturbation of the proton acceptor. This may result in modulation of the relative stabilities of intermediates such as tyrosyl radical states 53,57,58,63,122,145,146 in a species-dependent manner and is a subject that deserves further study.…”
Section: Resultsmentioning
confidence: 99%
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“…35 There appear to be differences in the concentration dependence of the effects of methanol on these signals that are S-state dependent, indicating that the binding affinity of MeOH at the Mn 4 CaO 5 cluster may change as a function of the oxidation state of the cluster. 34 …”
mentioning
confidence: 99%