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• W1969531330 endingPage "1586" @default.
• W1969531330 startingPage "1580" @default.
• W1969531330 abstract "We have previously reported the enthalpy and volume changes of charge separation in photosystem I from Synechocystis 6803 using pulsed photoacoustics on the microsecond time scale, assigned to the electron-transfer reaction from excited-state P700* to FA/B iron sulfur clusters. In the present work, we focus on the thermodynamics of two steps in photosystem I: (1) P700* → A1-FX (<10 ns) and (2) A1-FX → FA/B- (20−200 ns). The fit by convolution of photoacoustic waves on the nanosecond and microsecond time scales resolved two kinetic components: (1) a prompt component (<10 ns) with large negative enthalpy (−0.8 ± 0.1 eV) and large volume change (−23 ± 2 A3), which are assigned to the P700* → A1-FX step, and (2) a component with ∼200 ns lifetime, which has a positive enthalpy (+0.4 ± 0.2 eV) and a small volume change (−3 ± 2 A3) that are attributed to the A1-FX → FA/B- step. For the fast reaction using the redox potentials of A1FX (−0.67 V) and P700 (+0.45 V) and the energy of P700* (1.77 eV), the free energy change for the P700* → A1-FX step is −0.63 eV, and thus the entropy change (TΔS, T = 25 °C) is −0.2 ± 0.3 eV. For the slow reaction, A1-FX → FA/B-, taking the free energy of −0.14 eV [Santabara, S.; Heathcote, P; Evans, C. W. Biochim. Biophys. Acta 2005, 1708, 283−310], the entropy change (TΔS) is positive, +0.54 ± 0.3 eV. The positive entropy contribution is larger than the positive enthalpy, which indicates that the A-FX to FA/B- step in photosystem I is entropy driven. Other possible contributions to the measured values are discussed." @default.
• W1969531330 created "2016-06-24" @default.
• W1969531330 creator A5007187838 @default.
• W1969531330 creator A5089619712 @default.
• W1969531330 date "2006-01-13" @default.
• W1969531330 modified "2023-09-27" @default.
• W1969531330 title "The A^-F_X to F_A/B Step in <i>Synechocystis </i>6803 Photosystem I Is Entropy Driven" @default.
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• W1969531330 doi "https://doi.org/10.1021/ja054870y" @default.
• W1969531330 hasPubMedCentralId "https://www.ncbi.nlm.nih.gov/pmc/articles/2597517" @default.
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