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• W2548202225 abstract "Abstract The effect of dehydration on the kinetics of forward electron transfer (ET) has been studied in cyanobacterial photosystem I (PS I) complexes in a trehalose glassy matrix by time-resolved optical and EPR spectroscopies in the 100 fs to 1 ms time domain. The kinetics of the flash-induced absorption changes in the subnanosecond time domain due to primary and secondary charge separation steps were monitored by pump–probe laser spectroscopy with 20-fs low-energy pump pulses centered at 720 nm. The back-reaction kinetics of P 700 were measured by high-field time-resolved EPR spectroscopy and the forward kinetics of <m:math xmlns:m=http://www.w3.org/1998/Math/MathML> <m:mrow> <m:msubsup> <m:mtext>A</m:mtext> <m:mrow> <m:mtext>1A</m:mtext> </m:mrow> <m:mrow> <m:mo>•</m:mo> <m:mo>−</m:mo> </m:mrow> </m:msubsup> <m:mo>/</m:mo> <m:msubsup> <m:mtext>A</m:mtext> <m:mrow> <m:mn>1</m:mn> <m:mtext>B</m:mtext> </m:mrow> <m:mrow> <m:mo>•</m:mo> <m:mo>−</m:mo> </m:mrow> </m:msubsup> <m:mo>→</m:mo> <m:msub> <m:mtext>F</m:mtext> <m:mtext>X</m:mtext> </m:msub> </m:mrow> </m:math> ${rm{A}}_{{rm{1A}}}^{ bullet - }/{rm{A}}_{1{rm{B}}}^{ bullet - } to {{rm{F}}_{rm{X}}}$ by time-resolved optical spectroscopy at 480 nm. The kinetics of the primary ET reactions to form the primary <m:math xmlns:m=http://www.w3.org/1998/Math/MathML> <m:mrow> <m:msubsup> <m:mtext>P</m:mtext> <m:mrow> <m:mn>700</m:mn> </m:mrow> <m:mrow> <m:mo>•</m:mo> <m:mo>+</m:mo> </m:mrow> </m:msubsup> <m:msubsup> <m:mtext>A</m:mtext> <m:mn>0</m:mn> <m:mrow> <m:mo>•</m:mo> <m:mo>−</m:mo> </m:mrow> </m:msubsup> </m:mrow> </m:math> ${rm{P}}_{700}^{ bullet + }{rm{A}}_0^{ bullet - }$ and the secondary <m:math xmlns:m=http://www.w3.org/1998/Math/MathML> <m:mrow> <m:msubsup> <m:mtext>P</m:mtext> <m:mrow> <m:mn>700</m:mn> </m:mrow> <m:mrow> <m:mo>•</m:mo> <m:mo>+</m:mo> </m:mrow> </m:msubsup> <m:msubsup> <m:mtext>A</m:mtext> <m:mn>1</m:mn> <m:mrow> <m:mo>•</m:mo> <m:mo>−</m:mo> </m:mrow> </m:msubsup> </m:mrow> </m:math> ${rm{P}}_{700}^{ bullet + }{rm{A}}_1^{ bullet - }$ ion radical pairs were not affected by dehydration in the trehalose matrix, while the yield of the <m:math xmlns:m=http://www.w3.org/1998/Math/MathML> <m:mrow> <m:msubsup> <m:mtext>P</m:mtext> <m:mrow> <m:mn>700</m:mn> </m:mrow> <m:mrow> <m:mo>•</m:mo> <m:mo>+</m:mo> </m:mrow> </m:msubsup> <m:msubsup> <m:mtext>A</m:mtext> <m:mn>1</m:mn> <m:mrow> <m:mo>•</m:mo> <m:mo>−</m:mo> </m:mrow> </m:msubsup> </m:mrow> </m:math> ${rm{P}}_{700}^{ bullet + }{rm{A}}_1^{ bullet - }$ was decreased by ~20%. Forward ET from the phylloquinone molecules in the <m:math xmlns:m=http://www.w3.org/1998/Math/MathML> <m:mrow> <m:msubsup> <m:mtext>A</m:mtext> <m:mrow> <m:mn>1</m:mn> <m:mtext>A</m:mtext> </m:mrow> <m:mrow> <m:mo>•</m:mo> <m:mo>−</m:mo> </m:mrow> </m:msubsup> </m:mrow> </m:math> ${rm{A}}_{1{rm{A}}}^{ bullet - }$ and <m:math xmlns:m=http://www.w3.org/1998/Math/MathML> <m:mrow> <m:msubsup> <m:mtext>A</m:mtext> <m:mrow> <m:mn>1</m:mn> <m:mtext>B</m:mtext> </m:mrow> <m:mrow> <m:mo>•</m:mo> <m:mo>−</m:mo> </m:mrow> </m:msubsup> </m:mrow> </m:math> ${rm{A}}_{1{rm{B}}}^{ bullet - }$ sites to the iron–sulfur cluster F X slowed from ~220 ns and ~20 ns in solution to ~13 μs and ~80 ns, respectively. However, as shown by EPR spectroscopy, the ~15 μs kinetic phase also contains a small contribution from the recombination between <m:math xmlns:m=http://www.w3.org/1998/Math/MathML> <m:mrow> <m:msubsup> <m:mtext>A</m:mtext> <m:mrow> <m:mn>1</m:mn> <m:mtext>B</m:mtext> </m:mrow> <m:mrow> <m:mo>•</m:mo> <m:mo>−</m:mo> </m:mrow> </m:msubsup> </m:mrow> </m:math> ${rm{A}}_{1{rm{B}}}^{ bullet - }$ and <m:math xmlns:m=http://www.w3.org/1998/Math/MathML> <m:mrow> <m:msubsup> <m:mtext>P</m:mtext> <m:mrow> <m:mn>700</m:mn> </m:mrow> <m:mrow> <m:mo>•</m:mo> <m:mo>+</m:mo> </m:mrow> </m:msubsup> <m:mo>.</m:mo> </m:mrow> </m:math> ${rm{P}}_{700}^{ bullet + }.$ These data reveal that the initial ET reactions from P 700 to secondary phylloquinone acceptors in the A- and B-branches of cofactors (A 1A and A 1B ) remain unaffected whereas ET beyond A 1A and A 1B is slowed or prevented by constrained protein dynamics due to the dry trehalose glass matrix." @default.
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• W2548202225 date "2016-11-03" @default.
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• W2548202225 title "Effect of Dehydrated Trehalose Matrix on the Kinetics of Forward Electron Transfer Reactions in Photosystem I" @default.
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• W2548202225 doi "https://doi.org/10.1515/zpch-2016-0860" @default.
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