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Journal Article
Research Support, U.S. Gov't, Non-P.H.S.
Manipulating the Energetics and Rates of Electron Transfer in Rhodobacter capsulatus Reaction Centers with Asymmetric Pigment Content.
Journal of Physical Chemistry. B 2017 July 28
Seemingly redundant parallel pathways for electron transfer (ET), composed of identical sets of cofactors, are a cornerstone feature of photosynthetic reaction centers (RCs) involved in light-energy conversion. In native bacterial RCs, both A and B branches house one bacteriochlorophyll (BChl) and one bacteriopheophytin (BPh), but the A branch is used exclusively. Described herein are the results obtained for two Rhodobacter capsulatus RCs with an unnaturally high degree of cofactor asymmetry, two BPh on the RC's B side and two BChl on the A side. These pigment changes derive, respectively, from the His(M180)Leu mutation [a BPh (ΦB ) replaces the B-side BChl (BB )], and the Leu(M212)His mutation [a BChl (βA ) replaces the A-side BPh (HA )]. Additionally, Tyr(M208)Phe was employed to disfavor ET to the A branch; in one mutant, Val(M131)Glu creates a hydrogen bond to HB to enhance ET to HB . In both ΦB mutants, the decay kinetics of the excited primary ET donor (P*) resolve three populations with lifetimes of ∼9 ps (50-60%), ∼40 ps (10-20%), and ∼200 ps (20-30%), with P+ ΦB - formed predominantly from the 9 ps fraction. The 50-60% yield of P+ ΦB - is the highest yet observed for a ΦB -containing RC. The results provide insight into factors needed for efficient multistep ET.
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