Manipulating the Energetics and Rates of Electron Transfer in Rhodobacter capsulatus Reaction Centers with Asymmetric Pigment Content

Faries, Kaitlyn M.; Dylla, Nicholas P.; Hanson, Deborah K.; Holten, Dewey; Laible, Philip D.; Kirmaier, Christine

doi:10.1021/acs.jpcb.7b01389

Title: Manipulating the Energetics and Rates of Electron Transfer in Rhodobacter capsulatus Reaction Centers with Asymmetric Pigment Content

Journal Article · Mon Jul 17 04:00:00 UTC 2017 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

DOI: https://doi.org/10.1021/acs.jpcb.7b01389 · OSTI ID:1774946

Faries, Kaitlyn M. ^[1]; Dylla, Nicholas P. ^[2]; Hanson, Deborah K. ^[2]; Holten, Dewey ^[3]; Laible, Philip D. ^[2];

^[3]

Washington Univ., St. Louis, MO (United States); Washington University
Argonne National Lab. (ANL), Lemont, IL (United States)
Washington Univ., St. Louis, MO (United States)

Seemingly redundant parallel pathways for electron transfer (ET) – comprised of identical sets of cofactors – are a cornerstone feature of photosynthetic reaction centers (RCs) involved in light-energy conversion. In native bacterial RCs, both the A and B branches house one bacteriochlorophyll (BChl) and one bacteriopheophytin (BPh), but the A branch is used exclusively. Described herein are 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 (Φ_B) replaces the B-side BChl (B_B)], and the Leu(M212)His mutation [a BChl (β_A) replaces the A-side BPh (H_A)]. Additionally, Tyr(M208)Phe was employed to disfavor ET to the A branch and in one mutant Val(M131)Glu creates a hydrogen bond to H_B to enhance ET to H_B. In both Φ_B 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⁺Φ_B^- formed predominately from the 9-ps fraction. The 50-60% yield of P⁺Φ_B^- is the highest yet observed for a Φ_B-containing RC. Here, the results provide insight into factors needed for efficient multi-step ET.

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Research Organization:: Washington Univ., St. Louis, MO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation Graduate Research Fellowship

Grant/Contract Number:: SC0002036; AC02-06CH11357

OSTI ID:: 1774946

Journal Information:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry, Journal Name: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry Journal Issue: 29 Vol. 121; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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