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

Abstract

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 (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 and 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 predominately from the 9-ps fraction. The 50-60% yield of P+ΦB- is the highest yet observed for a ΦB-containing RC. Here, the results provide insightmore » into factors needed for efficient multi-step ET.« less

Authors:
 [1];  [2];  [2];  [1];  [2]; ORCiD logo [1]
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  1. Washington Univ., St. Louis, MO (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Washington Univ., St. Louis, MO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation Graduate Research Fellowship
OSTI Identifier:
1774946
Grant/Contract Number:  
SC0002036; AC02-06CH11357; DGE-1143954
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry
Additional Journal Information:
Journal Volume: 121; Journal Issue: 29; Journal ID: ISSN 1520-6106
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; Dyes and pigments; Free energy; Absorption; Genetics; Electrical properties

Citation Formats

Faries, Kaitlyn M., Dylla, Nicholas P., Hanson, Deborah K., Holten, Dewey, Laible, Philip D., and Kirmaier, Christine. Manipulating the Energetics and Rates of Electron Transfer in Rhodobacter capsulatus Reaction Centers with Asymmetric Pigment Content. United States: N. p., 2017. Web. doi:10.1021/acs.jpcb.7b01389.
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Faries, Kaitlyn M., Dylla, Nicholas P., Hanson, Deborah K., Holten, Dewey, Laible, Philip D., & Kirmaier, Christine. Manipulating the Energetics and Rates of Electron Transfer in Rhodobacter capsulatus Reaction Centers with Asymmetric Pigment Content. United States. https://doi.org/10.1021/acs.jpcb.7b01389
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Faries, Kaitlyn M., Dylla, Nicholas P., Hanson, Deborah K., Holten, Dewey, Laible, Philip D., and Kirmaier, Christine. Mon . "Manipulating the Energetics and Rates of Electron Transfer in Rhodobacter capsulatus Reaction Centers with Asymmetric Pigment Content". United States. https://doi.org/10.1021/acs.jpcb.7b01389. https://www.osti.gov/servlets/purl/1774946.
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@article{osti_1774946,
title = {Manipulating the Energetics and Rates of Electron Transfer in Rhodobacter capsulatus Reaction Centers with Asymmetric Pigment Content},
author = {Faries, Kaitlyn M. and Dylla, Nicholas P. and Hanson, Deborah K. and Holten, Dewey and Laible, Philip D. and Kirmaier, Christine},
abstractNote = {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 (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 and 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 predominately from the 9-ps fraction. The 50-60% yield of P+ΦB- is the highest yet observed for a ΦB-containing RC. Here, the results provide insight into factors needed for efficient multi-step ET.},
doi = {10.1021/acs.jpcb.7b01389},
journal = {Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry},
number = 29,
volume = 121,
place = {United States},
year = {Mon Jul 17 00:00:00 EDT 2017},
month = {Mon Jul 17 00:00:00 EDT 2017}
}
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https://doi.org/10.1021/acs.jpcb.7b01389
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