Mechanism of primary proton transfer in bacteriorhodopsin

Structure
Ana-Nicoleta BondarStefan Fischer

Abstract

Recent structures of putative intermediates in the bacteriorhodopsin photocycle have provided valuable snapshots of the mechanism by which protons are pumped across the membrane. However, key steps remain highly controversial, particularly the proton transfer occurring immediately after retinal trans-->cis photoisomerization. The gradual release of stored energy is inherently nonequilibrium: which photocycle intermediates are populated depends not only on their energy but also on their interconversion rates. To understand why the photocycle follows a productive (i.e., pumping), rather than some unproductive, relaxation pathway, it is necessary to know the relative energy barriers of individual steps. To discriminate between the many proposed scenarios of this process, we computed all its possible minimum-energy paths. This reveals that not one, but three very different pathways have energy barriers consistent with experiment. This result reconciles the conflicting views held on the mechanism and suggests a strategy by which the protein renders this essential step resilient.

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Citations

May 3, 2005·Proceedings of the National Academy of Sciences of the United States of America·Stefan FischerJeremy C Smith
May 29, 2009·Proceedings of the National Academy of Sciences of the United States of America·Vikram S BajajRobert G Griffin
May 23, 2014·Physical Chemistry Chemical Physics : PCCP·Qiang Cui, Marcus Elstner
Jul 10, 2014·Proceedings of the National Academy of Sciences of the United States of America·Farooq Ahmad Kiani, Stefan Fischer
Jan 13, 2006·The Journal of Physical Chemistry. a·P H KönigQ Cui
Jan 16, 2008·Proceedings of the National Academy of Sciences of the United States of America·Melody L Mak-JurkauskasJudith Herzfeld
Feb 13, 2009·The Journal of Biological Chemistry·Christoph PfistererStefan Fischer
Oct 23, 2010·PloS One·Moumita SaharayJeremy C Smith
May 13, 2011·The Journal of Physical Chemistry. B·Maike ClemensMarcus Elstner
Nov 30, 2010·The Journal of Membrane Biology·Ana-Nicoleta BondarJeremy C Smith
Jul 25, 2009·Journal of Molecular Modeling·Mirco S Till, G Matthias Ullmann
Jun 9, 2006·Photochemical & Photobiological Sciences : Official Journal of the European Photochemistry Association and the European Society for Photobiology·Ana-Nicoleta BondarStefan Fischer
Apr 26, 2006·Photochemistry and Photobiology·Akio MaedaThomas G Ebrey
Oct 18, 2006·Journal of Computer-aided Molecular Design·Marius WankoMarcus Elstner
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Sep 10, 2014·The Journal of Physical Chemistry. B·Tino WolterAna-Nicoleta Bondar
Nov 27, 2015·Biochimica Et Biophysica Acta·Stefan Milenkovic, Ana-Nicoleta Bondar
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Nov 21, 2013·Biochimica Et Biophysica Acta·Coral Del ValAna-Nicoleta Bondar
Mar 1, 2014·Journal of Structural Biology·Coral del ValAna-Nicoleta Bondar
Mar 20, 2013·Biochimica Et Biophysica Acta·M R GunnerJianxun Lu
Apr 20, 2005·Structure·Andreea D GruiaStefan Fischer
Jun 15, 2016·Physical Chemistry Chemical Physics : PCCP·Farooq Ahmad Kiani, Stefan Fischer
Apr 8, 2009·Journal of the American Chemical Society·Víctor A Lórenz-Fonfría, Hideki Kandori
May 14, 2017·Photochemistry and Photobiology·Thomas KöhlerJosef Wachtveitl

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