Kinetic-dynamic model for conformational control of an electron transfer photocycle: mixed-metal hemoglobin hybrids.

The Journal of Physical Chemistry. B
Ami D PatelBrian M Hoffman

Abstract

It is becoming increasingly clear that the transfer of an electron across a protein-protein interface is coupled to the dynamics of conformational conversion between and within ensembles of interface conformations. Electron transfer (ET) reactions in conformationally mobile systems provide a "clock" against which the rapidity of a dynamic process may be measured, and we here report a simple kinetic (master equation) model that self-consistently incorporates conformational dynamics into an ET photocycle comprised of a photoinitiated "forward" step and thermal return to ground. This kinetic/dynamic (KD) model assumes an ET complex exists as multiple interconverting conformations which partition into an ET-optimized (reactive; R) population and a less-reactive population ( S). We take the members of each population to be equivalent by constraining them to have the same conformational energy, the same average rate constant for conversion to members of the other population, and the same rate constants for forward and back ET. The result is a mapping of a complicated energy surface onto the simple "gating", two-well surface, but with rate constants that are defined microscopically. This model successfully describes the changes in the...Continue Reading

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Citations

May 1, 2010·Journal of the American Chemical Society·Karamatullah DanyalBrian M Hoffman
Oct 12, 2019·Journal of the American Chemical Society·Estella F YeeBrian R Crane

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