Controlling radical formation in the photoactive yellow protein chromophore

Angewandte Chemie
Ciarán R S MooneyHelen H Fielding

Abstract

To understand how photoactive proteins function, it is necessary to understand the photoresponse of the chromophore. Photoactive yellow protein (PYP) is a prototypical signaling protein. Blue light triggers trans-cis isomerization of the chromophore covalently bound within PYP as the first step in a photocycle that results in the host bacterium moving away from potentially harmful light. At higher energies, photoabsorption has the potential to create radicals and free electrons; however, this process is largely unexplored. Here, we use photoelectron spectroscopy and quantum chemistry calculations to show that the molecular structure and conformation of the isolated PYP chromophore can be exploited to control the competition between trans-cis isomerization and radical formation. We also find evidence to suggest that one of the roles of the protein is to impede radical formation in PYP by preventing torsional motion in the electronic ground state of the chromophore.

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Citations

Jan 11, 2017·Journal of Chemical Theory and Computation·Francisco F García-PrietoM Elena Martín
Apr 1, 2017·Journal of Chemical Theory and Computation·Joel M MilaneseChristine M Isborn
May 17, 2017·Chemical Science·Anastasia V BochenkovaHelen H Fielding
Mar 31, 2016·Physical Chemistry Chemical Physics : PCCP·Michael A ParkesHelen H Fielding
Sep 25, 2017·Physical Chemistry Chemical Physics : PCCP·Cate S AnstöterJan R R Verlet
May 29, 2018·Physical Chemistry Chemical Physics : PCCP·Michael A ParkesHelen H Fielding
Nov 23, 2017·Physical Chemistry Chemical Physics : PCCP·Alice HenleyHelen H Fielding
Sep 28, 2017·Scientific Reports·Frederico M PimentaArnaud Gautier
Dec 22, 2019·Nature Communications·James N BullJan R R Verlet
Mar 9, 2019·The Journal of Physical Chemistry. a·Joanne L WoodhouseHelen H Fielding
Jan 30, 2020·The Journal of Physical Chemistry. a·Satoru MuramatsuTakayuki Ebata
Sep 21, 2018·The Journal of Physical Chemistry. a·Alice HenleyHelen H Fielding
Apr 10, 2019·The Journal of Physical Chemistry. a·James N BullEvan J Bieske
Feb 28, 2020·The Journal of Physical Chemistry. a·James N BullJan R R Verlet
Sep 3, 2021·Physical Chemistry Chemical Physics : PCCP·Joanne L WoodhouseHelen H Fielding

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