Mechanism of resonant electron emission from the deprotonated GFP chromophore and its biomimetics

Chemical Science
Anastasia V BochenkovaHelen H Fielding

Abstract

The Green Fluorescent Protein (GFP), which is widely used in bioimaging, is known to undergo light-induced redox transformations. Electron transfer is thought to occur resonantly through excited states of its chromophore; however, a detailed understanding of the electron gateway states of the chromophore is still missing. Here, we use photoelectron spectroscopy and high-level quantum chemistry calculations to show that following UV excitation, the ultrafast electron dynamics in the chromophore anion proceeds via an excited shape resonance strongly coupled to the open continuum. The impact of this state is found across the entire 355-315 nm excitation range, from above the first bound-bound transition to below the opening of higher-lying continua. By disentangling the electron dynamics in the photodetachment channels, we provide an important reference for the adiabatic position of the electron gateway state, which is located at 348 nm, and discover the source of the curiously large widths of the photoelectron spectra that have been reported in the literature. By introducing chemical modifications to the GFP chromophore, we show that the detachment threshold and the position of the gateway state, and hence the underlying excited-...Continue Reading

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Citations

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
Sep 18, 2018·Physical Chemistry Chemical Physics : PCCP·Cate S AnstöterJan R R Verlet
Aug 1, 2020·Frontiers in Molecular Biosciences·Breland G OscarChong Fang
May 28, 2021·The Journal of Physical Chemistry. a·Cate S Anstöter, Jan R R Verlet
Jun 16, 2021·Journal of Environmental Science and Health. Part A, Toxic/hazardous Substances & Environmental Engineering·Mogos GirmatsionHe Qian
Nov 5, 2019·The Journal of Physical Chemistry Letters·Wyatt Zagorec-MarksJ Mathias Weber
Aug 16, 2021·Mass Spectrometry Reviews·František Tureček
Mar 9, 2019·The Journal of Physical Chemistry. a·Joanne L WoodhouseHelen H Fielding
Feb 20, 2020·The Journal of Physical Chemistry Letters·Wyatt Zagorec-MarksJ Mathias Weber
Jan 30, 2019·The Journal of Physical Chemistry. a·Joshua P RogersJan R R Verlet
May 5, 2018·The Journal of Physical Chemistry Letters·Eduardo CarrascosaEvan J Bieske
Sep 21, 2018·The Journal of Physical Chemistry. a·Alice HenleyHelen H Fielding
Feb 28, 2020·The Journal of Physical Chemistry. a·James N BullJan R R Verlet
Apr 3, 2020·The Journal of Physical Chemistry. a·Jan R R VerletJoshua P Rogers
Sep 3, 2021·Physical Chemistry Chemical Physics : PCCP·Joanne L WoodhouseHelen H Fielding
Jan 6, 2022·Physical Chemistry Chemical Physics : PCCP·Cate S AnstöterJan R R Verlet

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Methods Mentioned

BETA
fluorescence
biosensing

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