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  • Title: UV excited-state photoresponse of biochromophore negative ions.
    Author: Bochenkova AV, Klærke B, Rahbek DB, Rajput J, Toker Y, Andersen LH.
    Journal: Angew Chem Int Ed Engl; 2014 Sep 08; 53(37):9797-801. PubMed ID: 25044707.
    Abstract:
    Members of the green fluorescent protein (GFP) family may undergo irreversible phototransformation upon irradiation with UV light. This provides clear evidence for the importance of the higher-energy photophysics of the chromophore, which remains essentially unexplored. By using time-resolved action and photoelectron spectroscopy together with high-level electronic structure theory, we directly probe and identify higher electronically excited singlet states of the isolated para- and meta-chromophore anions of GFP. These molecular resonances are found to serve as a doorway for very efficient electron detachment in the gas phase. Inside the protein, this band is found to be resonant with the quasicontinuum of a solvated electron, thus enhancing electron transfer from the GFP to the solvent. This suggests a photophysical pathway for photoconversion of the protein, where GFP resonant photooxidation in solution triggers radical redox reactions inside these proteins.
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