Počet záznamů: 1

Phototriggering Electron Flow through ReI-modified Pseudomonas aeruginosa Azurins

  1. 1.
    0359154 - UFCH-W 2012 RIV DE eng J - Článek v odborném periodiku
    Blanco-Rodríguez, A. M. - Di Billio, A. J. - Shih, C. - Museth, A. K. - Clark, I. P. - Towrie, M. - Cannizzo, A. - Sudhamsu, J. - Crane, B. R. - Sýkora, Jan - Winkler, J. R. - Gray, H. B. - Záliš, Stanislav - Vlček Jr., Antonín
    Phototriggering Electron Flow through ReI-modified Pseudomonas aeruginosa Azurins.
    Chemistry - A European Journal. Roč. 17, č. 19 (2011), s. 5350-5361 ISSN 0947-6539
    Grant CEP: GA MŠk(CZ) ME10124; GA MŠk OC09043
    Výzkumný záměr: CEZ:AV0Z40400503
    Klíčová slova: density functional calculations * electron transfer * IR spectroscopy
    Kód oboru RIV: CG - Elektrochemie
    Impakt faktor: 5.925, rok: 2011

    The [ReI(CO)3(4,7-dimethyl-1,10-phenanthroline)(histidine-124)(tryptophan-122)] complex, denoted [ReI(dmp)(W122)], of Pseudomonas aeruginosa azurin behaves as a single photoactive unit that triggers very fast electron transfer (ET) from a distant (2 nm) CuI center in the protein. Analysis of time-resolved (ps–μs) IR spectroscopic and kinetics data collected on [ReI(dmp)(W122)AzM] (in which M=ZnII, CuII, CuI; Az=azurin) and position-122 tyrosine (Y), phenylalanine (F), and lysine (K) mutants, together with excited-state DFT/time-dependent (TD)DFT calculations and X-ray structural characterization, reveal the character, energetics, and dynamics of the relevant electronic states of the [ReI(dmp)(W122)] unit and a cascade of photoinduced ET and relaxation steps in the corresponding Re–azurins. Optical population of [ReI(imidazole-H124)(CO)3]→dmp 1CT states (CT=charge transfer) is followed by around 110 fs intersystem crossing and about 600 ps structural relaxation to a 3CT state.
    Trvalý link: http://hdl.handle.net/11104/0196990