The effect of oxidation on the electronic structure of the green fluorescent protein chromophore

被引：30

作者：

Epifanovsky, E. ^{[1
]}

Polyakov, I. ^{[2
]}

Grigorenko, B. ^{[2
]}

Nemukhin, A. ^{[2
,3
]}

Krylov, A. I. ^{[1
]}

机构：

[1] Univ So Calif, Dept Chem, Los Angeles, CA 90089 USA

[2] Moscow MV Lomonosov State Univ, Dept Chem, Moscow 119991, Russia

[3] Russian Acad Sci, Inst Biochem Phys, Moscow 119334, Russia

来源：

JOURNAL OF CHEMICAL PHYSICS | 2010年 / 132卷 / 11期

基金：

俄罗斯基础研究基金会; 美国国家科学基金会;

关键词：

biochemistry; dissociation; excited states; molecular biophysics; molecular electronic states; oxidation; proteins; red shift; EXCITED-STATE DYNAMICS; QUANTUM-CHEMICAL BENCHMARK; MOLECULAR-ORBITAL METHODS; VARIANT S65T/H148D; BOND-BREAKING; BASIS-SETS; OPEN-SHELL; LIGHT; DECARBOXYLATION; PHOTOACTIVATION;

D O I：

10.1063/1.3336425

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Electronic structure calculations of the singly and doubly ionized states of deprotonated 4(')-hydroxybenzylidene-2,3-dimethylimidazolinone (HBDI anion) are presented. One-electron oxidation produces a doublet radical that has blueshifted absorption, whereas the detachment of two electrons yields a closed-shell cation with strongly redshifted (by about 0.6 eV) absorption relative to the HBDI anion. The results suggest that the doubly oxidized species may be responsible for oxidative redding of green fluorescent protein. The proposed mechanism involves two-step oxidation via electronically excited states and is consistent with the available experimental information [A. M. Bogdanov, A. S. Mishin, I. V. Yampolsky, , Nat. Chem. Biol. 5, 459 (2009)]. The spectroscopic signatures of the ionization-induced structural changes in the chromophore are also discussed.

引用

页数：9

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