Dynamics of charge separation in the excited-state chemistry of protochlorophyllide

被引:16
作者
Dietzek, Benjamin [1 ,2 ]
Tschierlei, Stefanie [1 ]
Hanf, Robert [1 ]
Seidel, Sonja [3 ]
Yartsev, Arkady [4 ]
Schmitt, Michael [1 ]
Hermann, Gudrun [3 ]
Popp, Juergen [1 ,2 ]
机构
[1] Univ Jena, Inst Phys Chem, D-07743 Jena, Germany
[2] Inst Photon Technol Jena eV, D-07745 Jena, Germany
[3] Univ Jena, Inst Biochem & Biophys, D-07743 Jena, Germany
[4] Lund Univ, Dept Chem Phys, S-22100 Lund, Sweden
关键词
APPROXIMATE COULOMB POTENTIALS; TIME-RESOLVED ABSORPTION; AUXILIARY BASIS-SETS; GAUSSIAN-BASIS SETS; CHLOROPHYLL BIOSYNTHESIS; TRANSFER COMPLEX; ATOMS LI; SPECTROSCOPY; PHOTOREDUCTION; OXIDOREDUCTASE;
D O I
10.1016/j.cplett.2010.04.027
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
In this study the excited-state dynamics of protochlorophyllide a (PChlide), the substrate of the enzyme protochlorophyllide oxidoreductase, was examined by means of time-resolved absorption anisotropy and magic-angle measurements. The solvent polarity dependent anisotropy data provide strong evidence for the existence of an excited-state with charge-transfer character. A solvent dependency is also observed in the magic-angle kinetics. In a nonpolar environment wave packet oscillations are monitored while they are quenched in a polar solvent. These results show that the excited-state relaxations of PChlide are determined by the nature of the solvent environment. The implications of these findings are discussed with respect to the enzyme catalysed reaction. (C) 2010 Elsevier B. V. All rights reserved.
引用
收藏
页码:157 / 163
页数:7
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