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

Dynamics of charge separation in the excited-state chemistry of protochlorophyllide
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DOI:
10.1016/j.cplett.2010.04.027
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发表时间:
2010-05-26
影响因子:
2.8
通讯作者:
Popp, Juergen
Popp, Juergen
中科院分区:
化学4区
文献类型:
--
作者:
Dietzek, Benjamin;Tschierlei, Stefanie;Popp, Juergen

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在这项研究中,激发态动力学的原叶绿素a(PChlide),酶原叶绿素氧化还原酶的底物,通过时间分辨吸收各向异性和魔角测量检查。溶剂极性相关的各向异性数据提供了强有力的证据,存在一个激发态的电荷转移字符。在魔角动力学中也观察到溶剂依赖性。在非极性环境中,当波包振荡在极性溶剂中淬灭时,监测波包振荡。这些结果表明,PClide的激发态弛豫由溶剂环境的性质决定。这些研究结果的影响进行了讨论相对于酶催化反应。(C)2010年爱思唯尔B。V.保留所有权利。
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.