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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Light-induced Chromophore Activity And Signal Transduction In Phytochromes Observed By ~(13)c And ~(15)n Magic-angle Spinning Nmr
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Light-induced Chromophore Activity And Signal Transduction In Phytochromes Observed By ~(13)c And ~(15)n Magic-angle Spinning Nmr

机译：〜（13）c和〜（15）n幻角自旋Nmr观测到的光致色素中的光致发色团活性和信号转导

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摘要

Both thermally stable states of phytochrome, Pr and Pfr, have been studied by ~(13)C and ~(15)N cross-polarization (CP) magic-angle spinning (MAS) NMR using cyanobacterial (Cph1) and plant (phyA) phytochrome sensory modules containing uniformly ~(13)C- and ~(15)N-labeled bilin chromophores. Two-dimensional homo- and heteronuclear experiments allowed most of the ~(13)C chemical shifts to be assigned in both states. Chemical shift differences reflect changes of the electronic structure of the cofactor at the atomic level as well as its interactions with the chromophore-binding pocket. The chromophore in cyanobacterial and plant phytochromes shows very similar features in the respective Pr and Pfr states. The data are interpreted in terms of a strengthened hydrogen bond at the ring D carbonyl. The red shift in the Pfr state is explained by the increasing length of the conjugation network beyond ring C including the entire ring D. Enhanced conjugation within the π-system stabilizes the more tensed chromophore in the Pfr state. Concomitant changes at the ring C propionate carboxylate and the ring D carbonyl are explained by a loss of hydrogen bonding to Cph1-His-290 and transmittance of conformational changes to the ring C propionate via a water network. These and other conformational changes may lead to modified surface interactions, e.g., along the tongue region contacting the bilin chromophore.
机译：已通过〜（13）C和〜（15）N交叉极化（CP）幻角旋转（MAS）NMR使用蓝细菌（Cph1）和植物（phyA）研究了植物色素的热稳定状态Pr和Pfr。包含〜（13）C-和〜（15）N标记的Bilin生色团的植物色素感觉模块。二维同核和异核实验允许在两种状态下分配大多数〜（13）C化学位移。化学位移差异反映了辅因子在原子水平上的电子结构的变化及其与生色团结合袋的相互作用。蓝细菌和植物植物色素中的生色团在各自的Pr和Pfr状态下显示出非常相似的特征。数据解释为在D环羰基上的氢键加强。 Pfr状态下的红移是由包括整个环D在内的环C以外的共轭网络长度的增加所解释的。π系统内增强的共轭使Pfr状态下的发色团更稳定。 C环丙酸酯羧酸盐和D环羰基的伴随变化是通过氢与Cph1-His-290的键合损失以及构象变化通过水网络传递给C环丙酸酯而解释的。这些和其他构象变化可导致修饰的表面相互作用，例如沿着与胆汁发色团接触的舌头区域。

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