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Role of Coherent Low-Frequency Motion in Excited-State Proton Transfer of Green Fluorescent Protein Studied by Time-Resolved Impulsive Stimulated Raman Spectroscopy
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2016-03-21 , DOI: 10.1021/jacs.5b11038
Tomotsumi Fujisawa , Hikaru Kuramochi , Haruko Hosoi 1 , Satoshi Takeuchi , Tahei Tahara
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2016-03-21 , DOI: 10.1021/jacs.5b11038
Tomotsumi Fujisawa , Hikaru Kuramochi , Haruko Hosoi 1 , Satoshi Takeuchi , Tahei Tahara
Affiliation
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Green fluorescent protein (GFP) from jellyfish Aequorea victoria, an essential bioimaging tool, luminesces via excited-state proton transfer (ESPT) in which the phenolic proton of the p-hydroxybenzylideneimidazolinone chromophore is transferred to Glu222 through a hydrogen-bond network. In this process, the ESPT mediated by the low-frequency motion of the chromophore has been proposed. We address this issue using femtosecond time-resolved impulsive stimulated Raman spectroscopy. After coherently exciting low-frequency modes (<300 cm(-1)) in the excited state of GFP, we examined the excited-state structural evolution and the ESPT dynamics within the dephasing time of the low-frequency vibration. A clear anharmonic vibrational coupling is found between one high-frequency mode of the chromophore (phenolic CH bend) and a low-frequency mode at ∼104 cm(-1). However, the data show that this low-frequency motion does not substantially affect the ESPT dynamics.
中文翻译:
相干低频运动在绿色荧光蛋白激发态质子转移中的作用时间分辨脉冲受激拉曼光谱研究
来自水母 Aequorea victoria 的绿色荧光蛋白 (GFP),一种重要的生物成像工具,通过激发态质子转移 (ESPT) 发光,其中对羟基苯亚甲基咪唑啉酮发色团的酚类质子通过氢键网络转移到 Glu222。在这个过程中,有人提出了由发色团低频运动介导的ESPT。我们使用飞秒时间分辨脉冲受激拉曼光谱来解决这个问题。在 GFP 的激发态中连贯地激发低频模式 (<300 cm(-1)) 后,我们检查了低频振动的移相时间内的激发态结构演化和 ESPT 动力学。在发色团的一种高频模式(酚醛 CH 弯曲)和约 104 cm(-1) 处的低频模式之间发现了明显的非谐振动耦合。然而,数据表明,这种低频运动不会显着影响 ESPT 动力学。
更新日期:2016-03-21
中文翻译:
![](https://scdn.x-mol.com/jcss/images/paperTranslation.png)
相干低频运动在绿色荧光蛋白激发态质子转移中的作用时间分辨脉冲受激拉曼光谱研究
来自水母 Aequorea victoria 的绿色荧光蛋白 (GFP),一种重要的生物成像工具,通过激发态质子转移 (ESPT) 发光,其中对羟基苯亚甲基咪唑啉酮发色团的酚类质子通过氢键网络转移到 Glu222。在这个过程中,有人提出了由发色团低频运动介导的ESPT。我们使用飞秒时间分辨脉冲受激拉曼光谱来解决这个问题。在 GFP 的激发态中连贯地激发低频模式 (<300 cm(-1)) 后,我们检查了低频振动的移相时间内的激发态结构演化和 ESPT 动力学。在发色团的一种高频模式(酚醛 CH 弯曲)和约 104 cm(-1) 处的低频模式之间发现了明显的非谐振动耦合。然而,数据表明,这种低频运动不会显着影响 ESPT 动力学。