| 邻羟基绿色荧光蛋白发色团光物理机理的理论研究 |
| |
| 引用本文： | 郭巍巍,方业广,方遒,崔刚龙.邻羟基绿色荧光蛋白发色团光物理机理的理论研究[J].化学物理学报,2017,30(6):696-704. |
| |
| 作者姓名： | 郭巍巍 方业广 方遒 崔刚龙 |
| |
| 作者单位： | 北京师范大学化学学院, 理论与计算光化学教育部重点实验室, 北京 100875,北京师范大学化学学院, 理论与计算光化学教育部重点实验室, 北京 100875,北京师范大学化学学院, 理论与计算光化学教育部重点实验室, 北京 100875,北京师范大学化学学院, 理论与计算光化学教育部重点实验室, 北京 100875 |
| |
| 基金项目： | This work has been supported by the National Natural Science Foundation of China (No.21522302, No.21520102005, and No.21421003). |
| |
| 摘 要： |
|
| 收稿时间： | 2017/9/26 0:00:00 |
| 修稿时间： | 2017/10/30 0:00:00 |
Mechanistic Insights into the Photophysics of Ortho-hydroxyl GFP Core Chromophores |
| |
| Wei-wei Guo,Ye-guang Fang,Qiu Fang and Gang-long Cui.Mechanistic Insights into the Photophysics of Ortho-hydroxyl GFP Core Chromophores[J].Chinese Journal of Chemical Physics,2017,30(6):696-704. |
| |
| Authors: | Wei-wei Guo Ye-guang Fang Qiu Fang and Gang-long Cui |
| |
| Institution: | Key Laboratory of Theoretical and Computational Photochemistry, Ministry of Education, College of Chemistry, Beijing Normal University, Beijing 100875, China,Key Laboratory of Theoretical and Computational Photochemistry, Ministry of Education, College of Chemistry, Beijing Normal University, Beijing 100875, China,Key Laboratory of Theoretical and Computational Photochemistry, Ministry of Education, College of Chemistry, Beijing Normal University, Beijing 100875, China and Key Laboratory of Theoretical and Computational Photochemistry, Ministry of Education, College of Chemistry, Beijing Normal University, Beijing 100875, China |
| |
| Abstract: | Herein we have employed the MS-CASPT2//CASSCF method to study the S1 excited-state intramolecular proton transfers (ESIPTs) of recently synthesized ortho-hydroxyl GFP core chromophores, i.e. OHIM, CHBDI, and MHBID, and their excited-state relaxation pathways. We have found that in OHIM and CHBDI, the ESIPT process is associated with small barriers of 3.4 and 4.2 kcal/mol; while, in MHBDI, it becomes essentially barrierless. Moreover, we have found two main S1 excited-state radiationless channels. In the first one, the enol S1 species decays to the S0 state via the enol S1/S0 conical intersection after overcoming considerable barriers of 7.0 and 7.7 kcal/mol in OHIM and CHBDI (however, in MHBDI, it is nearly barrierless). In the second one, the keto S1 species is first generated through the ESIPT event; then, it is de-excited into the S0 state in the vicinity of the keto S1/S0 conical intersection. These energetically allowed excited-state decay channels rationalize experimentally observed ultralow fluorescence quantum yields. The insights gained from the present work may help to guide the design of new ortho-hydroxyl GFP core chromophores with improved fluorescence emission and brightness. |
| |
| Keywords: | Excited states Mechanism Conical intersections GFP chromophores |
|
| 点击此处可从《化学物理学报》浏览原始摘要信息 |
| 点击此处可从《化学物理学报》下载免费的PDF全文 |
|
