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邻羟基绿色荧光蛋白发色团光物理机理的理论研究
郭巍巍,方业广,方遒*,崔刚龙*
作者单位E-mail
郭巍巍 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  
方业广 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  
方遒* 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 fangqiu917@bnu.edu.cn 
崔刚龙* 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 ganglong.cui@bnu.edu.cn 
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DOI:10.1063/1674-0068/30/cjcp1709179
分类号:
基金项目:This work has been supported by the National Natural Science Foundation of China (No.21522302, No.21520102005, and No.21421003).
Mechanistic Insights into the Photophysics of Ortho-hydroxyl GFP Core Chromophores
Wei-wei Guo,Ye-guang Fang,Qiu Fang*,Gang-long Cui*
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.
Key words:  Excited states  Mechanism  Conical intersections  GFP chromophores