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题名: Site-specific solvation of the photoexcited protochlorophyllide a in methanol: Formation of the hydrogen-bonded intermediate state induced by hydrogen-bond strengthening
作者: Zhao, Guang-Jiu1;  Han, Ke-Li1
通讯作者: 韩克利
刊名: BIOPHYSICAL JOURNAL
发表日期: 2008
DOI: 10.1529/biophysj.107.113738
卷: 94, 期:1, 页:38-46
收录类别: SCI
文章类型: Article
部门归属: 11
项目归属: 1101
产权排名: 1;1
WOS标题词: Science & Technology ;  Life Sciences & Biomedicine
类目[WOS]: Biophysics
研究领域[WOS]: Biophysics
英文摘要: The site-specific solvation of the photoexcited protochlorophyllide a ( Pchlide a) in methanol solvent was investigated using the time-dependent density functional theory method for the first time to our knowledge. The intermolecular site-specific coordination and hydrogen-bonding interactions between Pchlide a and methanol molecules play a very important role in the steady-state and time-resolved spectra. All the calculated absorption and fluorescence spectra of the isolated Pchlide a and its coordinated and hydrogen-bonded complexes with methanol demonstrate that the novel fluorescence shoulder at similar to 690 nm of Pchlide a in methanol should be ascribed to the coordinated and hydrogen-bonded Pchlide a-(MeOH) 4 complex. This coordinated and hydrogen-bonded complex can also account for the intermediate state found in the time-resolved spectroscopic studies. Herein, we have theoretically confirmed that the intermolecular coordination and hydrogen bonds between Pchlide a and methanol molecules can be strengthened in the electronically excited state of Pchlide a. Furthermore, the site-specific solvation of the photoexcited Pchlide a can be induced by the intermolecular coordination and hydrogen-bond strengthening upon photoexcitation. Then the hydrogen-bonded intermediate state is formed in 22-27 ps timescales after the site-specific solvation. All the steady-state and time-resolved spectral features of Pchlide a in different solvents can be explained by the formation of this hydrogen-bonded intermediate state after the site-specific solvation, which is induced by the coordination and hydrogen-bond strengthening.
关键词[WOS]: TIME-RESOLVED ABSORPTION ;  PI-STACKING INTERACTIONS ;  EXCITED-STATE ;  AB-INITIO ;  CHLOROPHYLL BIOSYNTHESIS ;  BIOLOGICAL MACROMOLECULES ;  ENZYMATIC CATALYSIS ;  ETIOPLAST MEMBRANES ;  MOLECULAR-DYNAMICS ;  VISIBLE ABSORPTION
语种: 英语
原文出处: 查看原文
WOS记录号: WOS:000251615800007
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/99917
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China

Recommended Citation:
Zhao, Guang-Jiu,Han, Ke-Li. Site-specific solvation of the photoexcited protochlorophyllide a in methanol: Formation of the hydrogen-bonded intermediate state induced by hydrogen-bond strengthening[J]. BIOPHYSICAL JOURNAL,2008,94(1):38-46.
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