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DOI10.1073/PNAS.2001114117
Revealing the origin of multiphasic dynamic behaviors in cyanobacteriochrome
Wang D.; Li X.; Zhang S.; Wang L.; Yang X.; Zhong D.
发表日期2020
ISSN0027-8424
起始页码19731
结束页码19736
卷号117期号:33
英文摘要Cyanobacteriochromes are photoreceptors in cyanobacteria that exhibit a wide spectral coverage and unique photophysical properties from the photoinduced isomerization of a linear tetrapyrrole chromophore. Here, we integrate femtosecond-resolved fluorescence and transient-absorption methods and unambiguously showed the significant solvation dynamics occurring at the active site from a few to hundreds of picoseconds. These motions of local water molecules and polar side chains are continuously convoluted with the isomerization reaction, leading to a nonequilibrium processes with continuous active-site motions. By mutations of critical residues at the active site, the modified local structures become looser, resulting in faster solvation relaxations and isomerization reaction. The observation of solvation dynamics is significant and critical to the correct interpretation of often-observed multiphasic dynamic behaviors, and thus the previously invoked ground-state heterogeneity may not be relevant to the excited-state isomerization reaction. © 2020 National Academy of Sciences. All rights reserved.
英文关键词Active-site relaxation; Conical intersection; Double-bond twisting; Femtosecond spectroscopy; Site-directed mutation
语种英语
scopus关键词phytochrome; bacterial protein; visual proteins and pigments; absorption; Article; binding site; controlled study; cyanobacterium; excitation; fluorescence analysis; hydrogen bond; isomerization; molecular dynamics; nonhuman; photoreceptor; priority journal; solvation; steady state; surface property; chemistry; cyanobacterium; enzyme active site; genetics; isomerism; kinetics; metabolism; Bacterial Proteins; Catalytic Domain; Cyanobacteria; Isomerism; Kinetics; Photoreceptors, Microbial
来源期刊Proceedings of the National Academy of Sciences of the United States of America
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/160247
作者单位Wang, D., Department of Physics, Ohio State University, Columbus, OH 43210, United States, Program of Biochemistry, Ohio State University, Columbus, OH 43210, United States; Li, X., Department of Physics, Ohio State University, Columbus, OH 43210, United States, Department of Chemistry and Biochemistry, Ohio State University, Columbus, OH 43210, United States; Zhang, S., Department of Physics, Ohio State University, Columbus, OH 43210, United States; Wang, L., Department of Physics, Ohio State University, Columbus, OH 43210, United States; Yang, X., Department of Chemistry, University of Illinois at Chicago, Chicago, IL 60607, United States; Zhong, D., Department of Physics, Ohio State University, Columbus, OH 43210, United States, Program of Biochemistry, Ohio State University, Columbus, OH 43210, United States, Department of Chemistry and Biochemistry, Ohio State University, Columbus, OH 43210, United States, Program of Biophysics, Ohio State University, Columbus, OH 43210, United States, Pro...
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Wang D.,Li X.,Zhang S.,et al. Revealing the origin of multiphasic dynamic behaviors in cyanobacteriochrome[J],2020,117(33).
APA Wang D.,Li X.,Zhang S.,Wang L.,Yang X.,&Zhong D..(2020).Revealing the origin of multiphasic dynamic behaviors in cyanobacteriochrome.Proceedings of the National Academy of Sciences of the United States of America,117(33).
MLA Wang D.,et al."Revealing the origin of multiphasic dynamic behaviors in cyanobacteriochrome".Proceedings of the National Academy of Sciences of the United States of America 117.33(2020).
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