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Dynamic Stark Effect in Two-Dimensional Spectroscopy Revealing Modulation of Ultrafast Charge Separation in Bacterial Reaction Centers by an Inherent Electric Field

文献类型:期刊论文

作者Ma, Fei; Romero, Elisabet5; Jones, Michael R.; Novoderezhkin, Vladimir, I3; Yu, Long-Jiang; van Grondelle, Rienk
刊名JOURNAL OF PHYSICAL CHEMISTRY LETTERS
出版日期2021
卷号12期号:23页码:5526-5533
ISSN号1948-7185
DOI10.1021/acs.jpclett.1c01059
文献子类Article
英文摘要Despite extensive study, mysteries remain regarding the highly efficient ultrafast charge separation processes in photosynthetic reaction centers (RCs). In this work, transient Stark signals were found to be present in ultrafast two-dimensional electronic spectra recorded for purple bacterial RCs at 77 K. These arose from the electric field that is inherent to the intradimer charge-transfer intermediate of the bacteriochlorophyll pair (P), PA+PB-. By comparing three mutated RCs, a correlation was found between the efficient formation of PA+PB- and a fast charge separation rate. Importantly, the energy level of P* was changed due to the Stark shift, influencing the driving force for P* -> P+BA- electron transfer and hence its rate. Furthermore, the orientation and amplitude of the inherent electric field varied in different ways upon different mutation, leading to contrasting changes in the rates. This mechanism of modulation provides a solution to a long-lasting inconsistency between experimental observations and activation energy theory.
学科主题Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Atomic, Molecular & Chemical
出版地WASHINGTON
WOS关键词PHOTOSYNTHETIC REACTION CENTERS ; MUTANT REACTION CENTERS ; RHODOBACTER-SPHAEROIDES ; WATER MOLECULE ; WILD-TYPE ; KINETICS ; ABSORPTION ; STATES ; MECHANISM ; EXCITON
WOS研究方向Science Citation Index Expanded (SCI-EXPANDED)
语种英语
出版者AMER CHEMICAL SOC
WOS记录号WOS:000664329300013
资助机构Natural Science Foundation of China [21903086] ; National Key R&D Program of China [2019YFA0904600] ; European Research Council through an Advanced Investigator grant [267333] ; Biotechnology and Biological Sciences Research Council of the U.K. [BB/I022570/1] ; Russian Foundation for Basic Research [18-04-00105]
源URL[http://ir.ibcas.ac.cn/handle/2S10CLM1/26467]  
专题中科院光生物学重点实验室
作者单位1.Barcelona Inst Sci & Technol, Inst Chem Res Catalonia, Av Paisos Catalans 16, Tarragona 43007, Spain
2.Moscow MV Lomonosov State Univ, AN Belozersky Inst Phys Chem Biol, Moscow 119992, Russia
3.Jones, Michael R.] Univ Bristol, Sch Biochem, Bristol BS8 1TD, Avon, England
4.Chinese Acad Sci, Inst Bot, Key Lab Photo Biol, Beijing 100093, Peoples R China
5.Vrije Univ Amsterdam, Fac Sci, Dept Biophys, NL-1081 HV Amsterdam, Netherlands
推荐引用方式
GB/T 7714
Ma, Fei,Romero, Elisabet,Jones, Michael R.,et al. Dynamic Stark Effect in Two-Dimensional Spectroscopy Revealing Modulation of Ultrafast Charge Separation in Bacterial Reaction Centers by an Inherent Electric Field[J]. JOURNAL OF PHYSICAL CHEMISTRY LETTERS,2021,12(23):5526-5533.
APA Ma, Fei,Romero, Elisabet,Jones, Michael R.,Novoderezhkin, Vladimir, I,Yu, Long-Jiang,&van Grondelle, Rienk.(2021).Dynamic Stark Effect in Two-Dimensional Spectroscopy Revealing Modulation of Ultrafast Charge Separation in Bacterial Reaction Centers by an Inherent Electric Field.JOURNAL OF PHYSICAL CHEMISTRY LETTERS,12(23),5526-5533.
MLA Ma, Fei,et al."Dynamic Stark Effect in Two-Dimensional Spectroscopy Revealing Modulation of Ultrafast Charge Separation in Bacterial Reaction Centers by an Inherent Electric Field".JOURNAL OF PHYSICAL CHEMISTRY LETTERS 12.23(2021):5526-5533.

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来源:植物研究所

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