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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 | |
Ma, Fei; Romero, Elisabet1; Jones, Michael R.; Novoderezhkin, Vladimir, I3; Yu, Long-Jiang; van Grondelle, Rienk | |
2021 | |
发表期刊 | JOURNAL OF PHYSICAL CHEMISTRY LETTERS |
ISSN | 1948-7185 |
卷号 | 12期号:23页码:5526-5533 |
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. |
学科领域 | Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Atomic, Molecular & Chemical |
DOI | 10.1021/acs.jpclett.1c01059 |
收录类别 | SCI |
语种 | 英语 |
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) |
WOS记录号 | WOS:000664329300013 |
出版者 | AMER CHEMICAL SOC |
文献子类 | Article |
出版地 | WASHINGTON |
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] |
作者邮箱 | fma@ibcas.ac.cn ; longer@ibcas.ac.cn |
作品OA属性 | Green Published, Green Submitted |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | 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.Vrije Univ Amsterdam, Fac Sci, Dept Biophys, NL-1081 HV Amsterdam, Netherlands 2.Barcelona Inst Sci & Technol, Inst Chem Res Catalonia, Av Paisos Catalans 16, Tarragona 43007, Spain 3.Jones, Michael R.] Univ Bristol, Sch Biochem, Bristol BS8 1TD, Avon, England 4.Moscow MV Lomonosov State Univ, AN Belozersky Inst Phys Chem Biol, Moscow 119992, Russia 5.Chinese Acad Sci, Inst Bot, Key Lab Photo Biol, Beijing 100093, Peoples R China |
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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