Optical control of ultrafast structural dynamics in a fluorescent protein
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Published:2023-08-10
Issue:11
Volume:15
Page:1607-1615
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ISSN:1755-4330
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Container-title:Nature Chemistry
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language:en
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Short-container-title:Nat. Chem.
Author:
Hutchison Christopher D. M., Baxter James M.ORCID, Fitzpatrick AnnORCID, Dorlhiac Gabriel, Fadini AlisiaORCID, Perrett SamuelORCID, Maghlaoui Karim, Lefèvre Salomé BodetORCID, Cordon-Preciado VioletaORCID, Ferreira Josie L., Chukhutsina Volha U., Garratt DouglasORCID, Barnard Jonathan, Galinis GediminasORCID, Glencross Flo, Morgan Rhodri M.ORCID, Stockton Sian, Taylor Ben, Yuan Letong, Romei Matthew G., Lin Chi-YunORCID, Marangos Jon P.ORCID, Schmidt MariusORCID, Chatrchyan ViktoriaORCID, Buckup TiagoORCID, Morozov DmitryORCID, Park JaehyunORCID, Park Sehan, Eom Intae, Kim Minseok, Jang DogeunORCID, Choi Hyeongi, Hyun HyoJungORCID, Park Gisu, Nango Eriko, Tanaka RieORCID, Owada Shigeki, Tono KensukeORCID, DePonte Daniel P., Carbajo SergioORCID, Seaberg MattORCID, Aquila AndrewORCID, Boutet SebastienORCID, Barty Anton, Iwata SoORCID, Boxer Steven G.ORCID, Groenhof GerritORCID, van Thor Jasper J.ORCID
Abstract
AbstractThe photoisomerization reaction of a fluorescent protein chromophore occurs on the ultrafast timescale. The structural dynamics that result from femtosecond optical excitation have contributions from vibrational and electronic processes and from reaction dynamics that involve the crossing through a conical intersection. The creation and progression of the ultrafast structural dynamics strongly depends on optical and molecular parameters. When using X-ray crystallography as a probe of ultrafast dynamics, the origin of the observed nuclear motions is not known. Now, high-resolution pump–probe X-ray crystallography reveals complex sub-ångström, ultrafast motions and hydrogen-bonding rearrangements in the active site of a fluorescent protein. However, we demonstrate that the measured motions are not part of the photoisomerization reaction but instead arise from impulsively driven coherent vibrational processes in the electronic ground state. A coherent-control experiment using a two-colour and two-pulse optical excitation strongly amplifies the X-ray crystallographic difference density, while it fully depletes the photoisomerization process. A coherent control mechanism was tested and confirmed the wave packets assignment.
Publisher
Springer Science and Business Media LLC
Subject
General Chemical Engineering,General Chemistry
Reference64 articles.
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