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Serial Femtosecond Crystallography Reveals that Photoactivation in a Fluorescent Protein Proceeds via the Hula Twist Mechanism

Publiceringsår

2023

Upphovspersoner

Fadini, Alisia; Hutchison, Christopher D. M.; Morozov, Dmitry; Chang, Jeffrey; Maghlaoui, Karim; Perrett, Samuel; Luo, Fangjia; Kho, Jeslyn C. X.; Romei, Matthew G.; Morgan, R. Marc L.; Orr, Christian M.; Cordon-Preciado, Violeta; Fujiwara, Takaaki; Nuemket, Nipawan; Tosha, Takehiko; Tanaka, Rie; Owada, Shigeki; Tono, Kensuke; Iwata, So; Boxer, Steven G.; Groenhof, Gerrit; Nango, Eriko; van Thor, Jasper J.
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Abstrakt

Chromophore cis/trans photoisomerization is a fundamental process in chemistry and in the activation of many photosensitive proteins. A major task is understanding the effect of the protein environment on the efficiency and direction of this reaction compared to what is observed in the gas and solution phases. In this study, we set out to visualize the hula twist (HT) mechanism in a fluorescent protein, which is hypothesized to be the preferred mechanism in a spatially constrained binding pocket. We use a chlorine substituent to break the twofold symmetry of the embedded phenolic group of the chromophore and unambiguously identify the HT primary photoproduct. Through serial femtosecond crystallography, we then track the photoreaction from femtoseconds to the microsecond regime. We observe signals for the photoisomerization of the chromophore as early as 300 fs, obtaining the first experimental structural evidence of the HT mechanism in a protein on its femtosecond-to-picosecond timescale. We are then able to follow how chromophore isomerization and twisting lead to secondary structure rearrangements of the protein β-barrel across the time window of our measurements.
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Organisationer och upphovspersoner

Jyväskylä universitet

Morozov Dmitry Orcid -palvelun logo

Groenhof Gerrit Orcid -palvelun logo

Publikationstyp

Publikationsform

Artikel

Moderpublikationens typ

Tidning

Artikelstyp

En originalartikel

Målgrupp

Vetenskaplig

Kollegialt utvärderad

Kollegialt utvärderad

UKM:s publikationstyp

A1 Originalartikel i en vetenskaplig tidskrift

Publikationskanalens uppgifter

Volym

145

Nummer

29

Sidor

15796-15808

Publikationsforum

61812

Publikationsforumsnivå

3

Öppen tillgång

Öppen tillgänglighet i förläggarens tjänst

Ja

Öppen tillgång till publikationskanalen

Delvis öppen publikationskanal

Parallellsparad

Ja

Övriga uppgifter

Vetenskapsområden

Kemi

Nyckelord

[object Object],[object Object],[object Object]

Publiceringsland

Förenta staterna (USA)

Förlagets internationalitet

Internationell

Språk

engelska

Internationell sampublikation

Ja

Sampublikation med ett företag

Nej

DOI

10.1021/jacs.3c02313

Publikationen ingår i undervisnings- och kulturministeriets datainsamling

Ja