TY  - JOUR
A1  - Fischer, Tobias
A1  - Wilderen, Luuk J. G. W. van
A1  - Gnau, Petra
A1  - Bredenbeck, Jens
A1  - Essen, Lars-Oliver
A1  - Wachtveitl, Josef
A1  - Slavov, Chavdar
T1  - Ultrafast photoconversion dynamics of the knotless phytochrome SynCph2
T2  - International journal of molecular sciences
N2  - The family of phytochrome photoreceptors contains proteins with different domain architectures and spectral properties. Knotless phytochromes are one of the three main subgroups classified by their distinct lack of the PAS domain in their photosensory core module, which is in contrast to the canonical PAS-GAF-PHY array. Despite intensive research on the ultrafast photodynamics of phytochromes, little is known about the primary kinetics in knotless phytochromes. Here, we present the ultrafast Pr ⇆ Pfr photodynamics of SynCph2, the best-known knotless phytochrome. Our results show that the excited state lifetime of Pr* (~200 ps) is similar to bacteriophytochromes, but much longer than in most canonical phytochromes. We assign the slow Pr* kinetics to relaxation processes of the chromophore-binding pocket that controls the bilin chromophore’s isomerization step. The Pfr photoconversion dynamics starts with a faster excited state relaxation than in canonical phytochromes, but, despite the differences in the respective domain architectures, proceeds via similar ground state intermediate steps up to Meta-F. Based on our observations, we propose that the kinetic features and overall dynamics of the ultrafast photoreaction are determined to a great extent by the geometrical context (i.e., available space and flexibility) within the binding pocket, while the general reaction steps following the photoexcitation are most likely conserved among the red/far-red phytochromes.
KW  - tetrapyrrole-binding photoreceptors
KW  - phytochromes
KW  - photochemistry
KW  - photoisomerization
KW  - time-resolved spectroscopy
Y1  - 2021
UR  - http://publikationen.ub.uni-frankfurt.de/frontdoor/index/index/docId/63394
UR  - https://nbn-resolving.org/urn:nbn:de:hebis:30:3-633944
SN  - 1422-0067
N1  - This research was funded by the Deutsche Forschungsgemeinschaft (WA 1850/4-3, ES152/21). J.B. thanks the Alexander von Humboldt Foundation for a Sofia Kovalevskaja Award and the Deutsche Forschungsgemeinschaft for funding (No. INST 161/722-1 FUGG).
VL  - 22
IS  - 19, art. 10690
SP  - 1
EP  - 15
PB  - Molecular Diversity Preservation International
CY  - Basel
ER  -