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Femtosecond-to-nanosecond dynamics of flavin mononucleotide monitored by stimulated Raman spectroscopy and simulations
- 1.0538485 - BTÚ 2021 RIV GB eng J - Journal Article
Andrikopoulos, Prokopis C. - Liu, Yingliang - Picchiotti, Alessandra - Lenngren, Nils - Kloz, Miroslav - Chaudhari, Aditya S. - Přeček, Martin - Rebarz, Mateusz - Andreasson, Jakob - Hajdu, Janos - Schneider, Bohdan - Fuertes, Gustavo
Femtosecond-to-nanosecond dynamics of flavin mononucleotide monitored by stimulated Raman spectroscopy and simulations.
Physical Chemistry Chemical Physics. Roč. 22, č. 12 (2020), s. 6538-6552. ISSN 1463-9076. E-ISSN 1463-9084
R&D Projects: GA MŠMT EF16_019/0000789; GA MŠMT EF15_003/0000447; GA MŠMT LQ1606; GA MŠMT(CZ) LM2015043; GA MŠMT(CZ) LM2015047
Research Infrastructure: ELI Beamlines III - 90141
Institutional support: RVO:86652036 ; RVO:68378271
Keywords : adenine-dinucleotide fad * excited-state * electron-transfer
OECD category: Physical chemistry; Physical chemistry (FZU-D)
Impact factor: 3.676, year: 2020
Method of publishing: Limited access
https://pubs.rsc.org/en/content/articlelanding/2020/CP/C9CP04918E#!divAbstract
Flavin mononucleotide (FMN) belongs to the large family of flavins, ubiquitous yellow-coloured biological chromophores that contain an isoalloxazine ring system. As a cofactor in flavoproteins, it is found in various enzymes and photosensory receptors, like those featuring the light-oxygen-voltage (LOV) domain. The photocycle of FMN is triggered by blue light and proceeds via a cascade of intermediate states. In this work, we have studied isolated FMN in an aqueous solution in order to elucidate the intrinsic electronic and vibrational changes of the chromophore upon excitation. The ultrafast transitions of excited FMN were monitored through the joint use of femtosecond stimulated Raman spectroscopy (FSRS) and transient absorption spectroscopy encompassing a time window between 0 ps and 6 ns with 50 fs time resolution. Global analysis of the obtained transient visible absorption and transient Raman spectra in combination with extensive quantum chemistry calculations identified unambiguously the singlet and triplet FMN populations and addressed solvent dynamics effects. The good agreement between the experimental and theoretical spectra facilitated the assignment of electronic transitions and vibrations. Our results represent the first steps towards more complex experiments aimed at tracking structural changes of FMN embedded in light-inducible proteins upon photoexcitation.
Permanent Link: http://hdl.handle.net/11104/0316287
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