Open Access
Stalling chromophore synthesis of the fluorescent protein Venus reveals the molecular basis of the final oxidation step
Husam Sabah Auhim
1, 2
,
Bella Grigorenko
3, 4
,
Bella L Grigorenko
5, 6, 7, 8, 9
,
Tessa K Harris
1, 10, 11, 12, 13, 14
,
Ozan E Aksakal
1, 10, 11, 12, 13, 14
,
Igor V. Polyakov
3, 4, 5, 6, 7, 8, 9
,
Colin Berry
1, 10, 11, 12, 13, 14
,
Gabriel Dos Passos Gomes
15, 16, 17, 18, 19, 20, 21
,
Igor V. Alabugin
22, 23, 24, 25, 26
,
Pierre J. Rizkallah
12, 14, 27, 28
,
Alexander Nemukhin
3, 4, 5, 6, 7, 8, 9
,
D. Dafydd Jones
1, 10, 11, 12, 13, 14
4
5
Chemistry department
7
Moscow
8
RUSSIAN FEDERATION
|
10
School of BioSciences
11
Molecular Biosciences Division
13
CARDIFF
|
14
UK
|
15
17
DEPARTMENT OF CHEMISTRY
18
University of Toronto
|
19
Toronto
|
20
CANADA
|
21
DEPARTMENT OF COMPUTER SCIENCE
23
Department of Chemistry and Biochemistry
25
Tallahassee
|
26
Usa
|
28
School of Medicine
Publication type: Journal Article
Publication date: 2021-03-31
scimago Q1
wos Q1
SJR: 2.138
CiteScore: 12.6
Impact factor: 7.4
ISSN: 20416520, 20416539
PubMed ID:
34168826
General Chemistry
Abstract
Fluorescent proteins (FPs) have revolutionised the life sciences, but the mechanism of chromophore maturation is still not fully understood. Here we show that incorporation of a photo-responsive non-canonical amino acid within the chromophore stalls maturation of Venus, a yellow FP, at an intermediate stage; a crystal structure indicates the presence of O2 located above a dehydrated enolate form of the imidazolone ring, close to the strictly conserved Gly67 that occupies a twisted conformation. His148 adopts an “open” conformation so forming a channel that allows O2 access to the immature chromophore. Absorbance spectroscopy supported by QM/MM simulations suggests that the first oxidation step involves formation of a hydroperoxyl intermediate in conjunction with dehydrogenation of the methylene bridge. A fully conjugated mature chromophore is formed through release of H2O2, both in vitro and in vivo. The possibility of interrupting and photochemically restarting chromophore maturation and the mechanistic insights open up new approaches for engineering optically controlled fluorescent proteins.
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14
Total citations:
14
Citations from 2024:
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(53.84%)
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GOST
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Auhim H. S. et al. Stalling chromophore synthesis of the fluorescent protein Venus reveals the molecular basis of the final oxidation step // Chemical Science. 2021. Vol. 12. No. 22. pp. 7735-7745.
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Auhim H. S. et al. Stalling chromophore synthesis of the fluorescent protein Venus reveals the molecular basis of the final oxidation step // Chemical Science. 2021. Vol. 12. No. 22. pp. 7735-7745.
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TY - JOUR
DO - 10.1039/d0sc06693a
UR - https://xlink.rsc.org/?DOI=D0SC06693A
TI - Stalling chromophore synthesis of the fluorescent protein Venus reveals the molecular basis of the final oxidation step
T2 - Chemical Science
AU - Auhim, Husam Sabah
AU - Grigorenko, Bella
AU - Grigorenko, Bella L
AU - Harris, Tessa K
AU - Aksakal, Ozan E
AU - Polyakov, Igor V.
AU - Berry, Colin
AU - Gomes, Gabriel Dos Passos
AU - Alabugin, Igor V.
AU - Rizkallah, Pierre J.
AU - Nemukhin, Alexander
AU - Jones, D. Dafydd
PY - 2021
DA - 2021/03/31
PB - Royal Society of Chemistry (RSC)
SP - 7735-7745
IS - 22
VL - 12
PMID - 34168826
SN - 2041-6520
SN - 2041-6539
ER -
Cite this
BibTex (up to 50 authors)
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@article{2021_Auhim,
author = {Husam Sabah Auhim and Bella Grigorenko and Bella L Grigorenko and Tessa K Harris and Ozan E Aksakal and Igor V. Polyakov and Colin Berry and Gabriel Dos Passos Gomes and Igor V. Alabugin and Pierre J. Rizkallah and Alexander Nemukhin and D. Dafydd Jones and others},
title = {Stalling chromophore synthesis of the fluorescent protein Venus reveals the molecular basis of the final oxidation step},
journal = {Chemical Science},
year = {2021},
volume = {12},
publisher = {Royal Society of Chemistry (RSC)},
month = {mar},
url = {https://xlink.rsc.org/?DOI=D0SC06693A},
number = {22},
pages = {7735--7745},
doi = {10.1039/d0sc06693a}
}
Cite this
MLA
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Auhim, Husam Sabah, et al. “Stalling chromophore synthesis of the fluorescent protein Venus reveals the molecular basis of the final oxidation step.” Chemical Science, vol. 12, no. 22, Mar. 2021, pp. 7735-7745. https://xlink.rsc.org/?DOI=D0SC06693A.