Engineering excitonically coupled dimers in an artificial protein for light harvesting via computational modeling.
artificial photosynthesis
cofactor binding
de novo protein design
molecular dynamics
Journal
Protein science : a publication of the Protein Society
ISSN: 1469-896X
Titre abrégé: Protein Sci
Pays: United States
ID NLM: 9211750
Informations de publication
Date de publication:
03 2023
03 2023
Historique:
revised:
23
01
2023
received:
15
11
2022
accepted:
25
01
2023
pubmed:
31
1
2023
medline:
3
3
2023
entrez:
30
1
2023
Statut:
ppublish
Résumé
In photosynthesis, pigment-protein complexes achieve outstanding photoinduced charge separation efficiencies through a set of strategies in which excited states delocalization over multiple pigments ("excitons") and charge-transfer states play key roles. These concepts, and their implementation in bioinspired artificial systems, are attracting increasing attention due to the vast potential that could be tapped by realizing efficient photochemical reactions. In particular, de novo designed proteins provide a diverse structural toolbox that can be used to manipulate the geometric and electronic properties of bound chromophore molecules. However, achieving excitonic and charge-transfer states requires closely spaced chromophores, a non-trivial aspect since a strong binding with the protein matrix needs to be maintained. Here, we show how a general-purpose artificial protein can be optimized via molecular dynamics simulations to improve its binding capacity of a chlorophyll derivative, achieving complexes in which chromophores form two closely spaced and strongly interacting dimers. Based on spectroscopy results and computational modeling, we demonstrate each dimer is excitonically coupled, and propose they display signatures of charge-transfer state mixing. This work could open new avenues for the rational design of chromophore-protein complexes with advanced functionalities.
Identifiants
pubmed: 36715022
doi: 10.1002/pro.4579
pmc: PMC9951196
doi:
Substances chimiques
Chlorophyll
1406-65-1
Light-Harvesting Protein Complexes
0
Types de publication
Journal Article
Research Support, Non-U.S. Gov't
Langues
eng
Sous-ensembles de citation
IM
Pagination
e4579Informations de copyright
© 2023 The Authors. Protein Science published by Wiley Periodicals LLC on behalf of The Protein Society.
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