Control of Protonated Schiff Base Excited State Decay within Visual Protein Mimics: A Unified Model for Retinal Chromophores.
QM/MM methods
excited state dynamics
retinal Schiff base
rhodopsin mimics
ultrafast optical spectroscopy
Journal
Chemistry (Weinheim an der Bergstrasse, Germany)
ISSN: 1521-3765
Titre abrégé: Chemistry
Pays: Germany
ID NLM: 9513783
Informations de publication
Date de publication:
25 Nov 2021
25 Nov 2021
Historique:
received:
02
07
2021
pubmed:
16
10
2021
medline:
15
12
2021
entrez:
15
10
2021
Statut:
ppublish
Résumé
Artificial biomimetic chromophore-protein complexes inspired by natural visual pigments can feature color tunability across the full visible spectrum. However, control of excited state dynamics of the retinal chromophore, which is of paramount importance for technological applications, is lacking due to its complex and subtle photophysics/photochemistry. Here, ultrafast transient absorption spectroscopy and quantum mechanics/molecular mechanics simulations are combined for the study of highly tunable rhodopsin mimics, as compared to retinal chromophores in solution. Conical intersections and transient fluorescent intermediates are identified with atomistic resolution, providing unambiguous assignment of their ultrafast excited state absorption features. The results point out that the electrostatic environment of the chromophore, modified by protein point mutations, affects its excited state properties allowing control of its photophysics with same power of chemical modifications of the chromophore. The complex nature of such fine control is a fundamental knowledge for the design of bio-mimetic opto-electronic and photonic devices.
Identifiants
pubmed: 34653286
doi: 10.1002/chem.202102383
pmc: PMC8906800
mid: NIHMS1754295
doi:
Substances chimiques
Schiff Bases
0
Rhodopsin
9009-81-8
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM
Pagination
16389-16400Subventions
Organisme : NIGMS NIH HHS
ID : R01 GM101353
Pays : United States
Organisme : NIH HHS
ID : GM101353
Pays : United States
Organisme : école normale supérieure
ID : MI-LOURD-FR15
Informations de copyright
© 2021 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH.
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