A photo-switchable molecular capsule: ...
Document type :
Article dans une revue scientifique: Article original
DOI :
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Title :
A photo-switchable molecular capsule: sequential photoinduced processes
Author(s) :
Choudhari, Manjiri [Auteur]
Monash University [Clayton]
Xu, Jingjing [Auteur]
Monash University [Clayton]
Shanghai Normal University [SHNU]
Mckay, Alasdair I. [Auteur]
Monash University [Clayton]
Guerrin, Clement [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
Forsyth, Craig [Auteur]
Monash University [Clayton]
Ma, Howard Z. [Auteur]
University of Melbourne
Goerigk, Lars [Auteur]
University of Melbourne
O'hair, Richard A. J. [Auteur]
University of Melbourne
Bonnefont, Antoine [Auteur]
Laboratoire d'Electrochimie et de Chimie Physique du Corps Solide
Ruhlmann, Laurent [Auteur]
Laboratoire d'Electrochimie et de Chimie Physique du Corps Solide
Aloise, Stephane [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
Ritchie, Chris [Auteur]
Monash University [Clayton]
Monash University [Clayton]
Xu, Jingjing [Auteur]
Monash University [Clayton]
Shanghai Normal University [SHNU]
Mckay, Alasdair I. [Auteur]
Monash University [Clayton]
Guerrin, Clement [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
Forsyth, Craig [Auteur]
Monash University [Clayton]
Ma, Howard Z. [Auteur]
University of Melbourne
Goerigk, Lars [Auteur]
University of Melbourne
O'hair, Richard A. J. [Auteur]
University of Melbourne
Bonnefont, Antoine [Auteur]
Laboratoire d'Electrochimie et de Chimie Physique du Corps Solide
Ruhlmann, Laurent [Auteur]
Laboratoire d'Electrochimie et de Chimie Physique du Corps Solide
Aloise, Stephane [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
Ritchie, Chris [Auteur]
Monash University [Clayton]
Journal title :
Chemical Science
Abbreviated title :
Chem. Sci.
Volume number :
46
Pages :
13732-13740
Publication date :
2022-12-04
ISSN :
2041-6520
HAL domain(s) :
Chimie/Chimie théorique et/ou physique
English abstract : [en]
The metastable trilacunary heteropolyoxomolybdate [PMo9O31(py)3]3− – {PMo9}; py = pyridine) and the ditopic pyridyl bearing diarylethene (DAE) (C25H16N2F6S2) self-assemble via a facile ligand replacement methodology to ...
Show more >The metastable trilacunary heteropolyoxomolybdate [PMo9O31(py)3]3− – {PMo9}; py = pyridine) and the ditopic pyridyl bearing diarylethene (DAE) (C25H16N2F6S2) self-assemble via a facile ligand replacement methodology to yield the photo-active molecular capsule [(PMo9O31)2(DAE)3]6−. The spatial arrangement and conformation of the three DAE ligands are directed by the surface chemistry of the molecular metal oxide precursor with exclusive ligation of the photo-active antiparallel rotamer to the polyoxometalate (POM) while the integrity of the assembly in solution has been verified by a suite of spectroscopic techniques. Electrocyclisation of the three DAEs occurs sequentially and has been investigated using a combination of steady-state and time-resolved spectroscopies with the discovery of a photochemical cascade whereby rapid photoinduced ring closure is followed by electron transfer from the ring-closed DAE to the POM in the latent donor–acceptor system on subsequent excitation. This interpretation is also supported by computational and detailed spectroelectrochemical analysis. Ring-closing quantum yields were also determined using a custom quantum yield determination setup (QYDS), providing insight into the impact of POM coordination on these processes.Show less >
Show more >The metastable trilacunary heteropolyoxomolybdate [PMo9O31(py)3]3− – {PMo9}; py = pyridine) and the ditopic pyridyl bearing diarylethene (DAE) (C25H16N2F6S2) self-assemble via a facile ligand replacement methodology to yield the photo-active molecular capsule [(PMo9O31)2(DAE)3]6−. The spatial arrangement and conformation of the three DAE ligands are directed by the surface chemistry of the molecular metal oxide precursor with exclusive ligation of the photo-active antiparallel rotamer to the polyoxometalate (POM) while the integrity of the assembly in solution has been verified by a suite of spectroscopic techniques. Electrocyclisation of the three DAEs occurs sequentially and has been investigated using a combination of steady-state and time-resolved spectroscopies with the discovery of a photochemical cascade whereby rapid photoinduced ring closure is followed by electron transfer from the ring-closed DAE to the POM in the latent donor–acceptor system on subsequent excitation. This interpretation is also supported by computational and detailed spectroelectrochemical analysis. Ring-closing quantum yields were also determined using a custom quantum yield determination setup (QYDS), providing insight into the impact of POM coordination on these processes.Show less >
Language :
Anglais
Peer reviewed article :
Oui
Audience :
Internationale
Popular science :
Non
Administrative institution(s) :
Université de Lille
CNRS
CNRS
Collections :
Submission date :
2024-02-28T22:15:13Z
2024-03-18T12:43:37Z
2024-03-18T12:43:37Z
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