School of Chemistry - Research Publications

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Author: O'Hair, Richard × Author: McKay, Alasdair × Author: Goerigk, Lars × Start date: 2020 × Type: Journal Article ×

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    A photo-switchable molecular capsule: sequential photoinduced processes
    Choudhari, M ; Xu, J ; McKay, A ; Guerrin, C ; Forsyth, C ; Ma, HZ ; Goerigk, L ; O'Hair, RAJ ; Bonnefont, A ; Ruhlmann, L ; Aloise, S ; Ritchie, C (ROYAL SOC CHEMISTRY, 2022-11-30)
    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.