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• W147563006 abstract "A series of compounds which utilise the macrocycle, trans-6, 13-dimethyl-n1,4,8,11-tetraazacyclotetradecane-6,13-diamine, L1 as a linker between a photoactivenchromophore and an appropriate energy or electron donor have been synthesised andntheir properties explored by a combination of both steady state and time resolvednphotophysical measurements. Corresponding model compounds of the parentnmacrocycle with a single photoactive component were also prepared. In their freenbase forms, these ligands display pronounced photoactivity, undergoingnintramolecular photoinduced electron transfer reactions which efficiently quench thenemission. Upon complexation with Zn(II), the characteristic fluorescence of thenchromophore is revived to a varying extent, dependant on the oxidising potential ofnthe excited state.n n For the purpose of studying intramolecular electronic energy migration, thensymmetrically disubstituted compounds of L1 with the naphthalene and anthracenenchromophores were prepared. In their free base forms, the photophysical behaviour ofnthese ligands was analogous to the model compounds. As their Zn(II) complexes,nemission from the chromophore is revived, although the electronic coupling betweennchromophores was ineffective in promoting energy migration.n n The asymmetrically disubstituted compounds of L1 with the naphthalene,nanthracene and pyrene chromophores were prepared in order to study intramolecularnelectronic energy transfer (EET). In complex with Zn(II), steady state measurementsnhave established the electronic coupling between chromophores in this case wasnsufficient to promote EET. Time resolved measurements, together with molecularnmechanics calculations, have allowed an identification of this coupling as primarily Coulombic, and the kinetics of the energy transfer process are well approximated bynthe Forster mechanism for dipole-dipole interactions.n n For the purpose of studying intramolecular photoinduced electron transfern(PET), ligands incorporating the naphthalene or anthracene chromophore inncombination with the organic or organometallic electron donors, dimethylaniline andnferrocene, were prepared. For Zn(II) complexes of the former ligands, only limitednevidence of PET activity was observed, manifest as a moderate reduction in theirnexcited state lifetimes compared to model complexes. This lack of PET activity wasnattributed to inefficient electronic coupling induced by the remoteness of the donornacceptor pair, and the absence of an operant through-bond pathway. For the latterncomplexes, with ferrocene as the electron donor, efficient excited state deactivationnwas observed, but the mechanism in this case was attributed to energy transfer.n" @default.
• W147563006 created "2016-06-24" @default.
• W147563006 creator A5057877864 @default.
• W147563006 date "2004-01-01" @default.
• W147563006 modified "2023-09-26" @default.
• W147563006 title "A macrocyclic scaffold for electronic energy transfer and photoinduced electron transfer" @default.
• W147563006 hasPublicationYear "2004" @default.
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