Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 14, Issue 10, Pages 2994-3005Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.200701465
Keywords
helical structures; multicomponent assembly; polynuclear; statistical factors; thermodynamics
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The contribution of the solvation energies to the assembly of polynuclear helicates reduces the free energy of intermetallic repulsion, Delta E-MM, in condensed phase to such an extent that stable D-3-symmetrical tetranuclear lanthanide-containing triple-stranded helicates [Ln(4)(L4)(3)](12+) are quantitatively produced at millimolar concentrations, despite the twelve positive charge borne by these complexes. A detailed modelling of the formation constants using statistical factors, adapted to self-assembly processes involving intra- and intermolecular connections, provides a set of five microscopic parameters, which can be successfully used for rationalizing the stepwise generation of linear bi-, tri- and tetranuclear analogues. Photophysical studies of [Eu-4(L4)(3)](12+) confirm the existence of two different binding sites producing differentiated metal-centred emission at low temperature, which transforms into single site luminescence at room temperature because of intramolecular energy funelling processes.
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