Inorganic Chemistry · 2019 · 22 citations · 61 references
Natural SciencesChemistryMolecular RecognitionPolymer ChemistrySupramolecular ChemistryChiral RecognitionCoordination PolymersMacromolecular AssemblySelf-assemblySupramolecular MaterialsSupramolecular PolymersChiral Host InteractionsChiralityConfiguration At Chiral CentersHost-guest Supramolecular PolymersOptical PropertiesPorphyrin ComplexesSupramolecular ComplexationSupramolecular Polymerization
A clear and unambiguous rationalization of chirality induction, amplification, and subsequent inversion processes has been demonstrated using an achiral Mg(II)porphyrin dimer (host) and a series of chiral diols (guests) upon stepwise formation of a 1:1 host–guest polymer and 1:2 host–guest monomer via intermolecular assembling and disassembling processes. Crystallographic characterizations are reported here for both the polymer and the monomeric complexes, which enable us to completely scrutinize the structural and geometrical changes systematically in rationalizing their optical properties. The sign of the CD couplets for both the polymer and monomer are just opposite between R and S guests, which suggests that the chirality is dictated solely by the stereogenic projection of the chiral centers. Stronger intra- and intermolecular coupling in the polymeric complexes is responsible for the highly enhanced CD couplets as compared to the monomer and have only intramolecular coupling as also observed in their X-ray structures. DFT studies clearly support the experimental observations.
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Density-functional thermochemistry. III. The role of exact exchange
Axel D. Becke · The Journal of Chemical Physics · 1993 · 102.8K citations
Natural Sciences, Chemistry, Physics +13