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Hydrogen-Bond-Driven Synergistically Enhanced Hyperpolarizability: Chiral Coordination Polymers with Nonpolar Structures Exhibiting Unusually Strong Second-Harmonic Generation.

Joonhyuk KeeKang Min Ok
Published in: Angewandte Chemie (International ed. in English) (2021)
Four chiral coordination polymers (CPs), M[(S,S)-C14 H14 N2 O6 ] and M[(R,R)-C14 H14 N2 O6 ] (M=Zn or Cd), have been exclusively synthesized in high yields with the aid of newly designed chiral ligand under hydrothermal condition. The CPs crystallizing in the orthorhombic nonpolar space group, C2221 , reveal three-dimensional framework structures composed of MO4 tetrahedra and the corresponding homochiral linkers. Powder second-harmonic generation (SHG) measurements indicate that the nonpolar CPs reveal very strong SHG efficiency of ca. 5-9 times that of KH2 PO4 and exhibit type-I phase-matching behavior. Density functional theory calculations suggest that the unusually large SHG efficiency found from the nonpolar CPs should be attributable to the synergistic effect of polarizable metal cations and enhanced hyperpolarizability in the donor-acceptor system originating from the hydrogen bonding in the coordinated linkers.
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