Four-Arm Oligonucleotide Ni(II)−Cyclam-Centered Complexes as Precursors for the Generation of Supramolecular Periodic Assemblies

Abstract

The development of a multiarm metal-centered DNA building block as a precursor for the construction of supramolecular assemblies has relied upon the preparation of a Ni(II)−1,4,8,11-tetrazacyclotetradecane ligand (cyclam) functionalized with four linkers. This complex can be incorporated into a support-bound DNA sequence and the remaining three linkers can then be elongated by DNA synthesis. The result is a Ni(II)−cyclam complex tethering four 20-mer DNA strands. This building block, designed to be tetrahedral in nature, can in principle be used to form tetrahedral assemblies. These assemblies can be designed to be of known size and composition or permitted to grow into complexes of essentially infinite size, ideally the macroscopic version of a crystal.