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Hydrogen bonding between nucleobases produces diverse DNA structural motifs,including canonical duplexes, guanine (G) quadruplexes and cytosine (C)i-motifs. Incorporating metal-mediated base pairs into nucleic acid structurescan introduce new functionalities and enhanced stabilities. Here wedemonstrate, using mass spectrometry (MS), ion mobility spectrometry (IMS) andfluorescence resonance energy transfer (FRET), that parallel-strandedstructures consisting of up to 20 G-Ag(I)-G contiguous base pairs are formedwhen natural DNA sequences are mixed with silver cations in aqueous solution.FRET indicates that duplexes formed by poly(cytosine) strands with 20contiguous C-Ag(I)-C base pairs are also parallel. Silver-mediated G-duplexesform preferentially over G-quadruplexes, and the ability of Ag+ to convertG-quadruplexes into silver-paired duplexes may provide a new route tomanipulating these biologically relevant structures. IMS indicates thatG-duplexes are linear and more rigid than B-DNA. DFT calculations were used topropose structures compatible with the IMS experiments. Such inexpensive,defect-free and soluble DNA-based nanowires open new directions in the designof novel metal-mediated DNA nanotechnology.

Parallel G-duplex and C-duplex DNA with Uninterrupted Spines of AgI-Mediated Base Pairs