Concerted dynamics of metallo-base pairs in an A/B-form helical transition

Olivia P. Schmidt, Simon Jurt, Silke Johannsen, Ashkan Karimi, Roland K. O. Sigel and Nathan W. Luedtke ()
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Olivia P. Schmidt: University of Zurich
Simon Jurt: University of Zurich
Silke Johannsen: University of Zurich
Ashkan Karimi: University of Zurich
Roland K. O. Sigel: University of Zurich
Nathan W. Luedtke: University of Zurich

Nature Communications, 2019, vol. 10, issue 1, 1-11

Abstract: Abstract Metal-mediated base pairs expand the repertoire of nucleic acid structures and dynamics. Here we report solution structures and dynamics of duplex DNA containing two all-natural C-HgII-T metallo base pairs separated by six canonical base pairs. NMR experiments reveal a 3:1 ratio of well-resolved structures in dynamic equilibrium. The major species contains two (N3)T-HgII-(N3)C base pairs in a predominantly B-form helix. The minor species contains (N3)T-HgII-(N4)C base pairs and greater A-form characteristics. Ten-fold different 1J coupling constants (15N,199Hg) are observed for (N3)C-HgII (114 Hz) versus (N4)C-HgII (1052 Hz) connectivities, reflecting differences in cytosine ionization and metal-bonding strengths. Dynamic interconversion between the two types of C-HgII-T base pairs are coupled to a global conformational exchange between the helices. These observations inspired the design of a repetitive DNA sequence capable of undergoing a global B-to-A-form helical transition upon adding HgII, demonstrating that C-HgII-T has unique switching potential in DNA-based materials and devices.

Date: 2019
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DOI: 10.1038/s41467-019-12440-x

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