Kari Pederson - Solid-State Nuclear Magnetic Resonance Spectroscopy Studies of Furanose Ring Dynamics in the DNA HhaI Binding Site

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      Publication Details (including relevant citation   information):

      Meints, G. A.; Miller, P. A.; Pederson, K.; Shajani, Z.; Drobny,   G. P. J. Am. Chem. Soc. 2008, 130, 7305-7314.


      The dynamics of the furanose rings in the GCGC moiety of the DNA   oligomer   [d(G1A2T3A4G5C6G7C8T9A10T11C12)]2  are studied using deuterium solid-state NMR (SSNMR). SSNMR   spectra obtained from DNAs selectively deuterated on the furanose   rings of nucleotides within the 5'-GCGC-3' moiety indicated that   all of these positions are structurally flexible. The furanose   ring within the deoxycytidine that is the methylation target   displays the largest amplitude structural changes according to   the observed deuterium NMR lineshapes while the furanose rings of   nucleotides more remote from the methylation site have less   mobile furanose rings  (i.e. with puckering amplitudes <   0.3 Å). Previous work has shown that methylation reduces the   amplitude of motion in the phosphodiester backbone of the same   DNA, and our observations indicate that methylation perturbs   backbone dynamics through the furanose ring. These NMR data   indicate that the 5'-GCGC-3' is dynamic, with the largest   amplitude motions occurring nearest the methylation site. The   inherent flexibility of this moiety in DNA makes the molecule   more amenable to the large amplitude structural rearrangements   that must occur when the DNA binds to the HhaI   methyltransferase.

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