Effect of GC-termini on the self-assembly of G-quadruplexes
Ilc, Tina ...
Recent studies show that some guanine-rich oligonucleotides with GC termini are able to form prolonged G-quadruplex-based superstructures termed G-wires. The unperturbed quadruplex stem and length of ...these G-wires as wellas their mechanical and thermal stability on solid substrates make them very promising candidates for molecular electronic devices. Our previous investigations show that oligonucleotide with the sequence GCGGTG4TGGCG isa possible candidate for G-wire formation. The proposed folding conformation of this oligonucleotide is illustrated in Figure 1. The GC ends, located at each side of the core, presumably link the quadruplexes to each other into G-wire structures via formation of (G:C:G:C) tetrads. To obtain more insight into the self-assembly mechanism and assess the validity of our model, we investigated four analogous oligonucleotides: the above denoted one and analogues with either 5', 3' or both GC-ends missing. The results of UV-melting experiments revealed that the GC-ends contribute greatly to the thermal stability of the G-quadruplexes (Figure 1). However, the GC-ends appear to hinder the formation of larger structures, as shown by the results of a dynamic light scattering study (Figure 2). Of all four oligonucleotides only the one without GC-ends formed larger structures, consisting of up to 14 stacked quadruplexes, based on rod-like particle approximation. Presumably the driving force behind the aggregation is base stacking of the terminal G-quartets. Formation and growth of G-wires from oligonucleotides with GC-termini require formation of the (G:C:G:C) tetrads on both 5' and 3'-ends. NMR results suggest that the (G:C:G:C)-tetrads can only link two G-quadruplexes via their 5'-ends but not via 3'-ends. Therefore the formation of long G-wires via (G:C:G:C)-linkages is not feasible under the investigated experimental conditions.
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