Mechanism of formation of supramolecular DNA-Templated polymer nanowires

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[1] Watson, Scott M. D.

[2] Galindo, Miguel A.

[3] Horrocks, Benjamin R.

[4] Houlton, Andrew

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Houlton, A. (andrew.houlton@ncl.ac.uk) | 1600年 / American Chemical Society卷 / 136期

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Details of the mechanism of formation of supramolecular polymer nanowires by templating on DNA are revealed for the first time using AFM. Overall these data reveal that the smooth; regular; structures produced are rendered by highly dynamic supramolecular transformations occurring over the micrometre scale. In the initial stages of the process a low density of conducting polymer (CP) binds to the DNA as; essentially; spherical particles. Further reaction time produces DNA strands which are more densely packed with particles giving a beads-on-a-string appearance. The particles subsequently undergo dynamic reconfiguration so as to elongate along the template axis and merge to yield the highly regular; smooth morphology of the final nanowire. MD simulations illustrate the early stages of the process showing the binding of globular CP to duplex DNA; while the latter stages can be modeled effectively by a linear thermodynamic description based on the balance between the line energy; which accounts for adhesion of the material to the template; and its surface tension. This model accounts for the phenomena observed in the AFM studies: the relative success of DNA templating of polymers compared to metals; the slow approach to equilibrium; and the observed thinning and necking phenomena as the structures transform from beads-on-a-string to smooth nanowire. © 2014 American Chemical Society;

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