Excited electronic states in DNA have long been of interest as the precursors of mutagenic photoproducts. During the past twenty years, pump-probe experiments using femtosecond UV, visible, and mid-IR pulses have provided unprecedented insight into the dynamics of electronic excitations in DNA. Thanks to synergistic advances in experiment and theory it is increasingly feasible to map deactivation pathways in multichromophoric assemblies of nucleobases such as those found in natural DNA strands. Excited states of DNA are also newly relevant to designing and optimizing DNA-based nanostructures for photonic applications. Although less familiar than hydrogen bonding and π-π stacking, metal coordination contributes to the rich and frequently reversible self-assembly and templating properties of DNA and its constituent nucleotides. Metal ions mediate new base pairing motifs, giving rise to new structures and imparting ‘metallic’ properties to DNA. Our recent studies of excited-state dynamics in self-assembled nanostructures formed from purine nucleobase monomers and silver(I) ions will be reported. Silver ions bind preferentially to the nucleobases, influencing excited state relaxation through the introduction of new states such as ligand-to-metal charge transfer states and through the formation of metal ion-mediated nanostructures.<br/>

Dynamics of excited electronic states in silver(I) complexes with DNA nucleobases and their self-assembled nanostructures

256th National Meeting (2018)

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