6 research outputs found
Metallationâinduced heterogeneous dynamics of DNA revealed by singleâmolecule FRET
The metallation of nucleic acids is key to wideâranging applications, from anticancer medicine to nanomaterials, yet there is a lack of understanding of the molecularâlevel effects of metallation. Here, we apply singleâmolecule fluorescence methods to study the reaction of an organoâosmium anticancer complex and DNA. Individual metallated DNA hairpins are characterized using Förster resonance energy transfer (FRET). Although ensemble measurements suggest a simple twoâstate system, singleâmolecule experiments reveal an underlying heterogeneity in the oligonucleotide dynamics, attributable to different degrees of metallation of the GCârich hairpin stem. Metallated hairpins display fast twoâstate transitions with a twoâfold increase in the opening rate to ~2 sâ1, relative to the unmodified hairpin, and relatively static conformations with longâlived open (and closed) states of 5 s to â„ 50 s. These studies show that a singleâmolecule approach can provides new insight into metallationâinduced changes in DNA structure and dynamics