Large Heterogeneity Observed in Single Molecule Measurements of Intramolecular Electron Transfer Rates through DNA

Abstract

Abstract Current understanding of electron transfer (ET) kinetics is largely based on ensemble measurements that obscure the underlying single-molecule behavior. We previously reported systematic distance-dependent single molecule ET measurements that show a large heterogeneity. Here we study and discuss this heterogeneity in more detail and suggest that it is a rather fundamental phenomenon that is difficult to explain solely by the distribution of DNA conformations. This heterogeneity may arise from the uniqueness of each molecule, or it may reflect the uncertainty of ET kinetics.