Current understanding of electron transfer (ET) kinetics is largely based on ensemble measurements that obscure the underlying single-mol. behavior. We previously reported systematic distance-dependent single mol. 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 mol., or it may reflect the uncertainty of ET kinetics.
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