Abstract
In the framework of a multistep mechanism in which environmental motion triggers comparatively faster elementary electron-transfer steps and stabilizes hole-transfer products, microscopic coherence is crucial for rationalizing the observed yield ratios of oxidative damage to DNA. Interference among probability amplitudes of indistinguishable electron-transfer paths is able to drastically change the final outcome of charge transport, even in DNA oligomers constituted by similar building blocks, and allows for reconciling apparently discordant experimental observations. Properly tailored DNA oligomers appear to be a promising workbench for studying tunneling in the presence of dissipation at the macroscopic level.
Highlights
In the framework of a multistep mechanism in which environmental motion triggers comparatively faster elementary electron-transfer steps and stabilizes hole-transfer products, microscopic coherence is crucial for rationalizing the observed yield ratios of oxidative damage to DNA
Several pieces of experimental evidence have suggested that charge transport in DNA is characterized by two distinct regimes:[3,16] a short-range regime, in which hole-transfer (HT) rates exponentially decay with the donor−acceptor (DA) distance, and a long-range regime, where HT rates display a much weaker distance dependence
We propose a unifying mechanism of hole transport in DNA, for both short- and long-range regimes, which accounts almost quantitatively for the observed distributions of oxidative damage at DNA nucleobases in different sets of oligomers, and allows for reconciling apparently discordant experimental observations, obtained for two separated sets of DNA oligomers, which, sharing similar structural motifs, exhibit drastically different charge transport properties.[3,4]
Summary
In the framework of a multistep mechanism in which environmental motion triggers comparatively faster elementary electron-transfer steps and stabilizes hole-transfer products, microscopic coherence is crucial for rationalizing the observed yield ratios of oxidative damage to DNA.
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