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Photochemistry

Electronic motion in DNA

Nature volume 397, pages 480–481 (1999)Cite this article

The fundamental mechanism of molecular electron transfer requires an electronic mixing pathway between the initial and final states. In most intramolecular and intermolecular electron-transfer reactions, the charge is localized only at the first and last sites: the charge is thought to move between these two points in a single, coherent jump — much like a kicked football2. But when the states between the initial and final ones are sufficiently low in energy the charge can stop along the way, so that its overall trajectory looks more like the path of a wandering drunk. The coherent transfer process cannot get very far at room temperature, because the orbitals in which the electron density is found do not extend effectively over long distances and thermal disorder further localizes the charge. The latter, diffusive motion is responsible for the ordinary conductivity of real metals3,4,5 (as described by Ohm'slaw).

So, depending on the energy, one expects different mechanistic behaviour: if the ‘bridging states’ (in DNA, these are the intervening base pairs) are very high in energy compared with the initial and final states, we should see coherent transport. This is generally called superexchange, and is characterized by a rapid exponential decay of the transfer rate or yield as a function of distance2. But if the intermediate bridging states are comparable in energy, or lower in energy, than the initial state, then one expects to see incoherent, hopping behaviour that decays only slowly with distance.

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Figure 1: Conduction in double-stranded DNA measured by Meggers et al.1.

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  1. the Chemistry Department, Northwestern University, Evanston, 60208, Illinois, USA

    Mark Ratner

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Ratner, M. Electronic motion in DNA. Nature 397, 480–481 (1999). https://doi.org/10.1038/17232

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