Sequence-independent and rapid long-range charge transfer through DNA

Interest in using DNA as a building block for nanoelectronic sensors and devices stems from its efficient hole-conducting properties and the relative ease with which it can be organized into predictable nanometre-sized two- and three-dimensional structures. However, because a hole migrates along DNA through the highest occupied molecular orbital of the guanine bases, its conductivity decreases as the adenine-thymine base-pair content increases. This means that there are limitations on what sequences can be used to construct functional nanoelectronic circuits, particularly those rich in adenine-thymine pairs. Here we show that the charge-transfer efficiency can be dramatically increased in a manner independent of guanine-cytosine content by adjusting the highest occupied molecular orbital level of the adenine-thymine base pair to be closer to that of the guanine-cytosine pair. This is achieved by substituting the N7 nitrogen atom of adenine with a C-H group to give 7-deazaadenine, which does not disturb the complementary base pairing observed in DNA.