Molecular rectifier composed of DNA with high rectification ratio enabled by intercalation

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Abstract

The predictability, diversity and programmability of DNA make it a leading candidate for the design of functional electronic devices that use single molecules, yet its electron transport properties have not been fully elucidated. This is primarily because of a poor understanding of how the structure of DNA determines its electron transport. Here, we demonstrate a DNA-based molecular rectifier constructed by site-specific intercalation of small molecules (coralyne) into a custom-designed 11-base-pair DNA duplex. Measured current-voltage curves of the DNA-coralyne molecular junction show unexpectedly large rectification with a rectification ratio of about 15 at 1.1 V, a counter-intuitive finding considering the seemingly symmetrical molecular structure of the junction. A non-equilibrium Green's function-based model - parameterized by density functional theory calculations - revealed that the coralyne-induced spatial asymmetry in the electron state distribution caused the observed rectification. This inherent asymmetry leads to changes in the coupling of the molecular HOMO-1 level to the electrodes when an external voltage is applied, resulting in an asymmetric change in transmission.

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Guo, C., Wang, K., Zerah-Harush, E., Hamill, J., Wang, B., Dubi, Y., & Xu, B. (2016). Molecular rectifier composed of DNA with high rectification ratio enabled by intercalation. Nature Chemistry, 8(5), 484–490. https://doi.org/10.1038/nchem.2480

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