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DNA Electrochemistry: Charge-Transport Pathways through DNA Films on Gold

Nano, Adela and Furst, Ariel L. and Hill, Michael G. and Barton, Jacqueline K. (2021) DNA Electrochemistry: Charge-Transport Pathways through DNA Films on Gold. Journal of the American Chemical Society, 143 (30). pp. 11631-11640. ISSN 0002-7863. doi:10.1021/jacs.1c04713. https://resolver.caltech.edu/CaltechAUTHORS:20210730-174655133

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Abstract

Over the past 25 years, collective evidence has demonstrated that the DNA base-pair stack serves as a medium for charge transport chemistry in solution and on DNA-modified gold surfaces. Since this charge transport depends sensitively upon the integrity of the DNA base pair stack, perturbations in base stacking, as may occur with DNA base mismatches, lesions, and protein binding, interrupt DNA charge transport (DNA CT). This sensitivity has led to the development of powerful DNA electrochemical sensors. Given the utility of DNA electrochemistry for sensing and in response to recent literature, we describe critical protocols and characterizations necessary for performing DNA-mediated electrochemistry. We demonstrate DNA electrochemistry with a fully AT DNA sequence using a thiolated preformed DNA duplex and distinguish this DNA-mediated chemistry from that of electrochemistry of largely single-stranded DNA adsorbed to the surface. We also demonstrate the dependence of DNA CT on a fully stacked duplex. An increase in the percentage of mismatches within the DNA monolayer leads to a linear decrease in current flow for a DNA-bound intercalator, where the reaction is DNA-mediated; in contrast, for ruthenium hexammine, which binds electrostatically to DNA and the redox chemistry is not DNA-mediated, there is no effect on current flow with mismatches. We find that, with DNA as a well hybridized duplex, upon assembly, a DNA-mediated pathway facilitates the electron transfer between a well coupled redox probe and the gold surface. Overall, this report highlights critical points to be emphasized when utilizing DNA electrochemistry and offers explanations and controls for analyzing confounding results.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/jacs.1c04713DOIArticle
ORCID:
AuthorORCID
Nano, Adela0000-0002-1984-5770
Furst, Ariel L.0000-0001-9583-9703
Barton, Jacqueline K.0000-0001-9883-1600
Additional Information:© 2021 The Authors. Published by American Chemical Society. Received: May 6, 2021. We are grateful to the NIH (GM126904) for their continued support of this research. We are also grateful to our many collaborators over the years who developed this powerful chemistry, despite some skepticism, and creatively designed new sensor technology. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
NIHGM126904
Subject Keywords:Redox reactions, Electrochemistry, Genetics, Electrodes, Monolayers
Issue or Number:30
DOI:10.1021/jacs.1c04713
Record Number:CaltechAUTHORS:20210730-174655133
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20210730-174655133
Official Citation:DNA Electrochemistry: Charge-Transport Pathways through DNA Films on Gold. Adela Nano, Ariel L. Furst, Michael G. Hill, and Jacqueline K. Barton. Journal of the American Chemical Society 2021 143 (30), 11631-11640; DOI: 10.1021/jacs.1c04713
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:110102
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:02 Aug 2021 16:53
Last Modified:24 Aug 2021 18:06

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