Molecular Junctions and Nanostructures
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Abstract
Abstract
An approach combining both electrochemical and in-situ fluorescence imaging for characterizing a self-assembled monolayer(SAM) on a gold surface after carbodiimide conjugation with DNA is described. The characteristics of a carbodiimide modified mixed SAM (50:50 mercaptoundecanoic acid/mercaptoundecanol 11-MUA/MUDOL) with an amine modified DNA strand labeled with a redox active fluorophore was studied. The redox active ATTO655 fluorophore enabled comprehensive characterization of the coverage, ET kinetics, uniformity of surface modification and stability towards heating and reductive potentials and the influence of reaction conditions on the extent of surface modification. The surface coverage (ΓDNA) was determined by redox charge and correlated to the change in fluorescence intensity as ATTO655 is non-fluorescent when reduced. Conditions for surface conjugation were evaluated providing a low coverage (ΓDNA ≈ 3 pmol cm−2) uniformly distributed DNA on the SAM. Non-specifically adsorbed DNA on the activated SAM surface was hypothesized to increase the extent of surface modification as ΓDNA was significantly larger when compared to the surface coverage for a ATTO655 modified cadaverine. The non-specifically adsorbed DNA could be removed by soaking in low ionic strength buffer and/or in 55C PBS buffer (> 1hr) without compromising the SAM. Unactivated SAM did not show the presence of non-specifically adsorbed DNA, highlighting the challenge in creating modified SAMs using sNHS and DNA. The reductive desorption stability was dictated by the underlying 11-MUA/MUDOL SAM providing a negative potential window for selecting redox active labels appropriate for use in biosensing. These SAMs were shown to be regenerated after hybridization by soaking in 55C DI with some degradation as visualized using fluorescence imaging. The combined use of electrochemical redox and fluorescence imaging was effective in characterizing and optimizing the carbodiimide surface modification of an acid terminated thiol SAM.
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@article{Zhou2026coupled,
title = {A coupled redox and fluorescence study of carbodiimide conjugation of DNA to 11-mercaptoundecanoic acid SAMs on Au},
author = {Geyang Chris Zhou and Dan Bizzotto},
journal = {ChemRxiv},
year = {2026},
doi = {10.26434/chemrxiv.15007548/v1},
url = {https://doi.org/10.26434/chemrxiv.15007548/v1}
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