Electrochemical response of surface-attached redox DNA governed by low activation energy electron transfer kinetics

Zheng, Zhiyong; Kim, Soo Hyeon; Chovin, Arnaud; Nicolas, Clément; Demaille, Christophe

doi:10.1039/d3sc00320e

Cited by 9 publications

(31 citation statements)

References 56 publications

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“…The top and the bottom electrodes were biased at potentials respectively positive and negative enough vs Fc/Fc + , the standard potential of the Fc head, for the current not to depend on their exact values. In this situation, the Marcus rate saturation regime is reached, so that k V is the same at both electrodes (Figure S13). The z gap value was precisely calibrated from force–distance curves (see Figure S11).…”

Section: Resultsmentioning

confidence: 99%

“…It can be compared with an independent measurement (Figure S12). The second assumption is that, to account for low reorganization energy observed for Fc-DNA attached on an electrode (eq 14), 32 we assume a small dielectric constant of 1.8 for water at the interface, which is anyway the value found experimentally for water in nanogaps. 34,35 This is useful for discussing the value of k V (Figure S13).…”

Section: Methodsmentioning

confidence: 99%

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Ballistic Brownian Motion of Nanoconfined DNA

Madrid,

Zheng,

Gerbelot

et al. 2023

ACS Nano

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Theoretical treatments of polymer dynamics in liquid generally start with the basic assumption that motion at the smallest scale is heavily overdamped; therefore, inertia can be neglected. We report on the Brownian motion of tethered DNA under nanoconfinement, which was analyzed by molecular dynamics simulation and nanoelectrochemistry-based singleelectron shuttle experiments. Our results show a transition into the ballistic Brownian motion regime for short DNA in sub-5 nm gaps, with quality coefficients as high as 2 for double-stranded DNA, an effect mainly attributed to a drastic increase in stiffness. The possibility for DNA to enter the underdamped regime could have profound implications on our understanding of the energetics of biomolecular engines such as the replication machinery, which operates in nanocavities that are a few nanometers wide.

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Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Ballistic Brownian Motion of Nanoconfined DNA

Madrid,

Zheng,

Gerbelot

et al. 2023

ACS Nano

Self Cite

View full text Add to dashboard Cite

show abstract

“…The top and the bottom electrodes were biased at potentials respectively positive and negative enough vs. Fc/Fc + , the standard potential of the Fc head, for the current not to depend on their exact values. In this situation, the Marcus rate saturation regime is reached 28 , so that kV is the same at both electrodes (Supplementary Fig. 13).…”

Section: Single-electron Shuttle Experimentsmentioning

confidence: 98%

“…12). The second assumption is that, to account for low reorganization energy observed for Fc-DNA attached on an electrode (Equation ( 14)) 28 , we assume a small dielectric constant of 1.8 for water at the interface, which is anyway the value found experimentally for water in nanogaps 51,52 . This is useful for discussing the value of kV (Supplementary Fig.…”

Section: Q-biol Code (The "Digital Experiment" Counting Electrons)mentioning

confidence: 99%

Ballistic Brownian motion of nanoconfined DNA

Madrid

Zheng

Gerbelot

et al. 2023

Preprint

View full text Add to dashboard Cite

Theoretical treatments of polymer dynamics in liquid generally start with the basic assumption that motion at the smallest scale is heavily overdamped; therefore, inertia can be neglected. We report on the Brownian motion of tethered DNA under nanoconfinement, which was analyzed by molecular dynamics simulation and nanoelectrochemistry-based single-electron shuttle experiments. Our results show a transition into the ballistic Brownian motion regime for short DNA in sub-5-nm gaps, with quality coefficients as high as 2 for dsDNA, an effect mainly attributed to a drastic increase in stiffness. The possibility for DNA to enter the underdamped regime could have profound implications on our understanding of the energetics of biomolecular engines such as the replication machinery, which operates in nanocavities of a few nanometers wide.

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“…Compared to other methods, EC sensors have the merits of easy operation, high sensitivity, and portability. [10][11][12][13][14][15][16][17][18][19] For example, a recent technique using rolling circle amplification with aptamers could successfully demonstrate a limit of detection (LOD) as low as 5 CTC cells in whole blood (with 200 μL of the sample used for incubation). 20 Another approach using quantum dots as sensing probe attained a LOD of 2 cells/mL in human serum.…”

mentioning

confidence: 99%

Single-cell Electrochemical Aptasensor Array

Coffinier

Lagadec

et al. 2023

Preprint

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Despite several demonstrations of electrochemical devices with limits of detection (LOD) of 1 cell/mL, the implementation of single-cell bioelectrochemical sensor arrays has remained elusive due to their challenging implementation at large scale. Here, we show that the recently introduced nanopillar array technology combined with redox-labelled aptamers targeting epithelial cell adhesion molecule (EpCAM) is perfectly suited for such implementation. Combining nanopillar arrays with microwells determined for single cell trapping directly on the sensor surface, single target cells are successfully detected and analyzed. This first implementation of a single-cell electrochemical aptasensor array based on Brownian-fluctuating redox species opens new opportunities for large-scale implementation and statistical analysis of early cancer diagnosis and cancer therapy in clinical settings.

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Electrochemical response of surface-attached redox DNA governed by low activation energy electron transfer kinetics

Abstract: The mechanism responsible for electron transport within layers of redox DNA anchored to electrodes has been extensively studied over the last twenty years, but remains controversial. Herein, we thoroughly study...

Cited by 9 publications

References 56 publications

Ballistic Brownian Motion of Nanoconfined DNA

Ballistic Brownian Motion of Nanoconfined DNA

Ballistic Brownian motion of nanoconfined DNA

Single-cell Electrochemical Aptasensor Array

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