Potential‐Assisted DNA Immobilization as a Prerequisite for Fast and Controlled Formation of DNA Monolayers

Jambrec, Daliborka; Gębala, Magdalena; Mantia, Fabio La; Schuhmann, Wolfgang

doi:10.1002/anie.201506672

Cited by 57 publications

(78 citation statements)

References 30 publications

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“…Potential pulse‐assisted method for immobilization of thiolated DNA consist of sequential several ms long pulse‐type change of the applied potentials that must be more positive and more negative of the potential of zero charge during modification . When a positive potential pulse is applied, charging of the electrochemical double layer leads to an excess of negative charges in the vicinity of the electrified interface.…”

Section: Resultsmentioning

confidence: 99%

“…The thiol self‐assembly process is known to exhibit low reproducibility with sluggish kinetics, requiring hours to days for achieving best possible reproducible coverages, making it less attractive for microarray modification. Our group recently developed potential pulse‐assisted methods for fast and reproducible gold surface modification with charged and uncharged thiolated species, i. e., among others ssDNA strands and alkylthiols . Here, we combine features of this methodology together with potential pulse‐assisted surface cleaning to investigate the possibility of selectively electrochemically modifying microarrays with multiple probe capture DNA strands, while concomitantly controlling the DNA coverage in a reproducible way.…”

Section: Introductionmentioning

confidence: 99%

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Controlling DNA/Surface Interactions for Potential Pulse‐Assisted Preparation of Multi‐Probe DNA Microarrays

2019

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The possibility of selectively modifying microarray electrodes with different DNA sequences in a controlled way without the need for local positioning of solutions or local modification of array surfaces is demonstrated. Potential pulse sequences are employed to perform sequential surface modification of a 32‐gold‐electrode array with two different thiolated DNA capture sequences, surface passivation and regeneration of selected microarray electrodes, all by adjusting the potential intensities of the same potential pulse‐assisted method. We achieve reproducible and controlled DNA immobilization together with minimization of false signals originating from unspecific adsorption or undesired co‐immobilization. This methodology is not limited to DNA chips and it is potentially suitable for a wide range of applications employing Au−S chemistry. It can be employed in laboratory conditions for localizing different reactive chemistries onto predefined electrodes of an array without the need for complex and expensive apparatus and special conditions.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Controlling DNA/Surface Interactions for Potential Pulse‐Assisted Preparation of Multi‐Probe DNA Microarrays

2019

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“…Recently, we presented a highly reproducible and fast potential‐assisted DNA immobilization method on gold surfaces obtained by applying a pulse‐type potential modulation . Very fast immobilization kinetics were achieved by ion stirring in the vicinity of the electrode, invoked by potential pulsing that statistically facilitates the approach of DNA strands to the surface and the formation of the Au−S bond, contrary to the commonly believed electrostatic attraction/repulsion of the supposedly negatively charged DNA strand.…”

Section: Resultsmentioning

confidence: 99%

“…A new approach for the fast formation of highly compact thiol SAMs is presented. The process is based on our previously developed method for potential‐assisted ssDNA immobilization . SAM formation is supported by potential pulses comprising applied potentials that are more positive and negative as compared to the potential of zero charge (pzc), leading to ion stirring in the vicinity of the electrode that facilitates the approach of thiol molecules to the surface and formation of the gold−sulfur bond.…”

Section: Introductionmentioning

confidence: 99%

Potential‐Pulse‐Assisted Formation of Thiol Monolayers within Minutes for Fast and Controlled Electrode Surface Modification

et al. 2016

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We propose a potential‐pulse‐assisted method for the formation of highly compact thiol self‐assembled monolayers (SAMs), ensuring fully covered surfaces within minutes. By pulsing between potentials that are more positive and more negative with respect to the potential of zero charge, kinetics of SAM formation is substantially enhanced. The formation of the SAM is followed by using real‐time impedance measurements by superimposing the applied potential‐pulse profile with a high‐frequency AC signal that allows for calculation of the interfacial capacitance and provides information about the compactness of the formed layers. A systematic study of the influence of the pulse potential intensity, the pulse duration, and the nature of the thiol derivative on the potential‐pulse‐assisted SAM formation is performed. We show that compact thiol monolayers are obtained much faster with the suggested technique, as compared to SAM formation performed at the open‐circuit potential or by applying a constant potential.

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“…Au surfaces were then thoroughly rinsed with Milli‐Q water and dried under an Ar stream. The probe DNA was immobilized by using the potential‐assisted immobilization method, explained elsewhere, by switching between 10 ms long pulse potentials of 1.1 and 0.4 V versus Pb/PbF 2 for 5 min in the probe DNA solution (1 μ m probe DNA in 10 m m phosphate buffer and 450 m m K 2 SO 4 , pH 7.4). The electrode was then rinsed with phosphate buffer to remove any loosely bound DNA strands.…”

Section: Figurementioning

confidence: 99%

Differentiation between Single‐ and Double‐Stranded DNA through Local Capacitance Measurements

et al. 2016

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ArturoE strada-Vargas, Daliborka Jambrec, Yasin Ugur Kayran,V olodymyr Kuznetsov,a nd WolfgangS chuhmann* [a] Local differentiation of single-stranded (ss) and double-stranded (ds) DNA in microarrays by using electrochemical techniques has gained increasing interest. We proposeamethod for distinguishing areas on gold electrodes modified with ssDNA and dsDNA based on the differencei nt heir local capacitance. The local capacitance is visualized by means of scanning electrochemical impedancem icroscopy and alternatingcurrent scanning electrochemical microscopy.There is ag rowing interest in the label-free detection of DNA hybridization in localized areas of DNA microarrays by using electrochemical readout strategies, owing to their general high sensitivity,l ow cost, and ease of implementation,a sc ompared to commonly used DNA detection strategies.[1] Most of these techniques are based on the detection of the DNA hybridization event,o wing to the high efficiency and specificityi nt he presence of non-complementary nucleic acids. The operation principle of electrochemical detection strategies is based on the modulation of either redox processes or changes in the capacitance at the interface between the immobilized DNA probe and the electrolyte upon DNA hybridization. [2,3] Alternatively,s canning electrochemical microscopy (SECM) has been successfully applied to locally visualize DNA hybridization on measurement sites of aD NA microarray. [4][5][6][7][8][9] However,u ntil now,o nly faradaic processes involving the addition of free-diffusing redoxs pecies have been employed for locally characterizing DNA spots through SECM.The recent development of local impedance techniques, such as localized electrochemical impedance spectroscopy (LEIS), [10,11] alternating currentS ECM (AC-SECM), [12,13] and scanning electrochemical impedancem icroscopy (SEIM), [14][15][16] allows for studying electrochemical processes locally in the absence of any free-diffusing redox mediator. Here, we report the differentiationo fs elf-assembled single-(ss-) and double-stranded (ds-) DNA self-assembled monolayers (SAMs) according to the difference in the local capacitance, as visualized by means of SEIM.Briefly, SEIM involves recording impedance spectra at different spots of as ample using ap ositioned microdisk electrode in low-ionic-strength electrolyte solution. These impedance spectraa re fitted to as uitably chosen electrical equivalent circuit (EEC), as presented in Figure 1A.Here, Q T represents aconstant phase element( CPE) for the interfacial process at the tip.R TC and R TS represent the solutionr esistances for the direct current path through the solution and the indirect current path through the sample, respectively. C S represents the local capacitance of the interfacial process at the sample. As the stray capacitance of the potentiostati sc ontributing to the impedance spectra at high frequencies, its contribution has to be fitted in parallel with the circuit. Figure 1B shows aS EIM line scan over three different zones of aD NA...

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Potential‐Assisted DNA Immobilization as a Prerequisite for Fast and Controlled Formation of DNA Monolayers

Cited by 57 publications

References 30 publications

Controlling DNA/Surface Interactions for Potential Pulse‐Assisted Preparation of Multi‐Probe DNA Microarrays

Controlling DNA/Surface Interactions for Potential Pulse‐Assisted Preparation of Multi‐Probe DNA Microarrays

Potential‐Pulse‐Assisted Formation of Thiol Monolayers within Minutes for Fast and Controlled Electrode Surface Modification

Differentiation between Single‐ and Double‐Stranded DNA through Local Capacitance Measurements

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