Pinhole‐free large‐grained atomically smooth Au(111) substrates prepared by flame‐annealed template stripping

Banner, L. Todd; Richter, A. G.; Pinkhassik, Eugene

doi:10.1002/sia.2977

Cited by 26 publications

(30 citation statements)

References 42 publications

(47 reference statements)

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“…We further probed the applicability of our biophysical parameters for accurate base calling using different pH conditions to reversibly perturb the nucleic acid chemistry of DNA nucleobases . We used STS measurements of ssDNA homo‐oligomers on an atomically flat, clean Au(111) substrate prepared with template stripping, after the surface condition was pH adjusted (see a full methods description in the Experimental Section). At each biochemical condition (neutral, basic, acidic), we performed base calling simulations as previously described with LUMO and HOMO parameters only, all nine parameters, and then optimally tuned sets of parameters.…”

Section: Resultsmentioning

confidence: 99%

Single Nucleobase Identification Using Biophysical Signatures from Nanoelectronic Quantum Tunneling

Korshoj

Afsari

Khan

et al. 2017

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Nanoelectronic DNA sequencing can provide an important alternative to sequencing-by-synthesis by reducing sample preparation time, cost, and complexity as a high-throughput next-generation technique with accurate single-molecule identification. However, sample noise and signature overlap continue to prevent high-resolution and accurate sequencing results. Probing the molecular orbitals of chemically distinct DNA nucleobases offers a path for facile sequence identification, but molecular entropy (from nucleotide conformations) makes such identification difficult when relying only on the energies of lowest-unoccupied and highest-occupied molecular orbitals (LUMO and HOMO). Here, nine biophysical parameters are developed to better characterize molecular orbitals of individual nucleobases, intended for single-molecule DNA sequencing using quantum tunneling of charges. For this analysis, theoretical models for quantum tunneling are combined with transition voltage spectroscopy to obtain measurable parameters unique to the molecule within an electronic junction. Scanning tunneling spectroscopy is then used to measure these nine biophysical parameters for DNA nucleotides, and a modified machine learning algorithm identified nucleobases. The new parameters significantly improve base calling over merely using LUMO and HOMO frontier orbital energies. Furthermore, high accuracies for identifying DNA nucleobases were observed at different pH conditions. These results have significant implications for developing a robust and accurate high-throughput nanoelectronic DNA sequencing technique.

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Section: Resultsmentioning

confidence: 99%

Single Nucleobase Identification Using Biophysical Signatures from Nanoelectronic Quantum Tunneling

Korshoj

Afsari

Khan

et al. 2017

Small

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“…Deposited molecular films were characterized by atomic force microscopy (AFM), which suggested the formation of high-uniformity SAMs. All molecular films were grown on freshly prepared template stripped Au substrates 37,38 with a surface roughness of 80-150 pm (see Methods section). Averaged roughness, as measured across multiple random areas (ESI- Table S2), showed that SAMs of 1-4 conformally follow the underlying gold surface with comparable roughness.…”

Section: Sam Formation and Characterisationmentioning

confidence: 99%

Scale-Up of Room-Temperature Constructive Quantum Interference from Single Molecules to Self-Assembled Molecular-Electronic Films

et al. 2020

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The realization of self-assembled molecular-electronic films, whose room-temperature transport properties are controlled by quantum interference (QI), is an essential step in the scale-up QI effects from single molecules to parallel arrays of molecules. Recently, the effect of destructive QI (DQI) on the electrical conductance of self-assembled monolayers (SAMs) has been investigated. Here, through a combined experimental and theoretical investigation, we demonstrate chemical control of different forms of constructive QI (CQI) in cross-plane transport through SAMs and assess its influence on cross-plane thermoelectricity in SAMs. It is known that the electrical conductance of single molecules can be controlled in a deterministic manner, by chemically varying their connectivity to external electrodes. Here, by employing synthetic methodologies to vary the connectivity of terminal anchor groups around aromatic anthracene cores, and by forming SAMs of the resulting molecules, we clearly demonstrate that this signature of CQI can be translated into SAM-on-gold molecular films. We show that the conductance of vertical molecular junctions formed from anthracene-based molecules with two different connectivities differ by a factor of approximately 16, in agreement with theoretical predictions for their conductance ratio based on constructive QI effects within the core. We also demonstrate that for molecules with thiol anchor groups, AUTHOR INFORMATION

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“…Therefore, the structure and properties of SAMs significantly depend on the substrate. [53] Template stripping can generate surfaces with roughness <1 nm [25], in which technique a glass slide or other solid support is glued to the exposed surface of a metal film deposited on silicon wafer, and then the metal film is peeled from the wafer to expose the surface that had been in direct contact with the wafer. Chen et al (2015) reported a new method, referred to as "remote mechanical annealing (ReMA)" to fabricate ultra-flat Au surface with RMS roughness as low as 0.2 nm [26].…”

Section: Substrates Roughnessmentioning

confidence: 99%

The Porter-Whitesides Discrepancy: Revisiting Odd-Even Effects in Wetting Properties of n-Alkanethiolate SAMs

2015

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This review discusses the Porter-Whitesides discrepancy in wetting properties of n-alkanethiolate self-assembled monolayers (SAMs). About 25 years ago, Whitesides and coworker failed to observe any odd-even effect in wetting, however, Porter and his coworker did, albeit in select cases. Most previous studies agreed with Whitesides' results, suggesting the absence of the odd-even effect in hydrophobicity of n-alkanethiolate SAMs. Recent reports have, however, found the odd-even effect in hydrophobicity of n-alkanethiolate SAMs on smooth substrates, indicating that hydrophobicity, and analogous interfacial properties, of n-alkanethiolate SAMs significantly depends on the properties of substrate. Unfortunately, the Whitesides and Porter papers do not report on the quality of the surfaces used. Based on recent work, we inferred that the original discrepancy between Whitesides and Porter can be attributed to the quality of the surface. Odd-even effect of SAMs in charge transport, capacitance, friction, and SAM structure are also discussed in this review to inform the general discussion. The discrepancy between Porter's group and Whitesides' group could be due to surface roughness, morphology, oxidation, and adventitious contaminants. OPEN ACCESSCoatings 2015, 5 1035

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Pinhole‐free large‐grained atomically smooth Au(111) substrates prepared by flame‐annealed template stripping

Cited by 26 publications

References 42 publications

Single Nucleobase Identification Using Biophysical Signatures from Nanoelectronic Quantum Tunneling

Single Nucleobase Identification Using Biophysical Signatures from Nanoelectronic Quantum Tunneling

Scale-Up of Room-Temperature Constructive Quantum Interference from Single Molecules to Self-Assembled Molecular-Electronic Films

The Porter-Whitesides Discrepancy: Revisiting Odd-Even Effects in Wetting Properties of n-Alkanethiolate SAMs

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