Chemically Functionalizing Controlled Dielectric Breakdown Silicon Nitride Nanopores by Direct Photohydrosilylation
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Nanopores are a prominent enabling tool for single-molecule applications such as DNA sequencing, protein profiling, and glycomics, and the construction of ionic circuit elements. Silicon nitride (SiNx) is a leading scaffold for these <100 nm-diameter nanofluidic ion-conducting channels, but frequently challenging surface chemistry remains an obstacle to their use. We functionalized more than 100 SiNx nanopores with different surface terminations-acidic (Si-R-OH, Si-R-CO2H), basic (Si-R-NH2), and nonionizable (Si-R-C6H3(CF3)2)-to chemically tune the nanopore size, surface charge polarity, and subsequent chemical reactivity and to change their conductance by changes of solution pH. The initial one-reaction-step covalent chemical film formation was by hydrosilylation and could be followed by straightforward condensation and click reactions. The hydrosilylation reaction step used neat reagents with no special precautions such as guarding against water content. A key feature of the approach was to combine controlled dielectric breakdown (CDB) with hydrosilylation to create and functionalize SiNx nanopores. CDB thus replaced the detrimental but conventionally necessary surface pretreatment with hydrofluoric acid. Proof-of-principle detection of the canonical test molecule, λ-DNA, yielded signals that showed that the functionalized pores were not obstructed by chemical treatments but could translocate the biopolymer. The characteristics were tuned by the surface coating character. This robust and flexible surface coating method, freed by CDB from HF etching, portends the development of nanopores with surface chemistry tuned to match the application, extending even to the creation of biomimetic nanopores.Keywords:
Nanopore
Porous Silicon
Dielectric loss
Volume fraction
High-κ dielectric
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Nanopore
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Abstract Silicon nitride has been prepared by heating pure silicon in purified nitrogen at 1450°. X ‐ray studies showed the presence of two nitrides, and a method was therefore devised to separate them. Although these nitrides differ in their crystal structure, they have the same compositions, corresponding to Si3N4. A few chemical tests were performed on finely divided silicon nitride prepared at or above 145°. Several alloys containing various proportions of silicon were nitrided under different conditions, and the X ‐ray diffraction patterns of the nitrides extracted from these alloys were found to be in complete agreement with that of α‐Si 3 N 4 . The diffraction lines obtained from the nitrided alloy prior to any chemical treatment gave nitride lines which did not correspond to those of the α‐Si 3 N 4 or β‐Si 3 N 4 .
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Selective detection of attomolar proteins was achieved using gold lined nanopores in a nanopore blockade sensor.
Nanopore
Protein detection
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To slow the translocation of single-stranded DNA (ssDNA) through a solid-state nanopore, a nanopore was narrowed, and the effect of the narrowing on the DNA translocation speed was investigated. In order to accurately measure the speed, long (5.3 kb) ssDNA (namely, ss-poly(dA)) with uniform length (±0.4 kb) was synthesized. The diameters of nanopores fabricated by a transmission electron microscope were controlled by atomic-layer deposition. Reducing the nanopore diameter from 4.5 to 2.3 nm slowed down the translocation of ssDNA by more than 16 times (to 0.18 μs base(-1)) when 300 mV was applied across the nanopore. It is speculated that the interaction between the nanopore and the ssDNA dominates the translocation speed. Unexpectedly, the translocation speed of ssDNA through the 4.5 nm nanopore is more than two orders of magnitude higher than that of double-stranded DNA (dsDNA) through a nanopore of almost the same size. The cause of such a faster translocation of ssDNA can be explained by the weaker drag force inside the nanopore. Moreover, the measured translocation speeds of ssDNA and dsDNA agree well with those calculated by molecular-dynamics (MD) simulation. The MD simulation predicted that reducing the nanopore diameter to almost the same as that of ssDNA (i.e. 1.4 nm) decreases the translocation speed (to 1.4 μs base(-1)). Narrowing the nanopore is thus an effective approach for accomplishing nanopore DNA sequencing.
Nanopore
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Abstract ChemInform is a weekly Abstracting Service, delivering concise information at a glance that was extracted from about 100 leading journals. To access a ChemInform Abstract of an article which was published elsewhere, please select a “Full Text” option. The original article is trackable via the “References” option.
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Using nanopores for single-molecule sequencing of proteins - similar to nanopore-based sequencing of DNA - faces multiple challenges, including unfolding of the complex tertiary structure of the proteins and enforcing their unidirectional translocation through nanopores. Here, we combine molecular dynamics (MD) simulations with single-molecule experiments to investigate the utility of SDS (Sodium Dodecyl Sulfate) to unfold proteins for solid-state nanopore translocation, while simultaneously endowing them with a stronger electrical charge. Our simulations and experiments prove that SDS-treated proteins show a considerable loss of the protein structure during the nanopore translocation. Moreover, SDS-treated proteins translocate through the nanopore in the direction prescribed by the electrophoretic force due to the negative charge impaired by SDS. In summary, our results suggest that SDS causes protein unfolding while facilitating protein translocation in the direction of the electrophoretic force; both characteristics being advantageous for future protein sequencing applications using solid-state nanopores.
Nanopore
Transport protein
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Nanopores offer the potential for label-free analysis of individual proteins and low cost DNA sequencing. In order to design and evaluate nanopore devices, an understanding of nanopore electrokinetic transport is crucial. However, most studies of nanopore electrokinetic transport have neglected the effects of concentration polarization (CP) in the bulk fluid surrounding the pore. In this paper, we present a computational model which demonstrates the effects of CP on the background electrolyte in nanopore devices with tip diameters of 40–100 nm. We also present direct experimental observation of the distribution of an anionic dye in the vicinity of a conical nanopore. These results indicate that CP in a nanopore system can affect concentration distributions in the bulk solution tens of microns away from the pore, suggesting that typical boundary conditions used to model nanopore electrokinetic transport are incomplete.
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Nanofluidics
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ESCA is used to characterize silicon nitride surface oxidation. Si 2p, N 1s, and O 1s binding energies and photoelectron line intensities of oxidized nitride films are compared with the corresponding lines from thick reference films of silicon, silicon nitride, silcon dioxide, and a series of oxynitrides. Rapid initial oxidation of silicon nitride surfaces occurs at room temperature on exposure of nitride films to air. A graded oxidized nitride film forms between the film surface and the nitride. Similarly, oxynitride films with gradations in composition are obtained upon oxidation of nitride films at high temperatures.
Silicon oxynitride
Silicon dioxide
LOCOS
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