We investigate the diffusion and the drift motion of λ DNA molecules near solid-state nanopores prior to their translocation though the nanopores using fluorescence microscopy. The radial dependence of the electric field near a nanopore generated by an applied voltage in ionic solution can be estimated quantitatively in 3D by analyzing the motion of negatively charged DNA molecules. We find that the electric field is approximately spherically symmetric around the nanopore under the conditions investigated. In addition, DNA clogging at the nanopore was directly observed. Surprisingly, the probability of the clogging event increases with increasing external bias voltage. We also find that DNA molecules clogging the nanopore reduce the electric field amplitude at the nanopore membrane surface. To better understand these experimental results, analytical method with Ohm’s law and computer simulation with Poisson and Nernst-Planck (PNP) equations are used to calculate the electric field near the nanopore. These results are of great interest in both experimental and theoretical considerations of the motion of DNA molecules near voltage-biased nanopores. These findings will also contribute to the development of solid-state nanopore based DNA sensing devices.

An apparatus that integrates solid-state nanopore ionic current measurement with a Scanning Probe Microscope has been developed. When a micrometer-scale scanning probe tip is near a voltage biased nanometer-scale pore (10–100 nm), the tip partially blocks the flow of ions to the pore and increases the pore access resistance. The apparatus records the current blockage caused by the probe tip and the location of the tip simultaneously. By measuring the current blockage map near a nanopore as a function of the tip position in 3D space in salt solution, we estimate the relative pore resistance increase due to the tip, ΔR/R0, as a function of the tip location, nanopore geometry, and salt concentration. The amplitude of ΔR/R0 also depends on the ratio of the pore length to its radius as Ohm’s law predicts. When the tip is very close to the pore surface, ~10 nm, our experiments show that ΔR/R0 depends on salt concentration as predicted by the Poisson and Nernst-Planck equations. Furthermore, our measurements show that ΔR/R0 goes to zero when the tip is about five times the pore diameter away from the center of the pore entrance. The results in this work not only demonstrate a way to probe the access resistance of nanopores experimentally, they also provide a way to locate the nanopore in salt solution, and open the door to future nanopore experiments for detecting single biomolecules attached to a probe tip.

In pursuit of developing solid-state nanopore based DNA sequencing technology, we have designed and constructed an apparatus that can place a DNA tethered probe tip near a solid-state nanopore, control the DNA moving speed, and measure the ionic current change when a DNA is captured and released from a nanopore. The probe tip’s position is sensed and controlled by a tuning fork based feedback force sensor and a nanopositioning system. Using this newly constructed apparatus, a DNA strand moving rate of >100μs/base or <1nm/ms in silicon nitride nanopores has been accomplished. This rate is 10 times slower than by manipulating DNA tethered beads using optical tweezers and 1000 times slower than free DNA translocation through solid-state nanopores reported previously, which provides enough temporal resolution to read each base on a tethered DNA molecule using available single channel recording electronics on the market today. This apparatus can measure 3 signals simultaneously: ionic current through a nanopore, tip position, and tip vibrational amplitude during the process of a DNA’s capture and release by a nanopore. We show results of this apparatus for measuring λ DNA’s capture and release distances, and for current blockage signals of λ DNA molecules biotinylated with one end and with both ends tethered to a tip.

Since the isolation of graphene, various two-dimensional (2D) materials have been extensively investigated. Nevertheless, only few 2D oxides have been reported to date due to difficulties in their synthesis. However, it is expected that the layered transition-metal oxides (TMOs) could be missing blocks for van der Waals heterostructures and essential elements for 2D electronics. Herein, the crystal structure and band structure of van der Waals epitaxially grown α-MoO3 nanosheets on various 2D growth templates are characterized. Monolayer and multilayer α-MoO3 nanosheets are successfully grown on a 2D substrate by simply evaporating amorphous molybdenum oxide thin film in ambient conditions. A single-crystal α-MoO3 nanosheet without grain boundary is epitaxially grown on various 2D substrates despite a large lattice mismatch. During growth, the quasi-stable monolayer α-MoO3 first covers the 2D substrate, then additional layers are continuously grown on the first monolayer α-MoO3. The band gap of the α-MoO3 increases from 2.9 to 3.2 eV as the thickness decreases. Furthermore, due to oxygen vacancies and surface adsorbates, the synthesized α-MoO3 is highly n-doped with a small work function. Therefore, α-MoO3 field-effect transistors (FETs) exhibit a typical n-type conductance. This work shows the great potential of ultra-thin α-MoO3 in 2D-material-based electronics.

van der Waals (vdW) materials have shown unique electrical and optical properties depending on the thickness due to strong interlayer interaction and symmetry breaking at the monolayer level. In contrast, the study of electrical and tribological properties and their thickness-insensitivity of van der Waals oxides are lacking due to difficulties in the fabrication of high quality two-dimensional oxides and the investigation of nanoscale properties. Here we investigated various tribological and electrical properties, such as, friction, adhesion, work function, tunnel current, and dielectric constant, of the single-crystal α-MoO3 nanosheets epitaxially grown on graphite by using atomic force microscopy. The friction of atomically smooth MoO3 is rapidly saturated within a few layers. The thickness insensitivity of friction is due to very weak mechanical interlayer interaction. Similarly, work function (4.73 eV for 2 layers (hereafter denoted as L)) and dielectric constant (6 for 2L and 10.5–11 for >3L) of MoO3 in MoO3 showed thickness insensitivity due to weak interlayer coupling. Tunnel current measurements by conductive atomic force microscopy showed that even 2L MoO3 of 1.4 nm is resistant to tunneling with a high dielectric strength of 14 MV/cm. The thickness-indifferent electrical properties of high dielectric constant and tunnel resistance by weak interlayer coupling and high crystallinity show a promise in the use of MoO3 nanosheets for nanodevice applications.