Tuning the Sensitivity of MoS Nanopores: From Labeling to Labeling-Free Detection of DNA Methylation.

DNA methylation discrimination is often challenged by complicated pretreatment, insufficient sensitivity, and suboptimal accuracy. Here, single-molecule readout of DNA methylation is reported using single-layer MoS nanopores. By tuning pore dimension, the sensitivity of MoS nanopores is manipulated, empowering both labeling and labeling-free strategies for DNA methylation discrimination.

Water compression induced ionic negative differential resistance in nanopores.

The mass transport behavior through nanoscale channels, greatly influenced by the structures and dynamics of nanoconfined water, plays an essential role in many biophysical processes. However, the dynamics of nanoconfined water under an external field and its effects are still not fully understood. Here, on the basis of molecular dynamics simulations, we theoretically show that the ionic current of [Bmim][PF6] through narrow pores in graphene membrane exhibits an ionic negative differential resistance effect-the ionic current decreases as the voltage increases over a certain threshold.

Direct probing of single-molecule chemiluminescent reaction dynamics under catalytic conditions in solution.

Chemical reaction kinetics can be evaluated by probing dynamic changes of chemical substrates or physical phenomena accompanied during the reaction process. Chemiluminescence, a light emitting exoenergetic process, involves random reaction positions and kinetics in solution that are typically characterized by ensemble measurements with nonnegligible average effects. Chemiluminescent reaction dynamics at the single-molecule level remains elusive.

MoS nanopore identifies single amino acids with sub-1 Dalton resolution.

The sequencing of single protein molecules using nanopores is faced with a huge challenge due to the lack of resolution needed to resolve single amino acids. Here we report the direct experimental identification of single amino acids in nanopores. With atomically engineered regions of sensitivity comparable to the size of single amino acids, MoS nanopores provide a sub-1 Dalton resolution for discriminating the chemical group difference of single amino acids, including recognizing the amino acid isomers.

Inducing Electric Current in Graphene Using Ionic Flow.

Classical nanofluidic frameworks account for the confined fluid and ion transport under an electrostatic field at the solid-liquid interface, but the electronic property of the solid is often overlooked. Harvesting the interaction of the nanofluidic transport with the electron transport in solid requires a route effectively coupling ion and electron dynamics. Here we report a nanofluidic analogy of Coulomb drag for exploring the dynamic ion-electron interactions at the liquid-graphene interface.

Deep Learning Enhanced Electrochemiluminescence Microscopy.

Limited by the efficiency of electrochemiluminescence, tens of seconds of exposure time are typically required to get a high-quality image. Image enhancement of short exposure time images to obtain a well-defined electrochemiluminescence image can meet the needs of high-throughput or dynamic imaging. Here, we propose deep enhanced ECL microscopy (DEECL), a general strategy that utilizes artificial neural networks to reconstruct electrochemiluminescence images with millisecond exposure times to have similar quality as high-quality electrochemiluminescence images with second-long exposure time.

Light-Driven Ion Transport through Single-Heterojunction Nanopores.

Inspired by natural photosynthesis, light has become an emerging ionic behavior regulator and ion-pumping source. Nanoprocessing technology has allowed the bridge between the light-regulated nanofluids and the optoelectronic properties of two-dimensional (2D) materials, which inspires applications like energy harvesting and enhances fundamental understandings in nanofluidics. However, unlike light-induced ion pumping based on densely layered membranes with multiple nanochannels, experimental implementation on atomically thin materials featuring only a single nanochannel remains challenging.

Quantitative Single-Molecule Electrochemiluminescence Bioassay.

A single-molecule electrochemiluminescence bioassay is developed here which allows imaging and direct quantification of single biomolecules. Imaging single biomolecules is realized by localizing the electrochemiluminescence events of the labeled molecules. Such an imaging system allows mapping the spatial distribution of biomolecules with electrochemiluminescence and contains quantitative single-molecule insights.

Ionic Liquid Decelerates Single-Stranded DNA Transport through Molybdenum Disulfide Nanopores.

Nanopores in two-dimensional (2D) materials have emerged to offer in principle necessary spatial resolution for high-throughput DNA sequencing. However, their fidelity is severely limited by the fast DNA translocation. A recent experiment indicates that introducing ionic liquids could slow down DNA translocation in a MoS nanopore.

Ion Density-Dependent Dynamic Conductance Switching in Biomimetic Graphene Nanopores.

Gating in ion transport is at the center of many vital living-substance transmission processes, and understanding how gating works at an atomic level is essential but intricate. However, our understanding and finite experimental findings of subcontinuum ion transport in subnanometer nanopores are still limited, which is out of reach of the classical continuum nanofluidics. Moreover, the influence of ion density on subcontinuum ion transport is poorly understood.

Operando Imaging of Chemical Activity on Gold Plates with Single-Molecule Electrochemiluminescence Microscopy.

Classical electrochemical characterization tools cannot avoid averaging between the active reaction sites and their support, thus obscuring their intrinsic roles. Single-molecule electrochemical techniques are thus in high demand. Here, we demonstrate super-resolution imaging of Ru(bpy) based reactions on Au plates using single-molecule electrochemiluminescence microscopy.

Nonlinear electrohydrodynamic ion transport in graphene nanopores.

Mechanosensitivity is one of the essential functionalities of biological ion channels. Synthesizing an artificial nanofluidic system to mimic such sensations will not only improve our understanding of these fluidic systems but also inspire applications. In contrast to the electrohydrodynamic ion transport in long nanoslits and nanotubes, coupling hydrodynamical and ion transport at the single-atom thickness remains challenging.

Dynamic Optical Visualization of Proton Transport Pathways at Water-Solid Interfaces.

Probing proton transport is of vital importance for understanding cellular transport, surface catalysis and fuel cells. Conventional proton transport measurements rely on the use of electrochemical conductivity and do not allow for the direct visualization of proton transport pathways. The development of novel experimental techniques to spatiotemporally resolve proton transport is in high demand.

Etching-Engineered Low-Voltage Dielectrophoretic Nanotweezers for Trapping of Single Molecules.

Understanding the functions of biomolecules at the single-molecule level is crucial due to their important and diverse roles in cell regulation. Recently, nanotweezers made of dual carbon nanoelectrodes have been developed for single-cell biopsies by applying a high alternating voltage. However, high electric voltage can induce Joule heating, water electrolysis, and other side effects on cell activity, which may be unfavorable for cellular applications.

Synthetic Macrocycle Nanopore for Potassium-Selective Transmembrane Transport.

Reproducing the structure and function of biological membrane channels, synthetic nanopores have been developed for applications in membrane filtration technologies and biomolecular sensing. Stable stand-alone synthetic nanopores have been created from a variety of materials, including peptides, nucleic acids, synthetic polymers, and solid-state membranes. In contrast to biological nanopores, however, furnishing such synthetic nanopores with an atomically defined shape, including deliberate placement of each and every chemical group, remains a major challenge.

Direct imaging of single-molecule electrochemical reactions in solution.

Chemical reactions tend to be conceptualized in terms of individual molecules transforming into products, but are usually observed in experiments that probe the average behaviour of the ensemble. Single-molecule methods move beyond ensemble averages and reveal the statistical distribution of reaction positions, pathways and dynamics. This has been shown with optical traps and scanning probe microscopy manipulating and observing individual reactions at defined locations with high spatial resolution, and with modern optical methods using ultrasensitive photodetectors that enable high-throughput single-molecule measurements.

Fabrication and practical applications of molybdenum disulfide nanopores.

Among the different developed solid-state nanopores, nanopores constructed in a monolayer of molybdenum disulfide (MoS) stand out as powerful devices for single-molecule analysis or osmotic power generation. Because the ionic current through a nanopore is inversely proportional to the thickness of the pore, ultrathin membranes have the advantage of providing relatively high ionic currents at very small pore sizes. This increases the signal generated during translocation of biomolecules and improves the nanopores' efficiency when used for desalination or reverse electrodialysis applications.

Wide-Field Spectral Super-Resolution Mapping of Optically Active Defects in Hexagonal Boron Nitride.

Point defects can have significant impact on the mechanical, electronic, and optical properties of materials. The development of robust, multidimensional, high-throughput, and large-scale characterization techniques of defects is thus crucial for the establishment of integrated nanophotonic technologies and material growth optimization. Here, we demonstrate the potential of wide-field spectral single-molecule localization microscopy (SMLM) for the determination of ensemble spectral properties as well as the characterization of spatial, spectral, and temporal dynamics of single defects in chemical vapor deposition (CVD)-grown and irradiated exfoliated hexagonal boron-nitride materials.

Imaging of Optically Active Defects with Nanometer Resolution.

Point defects significantly influence the optical and electrical properties of solid-state materials due to their interactions with charge carriers, which reduce the band-to-band optical transition energy. There has been a demand for developing direct optical imaging methods that would allow in situ characterization of individual defects with nanometer resolution. Here, we demonstrate the localization and quantitative counting of individual optically active defects in monolayer hexagonal boron nitride using single molecule localization microscopy.

Single-layer MoS2 nanopores as nanopower generators.

Making use of the osmotic pressure difference between fresh water and seawater is an attractive, renewable and clean way to generate power and is known as 'blue energy'. Another electrokinetic phenomenon, called the streaming potential, occurs when an electrolyte is driven through narrow pores either by a pressure gradient or by an osmotic potential resulting from a salt concentration gradient. For this task, membranes made of two-dimensional materials are expected to be the most efficient, because water transport through a membrane scales inversely with membrane thickness.

Observation of ionic Coulomb blockade in nanopores.

Emergent behaviour from electron-transport properties is routinely observed in systems with dimensions approaching the nanoscale. However, analogous mesoscopic behaviour resulting from ionic transport has so far not been observed, most probably because of bottlenecks in the controlled fabrication of subnanometre nanopores for use in nanofluidics. Here, we report measurements of ionic transport through a single subnanometre pore junction, and the observation of ionic Coulomb blockade: the ionic counterpart of the electronic Coulomb blockade observed for quantum dots.

Identification of single nucleotides in MoS2 nanopores.

The size of the sensing region in solid-state nanopores is determined by the size of the pore and the thickness of the pore membrane, so ultrathin membranes such as graphene and single-layer molybdenum disulphide could potentially offer the necessary spatial resolution for nanopore DNA sequencing. However, the fast translocation speeds (3,000-50,000 nt ms(-1)) of DNA molecules moving across such membranes limit their usability. Here, we show that a viscosity gradient system based on room-temperature ionic liquids can be used to control the dynamics of DNA translocation through MoS2 nanopores.