Ultra-highly conductive optoelectronic modulated single-molecule nickel bis(dithiolene) junctions with strong molecule-electrode coupling.

Strong molecule-electrode coupling originating from orbit hybridization between gold and the delocalized molecular wires in single-molecule junctions facilitates facile transport towards smart molecular devices. In this paper, we report ultra-highly conductive single-molecule circuits based on highly delocalized nickel bis(dithiolene) (NiS) molecular junctions using scanning tunneling microscope break junction technique. Single-molecule charge transport measurement of both NiS reveals they exhibits high conductance of 10G and 10G, respectively.

Aniline tetramer conjugated N-doped graphene aerogel enabling efficient pH-universal aqueous supercapacitors.

The development of novel negative electrode (anode) materials for efficient aqueous supercapacitors (SCs) remains appealing yet significantly challenging. Here we propose an aniline tetramer conjugated nitrogen-doped graphene aerogel (AT-NGA) as the anode material, exhibiting a maximum capacitance of 699.1F g under 1 A/g in 1 M HSO as well as a long lifespan of 6,000 cycles at all pH levels.

Efficient Exciton Dissociation on Ceria Chelated Cerium-Based MOF Isogenous S-Scheme Photocatalyst for Acetaldehyde Purification.

Long-term exposure to low concentration indoor VOCs of acetaldehyde (CHCHO) is harmful to human health. Thus, a novel isogenous heterojunction CeO/Ce-MOF photocatalyst is synthesized via a one-step hydrothermal method for the effective elimination of CHCHO in this work. This CeO/Ce-MOF photocatalyst performs well in CHCHO removal and achieves an apparent quantum efficiency of 7.

Spatial charge separated two-dimensional/two-dimensional Cu-InS/CdS heterojunction for boosting photocatalytic hydrogen production.

Two-dimensional (2D) beta indium sulfide (β-InS) shows great potential in photocatalytic hydrogen production due to its broad-spectrum response, relatively negative conduction band edge, high carrier mobility and low toxicity. However, the high charge recombination rate limits the application of InS. Here, we in-situ grew 2D cadmium sulfide (CdS) on the surface of InS doped with copper ions (Cu) to construct a heterojunction photocatalyst that suppresses charge recombination.

Efficient pH-universal aqueous supercapacitors enabled by an azure C-decorated N-doped graphene aerogel.

Current aqueous supercapacitors (SCs) possess the relative low energy density, and there is therefore widespread interest in cost-effective fabrication of capacitive materials with promoted specific capacitance and/or broadened voltage window. Here, a redox-active azure C-decorated N-doped graphene aerogel (AC - NGA) is fabricated using a simple hydrothermal self-assembly method through strong noncovalent π-π interaction. AC - NGA highlights an excellent charge storage performance (a high 591F g gravimetric capacitance under a current density of 1.

Supramolecular Radical Electronics.

Supramolecular radical chemistry is an emerging area bridging supramolecular chemistry and radical chemistry, and the integration of radicals into the supramolecular architecture offers a new dimension for tuning their structures and functions. Although various efforts have been devoted to the fabrication of supramolecular junctions, the charge transport characterization through the supramolecular radicals remained unexplored due to the challenges in creating supramolecular radicals at the single-molecule level. Here, we demonstrate the fabrication and charge transport investigation of a supramolecular radical junction using the electrochemical scanning tunneling microscope-based break junction (EC-STM-BJ) technique.

Ternary dual S-scheme InO/SnInS/CdS heterojunctions for boosted light-to-hydrogen conversion.

Developing artificial S-scheme systems with highly active catalysts is significant to long-term solar-to-hydrogen conversion. Herein, CdS nanodots-modified hierarchical InO/SnInS hollow nanotubes were synthesized by an oil bath method for water splitting. Benefiting from the synergy among the hollow structure, tiny size effect, matched energy level positions, and abundant coupling heterointerfaces, the optimized nanohybrid attains an impressive photocatalytic hydrogen evolution rate of 110.

Scaling of quantum interference from single molecules to molecular cages and their monolayers.

The discovery of quantum interference (QI) is widely considered as an important advance in molecular electronics since it provides unique opportunities for achieving single-molecule devices with unprecedented performance. Although some pioneering studies suggested the presence of spin qubit coherence and QI in collective systems such as thin films, it remains unclear whether the QI can be transferred step-by-step from single molecules to different length scales, which hinders the application of QI in fabricating active molecular devices. Here, we found that QI can be transferred from a single molecule to their assemblies.

σ-dominated charge transport in sub-nanometer molecular junctions.

Quantum tunneling conductance of molecular junctions originates from the charge transport through the π-orbitals (π-transport) and the σ-orbitals (σ-transport) of the molecules, but the σ-transport can not be observed due to the more rapid decay of the tunneling conductance in the σ-system compared to that in the π-system. Here, we demonstrate that dominant σ-transport can be observed in π-conjugated molecular junctions at the sub-nanometer scale using the scanning tunneling microscope break junction technique (STM-BJ). We have found that the conductance of -connected picolinic acid, which mainly occurs by σ-transport, is ∼35 times higher than that of its -isomer, which is entirely different from what is expected from π-transport through these systems.

Corrigendum: Application of One-Dimensional Nanomaterials in Catalysis at the Single-Molecule and Single-Particle Scale.

[This corrects the article DOI: 10.3389/fchem.2021.

Application of One-Dimensional Nanomaterials in Catalysis at the Single-Molecule and Single-Particle Scale.

The morphology of nanomaterials has a great influence on the catalytic performance. One-dimensional (1D) nanomaterials have been widely used in the field of catalysis due to their unique linear morphology with large specific surface area, high electron-hole separation efficiency, strong light absorption capacity, plentiful exposed active sites, and so on. In this review, we summarized the recent progress of 1D nanomaterials by focusing on the applications in photocatalysis and electrocatalysis.

The Characterization of Electronic Noise in the Charge Transport through Single-Molecule Junctions.

With the goal of creating single-molecule devices and integrating them into circuits, the emergence of single-molecule electronics provides various techniques for the fabrication of single-molecule junctions and the investigation of charge transport through such junctions. Among the techniques for characterization of charge transport through molecular junctions, electronic noise characterization is an effective strategy with which issues from molecule-electrode interfaces, mechanisms of charge transport, and changes in junction configurations are studied. Electronic noise analysis in single-molecule junctions can be used to identify molecular conformations and even monitor reaction kinetics.

The Evolution of the Charge Transport Mechanism in Single-Molecule Break Junctions Revealed by Flicker Noise Analysis.

The electronic noise characterization of single-molecule devices provides insights into the mechanisms of charge transport. In this work, it is reported that flicker noise can serve as an indicator of the time-dependent evolution of charge transport mechanisms in the single-molecule break junction process. By introducing time-frequency analysis, the authors find that flicker noise components of the molecule junction show time evolution behavior in the dynamic break junction process.

Tracking Confined Reaction Based on Host-Guest Interaction Using Single-Molecule Conductance Measurement.

The host-guest interaction acts as an essential part of supramolecular chemistry, which can be applied in confined reaction. However, it is challenging to obtain the dynamic process during confined reactions below micromolar concentrations. In this work, a new method is provided to characterize the dimerization process of the guest 1,2-bis(4-pyridinyl) ethylene in host cucurbit[8]curil using scanning tunneling microscope-break junction (STM-BJ) technique.

Single-atom control of electrical conductance and thermopower through single-cluster junctions.

The control of single atoms offers fundamental insight into understanding the charge transport through single clusters, and the atomic precision of the clusters provides the opportunity to manipulate the charge transport even at the single-atom level. Herein, we designed and investigated the electrical conductance and thermopower of Anderson-type polyoxometalate (POM) clusters with single-atom variation using the scanning tunneling microscopy break-junction (STM-BJ) technique. Our results show the electrical conductance of single clusters can be changed by an order of magnitude by substituting different center-metal atoms, and the electrical conductance of clusters shows different bias-dependence.

Electric field-induced switching among multiple conductance pathways in single-molecule junctions.

Here, we report the switching among multiple conductance pathways achieved by sliding the scanning tunneling microscope tip among different binding sites under different electric fields. With an increase in the electric field, high molecular conductance states appear, suggesting the formation of different configurations in single-molecule junctions. The switch can be operated in situ and reversibly, which is also confirmed by the apparent conductance conversion in I-V measurements.