Creating functional electrical circuits using individual or ensemble molecules, often termed as “molecular-scale electronics”, not only meets the increasing technical demands of the miniaturization of traditional Si-based electronic devices, but also provides an ideal window of exploring the intrinsic properties of materials at the molecular level. This Review covers the major advances with the most general applicability and emphasizes new insights into the development of efficient platform methodologies for building reliable molecular electronic devices with desired functionalities through the combination of programmed bottom-up self-assembly and sophisticated top-down device fabrication. First, we summarize a number of different approaches of forming molecular-scale junctions and discuss various experimental techniques for examining these nanoscale circuits in details. We then give a full introduction of characterization techniques and theoretical simulations for molecular electronics. Third, we highlig...

Molecular-Scale Electronics: From Concept to Function

Due to the outstanding physicochemical properties arising from its truly two-dimensional (2D) planar structure with a single-atom thickness, graphene exhibits great potential for use in sensors, catalysts, electrodes, and in biological applications, etc. With further developments in the theoretical understanding and assembly techniques, graphene should enable great changes both in scientific research and practical industrial applications. By the look of development, it is of fundamental and practical significance to translate the novel physical and chemical properties of individual graphene nanosheets into the macroscale by the assembly of graphene building blocks into macroscopic architectures with structural specialities and functional novelties. The combined features of a 2D planar structure and abundant functional groups of graphene oxide (GO) should provide great possibilities for the assembly of GO nanosheets into macroscopic architectures with different macroscaled shapes through various assembly techniques under different bonding interactions. Moreover, macroscopic graphene frameworks can be used as ideal scaffolds for the incorporation of functional materials to offset the shortage of pure graphene in the specific desired functionality. The advantages of light weight, supra-flexibility, large surface area, tough mechanical strength, and high electrical conductivity guarantee graphene-based architectures wide application fields. This critical review mainly addresses recent advances in the design and fabrication of graphene-based macroscopic assemblies and architectures and their potential applications. Herein, we first provide overviews of the functional macroscopic graphene materials from three aspects, i.e., 1D graphene fibers/ribbons, 2D graphene films/papers, 3D network-structured graphene monoliths, and their composite counterparts with either polymers or nano-objects. Then, we present the promising potential applications of graphene-based macroscopic assemblies in the fields of electronic and optoelectronic devices, sensors, electrochemical energy devices, and in water treatment. Last, the personal conclusions and perspectives for this intriguing field are given.

Graphene-based macroscopic assemblies and architectures: an emerging material system.

Multifunctional carbon-based nanomaterials offer routes towards the realization of smart and high-performing (opto)electronic (nano)devices, sensors and logic gates. Meanwhile photochromic molecules exhibit reversible transformation between two forms, induced by the absorption of electromagnetic radiation. By combining carbon-based nanomaterials with photochromic molecules, one can achieve reversible changes in geometrical structure, electronic properties and nanoscale mechanics triggering by light. This thus enables a reversible modulation of numerous physical and chemical properties of the carbon-based nanomaterials towards the fabrication of cognitive devices. This review examines the state of the art with respect to these responsive materials, and seeks to identify future directions for investigation.

Coupling carbon nanomaterials with photochromic molecules for the generation of optically responsive materials.

Molecular electronic devices with tunable conductance states show great potential in building memories and logic components for next-generation circuits. In recent years, photoswitchable molecular devices have attracted worldwide interest because of the high spatial and temporal resolution, low cost and non-invasibility of light. Herein, an overview of the progress in photoswitching molecular junctions based on single molecules or self-assembled monolayers of photochromic molecules (i.e., azobenzene, diarylethene, dihydroazulene, spiropyran and dihydropyrene) in the recent decade and a brief description of methods to construct photoswitchable molecular devices are provided. An outlook of the future research directions and challenges for this field is also presented.

Recent progress in the development of molecular-scale electronics based on photoswitchable molecules

Photoswitching dynamics of common organic photoisomers in solid state are often reduced compared to the solution state due to the close packing of molecules that limits structural changes. The facile solid-state switching of photoisomers has implications in developing novel light-controlled devices such as actuator, field-effect transistor, and photodetector, as well as photon energy storage materials that can be charged by light and release thermal energy upon triggering. Thus, the solid-state photoswitching of organic molecules has been studied in relation to the structural characteristics, and various effective methods to enhance the switching in condensed phases have been developed. This review highlights isomerization dynamics of common photoswitches in solid and then introduces important strategies for facilitating the switching dynamics, including the covalent functionalization methods for small-molecule photoswitches as well as the incorporation of various templates such as porous medium, nanoparticle, and host-guest structure. Furthermore, the solid-state switching of molecules at the interface with inorganic substrates including 2D materials and the microscopy techniques for the characterization will be further described.

Solid-state photoswitching molecules: structural design for isomerization in condensed phase

Charge transport properties of chemically reduced graphene oxide (RGO) sheets prepared by treatment with hydrazine were examined using conductive atomic force microscopy. The current-voltage (I-V) characteristics of monolayer RGO sheets prepared under atmospheric pressure followed an exponentially increase due to 2D variable-range hopping conduction through small graphene domains in an RGO sheet containing defect regions of residual sp3 carbon clusters bonded to oxygen groups, whereas RGO sheets prepared in a closed container under moderate pressure showed linear I-V characteristics with a conductivity of 267.2−537.5 S/m. It was found that the chemical reduction under pressure results in larger graphene domains (sp2 networks) in the RGO sheets when compared to that prepared under atmospheric pressure, indicating that the present reduction of GO sheets under the pressure is one of the effective methods to make well-reduced GO sheets.

Local charge transport properties of hydrazine reduced monolayer graphene oxide sheets prepared under pressure condition

A new type of solid-state molecular junction is introduced, which employs reduced graphene oxide as a transparent top contact that permits a self-assembled molecular monolayer to be photoswitched in situ, while simultaneously enabling charge-transport measurements across the molecules. The electrical switching behavior of a less-studied molecular switch, dihydroazulene/vinylheptafulvene, is described, which is used as a test case.

Ultrathin Reduced Graphene Oxide Films as Transparent Top‐Contacts for Light Switchable Solid‐State Molecular Junctions

The hydrophilic poly(2,2,6,6-tetramethylpiperdinyloxy-4-yl-methacrylamide) (PTMAm) was utilized as redox target material in an aqueous organic redox targeting flow battery (RTFB). This polymer is processed into granules, which contain a conductive agent and an alginate binder. By this, a hydrophilic, yet water-insoluble redox target can be obtained. The target was combined with the redox mediator molecule N,N,N-trimethyl-2-oxo-2-((2,2,6,6-tetramethylpiperidin-4-yloxyl)amino)-ethan-1-ammonium chloride (TEMPOAmide), that has been reported earlier as flow battery active material. This target / mediator combination has been characterized electrochemically and flow battery testing has been done. Furthermore, in-operando characterization of the redox target via electrolyte state-of-charge (SOC) monitoring has been performed for the first time. The approach provides estimates for the redox target's SOC changes during cycling. In addition, a figure of merit - the "redox targetivity" - is proposed, which provides insights into the efficiency of the targeting reaction and supports the future optimization of materials, cell designs, and operational parameters for RTFBs.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/cssc.202300296

Organic redox targeting flow battery utilizing a hydrophilic polymer and its in-operando characterization via state-of-charge monitoring of the redox mediator.

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Local charge transport properties of hydrazine reduced monolayer graphene oxide sheets prepared under pressure condition

Ultrathin Reduced Graphene Oxide Films as Transparent Top‐Contacts for Light Switchable Solid‐State Molecular Junctions

Organic redox targeting flow battery utilizing a hydrophilic polymer and its in-operando characterization via state-of-charge monitoring of the redox mediator.