RESUMEN
Monitoring conductivity changes of discontinuous palladium (Pd) nanostructures upon hydrogenation is becoming one of the most promising approaches toward hydrogen sensing. Development of sensors in this type has long been impeded due to strong ubiquitous interfacial adhesion which could distinctly restrict Pd expansion so as to hinder the closing of a nanogap. Herein, graphene underlayers were applied in the fabrication of nanogap-based hydrogen sensors to promote the lateral expansion of a Pd nanowire upon hydrogenation by reducing the adhesion between the metal and the substrate. In order to clarify details as well as mechanisms underlaid of graphene-enhanced Pd expansion, nanowire samples with serial lengths (6-48 µm) and gaps (0-260 nm in width) were controllably prepared on single-layer graphene (SLG), double-layer graphene (DLG), and quadruple-layer graphene (QLG, DLG × 2) via the combination of electron beam lithography (EBL) and electron beam deposition (EBD) technology. Response features and intrinsic analysis in physical sense of the graphene-based discontinuous Pd circuits upon hydrogen were established, in light of which the effects of underlayers on Pd expansion and on nanogap closing process were investigated. Such graphene-promoted expansion was demonstrated through the achievement of the closure of a large gap threshold (Gt) up to 260 nm as well as the systematical investigation of its influence on the sensing performance.
RESUMEN
Surface plasmon resonance (SPR) is widely used as light trapping schemes in solar cells, because it can concentrate light fields surrounding metal nanostructures and realize light management at the nanoscale. SPR in photovoltaics generally occurs at the metal/dielectric interfaces. A well-defined interface is therefore required to elucidate interfacial SPR processes. Here, we designed a photovoltaic device (PVD) with an atomically flat TiO2 dielectric/dye/graphene/metal nanoparticle (NP) interface for quantitatively studying the SPR enhancement of the photovoltaic conversion. Theoretical and experimental results indicated that the graphene monolayer was transparent to the electromagnetic field. This transparency led to significant substrate-induced plasmonic hybridization at the heterostructure interface. Combined with interparticle plasmonic coupling, the substrate-induced plasmonics concentrated light at the interface and enhanced the photo-excitation of dyes, thus improving the photoelectric conversion. Such a mechanistic understanding of interfacial plasmonic enhancement will further promote the development of efficient plasmon-enhanced solar cells and composite photocatalysts.
RESUMEN
The development of reliable approaches to integrate individual or a small collection of molecules into electrical nanocircuits, often termed "molecular electronics", is currently a research focus because it can not only overcome the increasing difficulties and fundamental limitations of miniaturization of current silicon-based electronic devices, but can also enable us to probe and understand the intrinsic properties of materials at the atomic- and/or molecular-length scale. This development might also lead to direct observation of novel effects and fundamental discovery of physical phenomena that are not accessible by traditional materials or approaches. Therefore, researchers from a variety of backgrounds have been devoting great effort to this objective, which has started to move beyond simple descriptions of charge transport and branch out in different directions, reflecting the interdisciplinarity. This Account exemplifies our ongoing interest and great effort in developing efficient lithographic methodologies capable of creating molecular electronic devices through the combination of top-down micro/nanofabrication with bottom-up molecular assembly. These devices use nanogapped carbon nanomaterials (such as single-walled carbon nanotubes (SWCNTs) and graphene), with a particular focus on graphene, as point contacts formed by electron beam lithography and precise oxygen plasma etching. Through robust amide linkages, functional molecular bridges terminated with diamine moieties are covalently wired into the carboxylic acid-functionalized nanogaps to form stable carbon electrode-molecule junctions with desired functionalities. At the macroscopic level, to improve the contact interface between electrodes and organic semiconductors and lower Schottky barriers, we used SWCNTs and graphene as efficient electrodes to explore the intrinsic properties of organic thin films, and then build functional high-performance organic nanotransistors with ultrahigh responsivities. At the molecular level, to form robust covalent bonds between electrodes and molecules and improve device stability, we developed a reliable system to immobilize individual molecules within a nanoscale gap of either SWCNTs or graphene through covalent amide bond formation, thus affording two classes of carbon electrode-molecule single-molecule junctions. One unique feature of these devices is the fact that they contain only one or two molecules as conductive elements, thus forming the basis for building new classes of chemo/biosensors with ultrahigh sensitivity. We have used these approaches to reveal the dependence of the charge transport of individual metallo-DNA duplexes on π-stacking integrity, and fabricate molecular devices capable of realizing label-free, real-time electrical detection of biological interactions at the single-event level, or switching their molecular conductance upon exposure to external stimuli, such as ion, pH, and light. These investigations highlight the unique advantages and importance of these universal methodologies to produce functional carbon electrode-molecule junctions in current and future researches toward the development of practical molecular devices, thus offering a reliable platform for molecular electronics and the promise of a new generation of multifunctional integrated circuits and sensors.
RESUMEN
Broadband transparent electrodes based on 2D hybrid nanostructured Dirac materials between Bi2 Se3 and graphene are synthesized using a chemical vapor deposition (CVD) method. Bi2 Se3 nanoplates are preferentially grown along graphene grain boundaries as "smart" conductive patches to bridge the graphene boundary. These hybrid films increase by one- to threefold in conductivity while remaining highly transparent over broadband wavelength. They also display outstanding chemical stability and mechanical flexibility.
