We report transport measurements on a graphene-fullerene single-molecule transistor. The device architecture where a functionalized C60 binds to graphene nanoelectrodes results in strong electron-vibron coupling and weak vibron relaxation. Using a combined approach of transport spectroscopy, Raman spectroscopy, and DFT calculations, we demonstrate center-of-mass oscillations, redox-dependent Franck-Condon blockade, and a transport regime characterized by avalanche tunnelling in a single-molecule transistor.
Provided the electrical properties of electroburnt graphene junctions can be understood and controlled, they have the potential to underpin the development of a wide range of future sub-10-nm electrical devices. We examine both theoretically and experimentally the electrical conductance of electroburnt graphene junctions at the last stages of nanogap formation. We account for the appearance of a counterintuitive increase in electrical conductance just before the gap forms. This is a manifestation of room-temperature quantum interference and arises from a combination of the semimetallic band structure of graphene and a cross-over from electrodes with multiplepath connectivity to single-path connectivity just before breaking. Therefore, our results suggest that conductance enlargement before junction rupture is a signal of the formation of electroburnt junctions, with a picoscale current path formed from a single sp 2 bond.electroburning | graphene | quantum interference | nanoelectronics | picoelectronics
We demonstrate a robust graphene-molecule-graphene transistor architecture. We observe remarkably reproducible single electron charging, which we attribute to insensitivity of the molecular junction to the atomic configuration of the graphene electrodes. The stability of the graphene electrodes allow for high-bias transport spectroscopy and the observation of multiple redox states at room-temperature.
Single layer graphene nano-gaps are fabricated by applying the method of feedback-controlled electroburning to notched ribbon devices, which are plasma etched from CVD grown graphene that is wet-transferred onto pre-patterned metal electrodes. Electrical and structural characterizations show that nanometer size gaps form at the center of the notch. We have processed a total number of 1079 devices using this method with a fabrication yield of 71%. Our results demonstrate precise control over the size and position of the nano-gaps, and open up the possibility of graphene electrodes for large-scale integrated molecular devices.
A demonstration is presented of how significant improvements in all-2D photodetectors can be achieved by exploiting the type-II band alignment of vertically stacked WS /MoS semiconducting heterobilayers and finite density of states of graphene electrodes. The photoresponsivity of WS /MoS heterobilayer devices is increased by more than an order of magnitude compared to homobilayer devices and two orders of magnitude compared to monolayer devices of WS and MoS , reaching 10 A W under an illumination power density of 1.7 × 10 mW cm . The massive improvement in performance is due to the strong Coulomb interaction between WS and MoS layers. The efficient charge transfer at the WS /MoS heterointerface and long trapping time of photogenerated charges contribute to the observed large photoconductive gain of ≈3 × 10 . Laterally spaced graphene electrodes with vertically stacked 2D van der Waals heterostructures are employed for making high-performing ultrathin photodetectors.
We report quantum interference effects in the electrical conductance of chemical vapor deposited graphene nanoconstrictions fabricated using feedback controlled electroburning. The observed multimode Fabry-Pérot interferences can be attributed to reflections at potential steps inside the channel. Sharp antiresonance features with a Fano line shape are observed. Theoretical modeling reveals that these Fano resonances are due to localized states inside the constriction, which couple to the delocalized states that also give rise to the Fabry-Pérot interference patterns. This study provides new insight into the interplay between two fundamental forms of quantum interference in graphene nanoconstrictions.
We study the interactions in graphene/WS2 two-dimensional (2D) layered vertical heterostructures with variations in the areal coverage of graphene by the WS2. All 2D materials were grown by chemical vapor deposition and transferred layer by layer. Photoluminescence (PL) spectroscopy of WS2 on graphene showed PL quenching along with an increase in the ratio of exciton/trion emission, relative to WS2 on SiO2 surface, indicating a reduction in the n-type doping levels of WS2 as well as reduced radiative recombination quantum yield. Electrical measurements of a total of 220 graphene field effect transistors with different WS2 coverage showed double-Dirac points in the field effect measurements, where one is shifted closer toward the 0 V gate neutrality position due to the WS2 coverage. Photoirradiation of the WS2 on graphene region caused further Dirac point shifts, indicative of a reduction in the p-type doping levels of graphene, revealing that the photogenerated excitons in WS2 are split across the heterostructure by electron transfer from WS2 to graphene. Kelvin probe microscopy showed that regions of graphene covered with WS2 had a smaller work function and supports the model of electron transfer from WS2 to graphene. Our results demonstrate the formation of junctions within a graphene transistor through the spatial tuning of the work function of graphene using these 2D vertical heterostructures.
Two-dimensional transition
metal dichalcogenides (TMDCs) have properties
attractive for optoelectronic and quantum applications. A crucial
element for devices is the metal–semiconductor interface. However,
high contact resistances have hindered progress. Quantum transport
studies are scant as low-quality contacts are intractable at cryogenic
temperatures. Here, temperature-dependent transfer length measurements
are performed on chemical vapor deposition grown single-layer and
bilayer WS2 devices with indium alloy contacts. The devices
exhibit low contact resistances and Schottky barrier heights (∼10
kΩ μm at 3 K and 1.7 meV). Efficient carrier injection
enables high carrier mobilities (∼190 cm2 V–1 s–1) and observation of resonant
tunnelling. Density functional theory calculations provide insights
into quantum transport and properties of the WS2–indium
interface. Our results reveal significant advances toward high-performance
WS2 devices using indium alloy contacts.
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