Exceptionally clean single-electron transistors from solutions of molecular graphene nanoribbons.

Only single-electron transistors with a certain level of cleanliness, where all states can be properly accessed, can be used for quantum experiments. To reveal their exceptional properties, carbon nanomaterials need to be stripped down to a single element: graphene has been exfoliated into a single sheet, and carbon nanotubes can reveal their vibrational, spin and quantum coherence properties only after being suspended across trenches1-3. Molecular graphene nanoribbons4-6 now provide carbon nanostructures with single-atom precision but suffer from poor solubility, similar to carbon nanotubes. Here we demonstrate the massive enhancement of the solubility of graphene nanoribbons by edge functionalization, to yield ultra-clean transport devices with sharp single-electron features. Strong electron-vibron coupling leads to a prominent Franck-Condon blockade, and the atomic definition of the edges allows identifying the associated transverse bending mode. These results demonstrate how molecular graphene can yield exceptionally clean electronic devices directly from solution. The sharpness of the electronic features opens a path to the exploitation of spin and vibrational properties in atomically precise graphene nanostructures.

Deep learning-enabled prediction of 2D material breakdown.

Characterizing electrical breakdown limits of materials is a crucial step in device development. However, methods for repeatable measurements are scarce in two-dimensional materials, where breakdown studies have been limited to destructive methods. This restricts our ability to fully account for variability in local electronic properties induced by surface contaminants and the fabrication process. To tackle this, we implement a two-step deep-learning model to predict the breakdown mechanism and breakdown voltage of monolayer MoS2devices with varying channel lengths and resistances using current measured in the low-voltage regime as inputs. A deep neural network (DNN) first classifies between Joule and avalanche breakdown mechanisms using partial current traces from 0 to 20 V. Following this, a convolutional long short-term memory network (CLSTM) predicts breakdown voltages of these classified devices based on partial current traces. We test our model with electrical measurements collected using feedback-control of the applied voltage to prevent device destruction, and show that the DNN classifier achieves an accuracy of 79% while the CLSTM model has a 12% error when requiring only 80% of the current trace as inputs. Our results indicate that information encoded in the current behavior far from the breakdown point can be used for breakdown predictions, which will enable non-destructive and rapid material characterization for 2D material device development.

Conductance enlargement in picoscale electroburnt graphene nanojunctions.

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 multiple-path 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.

Redox-Dependent Franck-Condon Blockade and Avalanche Transport in a Graphene-Fullerene Single-Molecule Transistor.

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.

Quantum Interference in Graphene Nanoconstrictions.

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.

Nanoironing van der Waals Heterostructures toward Electrically Controlled Quantum Dots.

Assembling two-dimensional van der Waals (vdW)-layered materials into heterostructures is an exciting development that sparked the discovery of rich correlated electronic phenomena. vdW heterostructures also offer possibilities for designer device applications in areas such as optoelectronics, valley- and spintronics, and quantum technology. However, realizing the full potential of these heterostructures requires interfaces with exceptionally low disorder which is challenging to engineer. Here, we show that thermal scanning probes can be used to create pristine interfaces in vdW heterostructures. Our approach is compatible at both the material- and device levels, and monolayer WS2 transistors show up to an order of magnitude improvement in electrical performance from this technique. We also demonstrate vdW heterostructures with low interface disorder enabling the electrical formation and control of quantum dots that can be tuned from macroscopic current flow to the single-electron tunneling regime.

Dielectrics for Two-Dimensional Transition-Metal Dichalcogenide Applications.

Despite over a decade of intense research efforts, the full potential of two-dimensional transition-metal dichalcogenides continues to be limited by major challenges. The lack of compatible and scalable dielectric materials and integration techniques restrict device performances and their commercial applications. Conventional dielectric integration techniques for bulk semiconductors are difficult to adapt for atomically thin two-dimensional materials. This review provides a brief introduction into various common and emerging dielectric synthesis and integration techniques and discusses their applicability for 2D transition metal dichalcogenides. Dielectric integration for various applications is reviewed in subsequent sections including nanoelectronics, optoelectronics, flexible electronics, valleytronics, biosensing, quantum information processing, and quantum sensing. For each application, we introduce basic device working principles, discuss the specific dielectric requirements, review current progress, present key challenges, and offer insights into future prospects and opportunities.

Liquid-Metal-Printed Ultrathin Oxides for Atomically Smooth 2D Material Heterostructures.

Two-dimensional (2D) semiconductors are promising channel materials for continued downscaling of complementary metal-oxide-semiconductor (CMOS) logic circuits. However, their full potential continues to be limited by a lack of scalable high-k dielectrics that can achieve atomically smooth interfaces, small equivalent oxide thicknesses (EOTs), excellent gate control, and low leakage currents. Here, large-area liquid-metal-printed ultrathin Ga2O3 dielectrics for 2D electronics and optoelectronics are reported. The atomically smooth Ga2O3/WS2 interfaces enabled by the conformal nature of liquid metal printing are directly visualized. Atomic layer deposition compatibility with high-k Ga2O3/HfO2 top-gate dielectric stacks on a chemical-vapor-deposition-grown monolayer WS2 is demonstrated, achieving EOTs of ∼1 nm and subthreshold swings down to 84.9 mV/dec. Gate leakage currents are well within requirements for ultrascaled low-power logic circuits. These results show that liquid-metal-printed oxides can bridge a crucial gap in dielectric integration of 2D materials for next-generation nanoelectronics.

Gate-Defined Quantum Confinement in CVD 2D WS2.

Temperature-dependent transport measurements are performed on the same set of chemical vapor deposition (CVD)-grown WS2 single- and bilayer devices before and after atomic layer deposition (ALD) of HfO2 . This isolates the influence of HfO2 deposition on low-temperature carrier transport and shows that carrier mobility is not charge impurity limited as commonly thought, but due to another important but commonly overlooked factor: interface roughness. This finding is corroborated by circular dichroic photoluminescence spectroscopy, X-ray photoemission spectroscopy, cross-sectional scanning transmission electron microscopy, carrier-transport modeling, and density functional modeling. Finally, electrostatic gate-defined quantum confinement is demonstrated using a scalable approach of large-area CVD-grown bilayer WS2 and ALD-grown HfO2 . The high dielectric constant and low leakage current enabled by HfO2 allows an estimated quantum dot size as small as 58 nm. The ability to lithographically define increasingly smaller devices is especially important for transition metal dichalcogenides due to their large effective masses, and should pave the way toward their use in quantum information processing applications.

Quantum Transport in Two-Dimensional WS2 with High-Efficiency Carrier Injection through Indium Alloy Contacts.

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.

Carrier control in 2D transition metal dichalcogenides with Al2O3 dielectric.

We report transport measurements of dual gated MoS2 and WSe2 devices using atomic layer deposition grown Al2O3 as gate dielectrics. We are able to achieve current pinch-off using independent split gates and observe current steps suggesting possible carrier confinement. We also investigated the impact of gate geometry and used electrostatic potential simulations to explain the observed device physics.

Lateral Graphene-Contacted Vertically Stacked WS2 /MoS2 Hybrid Photodetectors with Large Gain.

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 WS2 /MoS2 semiconducting heterobilayers and finite density of states of graphene electrodes. The photoresponsivity of WS2 /MoS2 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 WS2 and MoS2 , reaching 103 A W-1 under an illumination power density of 1.7 × 102 mW cm-2 . The massive improvement in performance is due to the strong Coulomb interaction between WS2 and MoS2 layers. The efficient charge transfer at the WS2 /MoS2 heterointerface and long trapping time of photogenerated charges contribute to the observed large photoconductive gain of ≈3 × 104 . Laterally spaced graphene electrodes with vertically stacked 2D van der Waals heterostructures are employed for making high-performing ultrathin photodetectors.

Doping Graphene Transistors Using Vertical Stacked Monolayer WS2 Heterostructures Grown by Chemical Vapor Deposition.

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.

Graphene-porphyrin single-molecule transistors.

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.