Intrinsic Electronic Transport Properties of High-Quality Monolayer and Bilayer MoS₂

We report electronic transport measurements of devices based on monolayers and bilayers of the transition-metal dichalcogenide MoS₂. Through a combination of in situ vacuum annealing and electrostatic gating we obtained ohmic contact to the MoS₂ down to 4 K at high carrier densities. At lower carrier densities, low-temperature four probe transport measurements show a metal–insulator transition in both monolayer and bilayer samples. In the metallic regime, the high-temperature behavior of the mobility showed strong temperature dependence consistent with phonon-dominated transport. At low temperature, intrinsic field-effect mobilities approaching 1000 cm²/(V·s) were observed for both monolayer and bilayer devices. Mobilities extracted from Hall effect measurements were several times lower and showed a strong dependence on density, likely caused by screening of charged impurity scattering at higher densities

Photoresponse of an Electrically Tunable Ambipolar Graphene Infrared Thermocouple

We explore the photoresponse of an ambipolar graphene infrared thermocouple at photon energies close to or below monolayer graphene’s optical phonon energy and electrostatically accessible Fermi energy levels. The ambipolar graphene infrared thermocouple consists of monolayer graphene supported by an infrared absorbing material, controlled by two independent electrostatic gates embedded below the absorber. Using a scanning infrared laser microscope, we characterize these devices as a function of carrier type and carrier density difference controlled at the junction between the two electrostatic gates. On the basis of these measurements, conducted at both mid- and near-infrared wavelengths, the primary detection mechanism can be modeled as a thermoelectric response. By studying the effect of different infrared absorbers, we determine that the optical absorption and thermal conduction of the substrate play the dominant role in the measured photoresponse of our devices. These experiments indicate a path toward hybrid graphene thermal detectors for sensing applications such as thermography and chemical spectroscopy

Electronic Transport of Encapsulated Graphene and WSe₂ Devices Fabricated by Pick-up of Prepatterned hBN

We report high quality graphene and WSe₂ devices encapsulated between two hexagonal boron nitride (hBN) flakes using a pick-up method with etched hBN flakes. Picking up prepatterned hBN flakes to be used as a gate dielectric or mask for other 2D materials opens new possibilities for the design and fabrication of 2D heterostructures. In this Letter, we demonstrate this technique in two ways: first, a dual-gated graphene device that is encapsulated between an hBN substrate and prepatterned hBN strips. The conductance of the graphene device shows pronounced Fabry–Pérot oscillations as a function of carrier density, which implies strong quantum confinement and ballistic transport in the locally gated region. Second, we describe a WSe₂ device encapsulated in hBN with the top hBN patterned as a mask for the channel of a Hall bar. Ionic liquid selectively tunes the carrier density of the contact region of the device, while the hBN mask allows independent tunability of the contact region for low contact resistance. Hall mobility larger than 600 cm²/(V·s) for few-layer p-type WSe₂ at 220 K is measured, the highest mobility of a thin WSe₂ device reported to date. The observations of ballistic transport in graphene and high mobility in WSe₂ confirm pick-up of prepatterned hBN as a versatile technique to fabricate ultraclean devices with high quality contact

Disorder Imposed Limits of Mono- and Bilayer Graphene Electronic Modification Using Covalent Chemistry

A central question in graphene chemistry is to what extent chemical modification can control an electronically accessible band gap in monolayer and bilayer graphene (MLG and BLG). Density functional theory predicts gaps in covalently functionalized graphene as high as 2 eV, while this approach neglects the fact that lattice symmetry breaking occurs over only a prescribed radius of nanometer dimension, which we label the S-region. Therefore, high chemical conversion is central to observing this band gap in transport. We use an electrochemical approach involving phenyl-diazonium salts to systematically probe electronic modification in MLG and BLG with increasing functionalization for the first time, obtaining the highest conversion values to date. We find that both MLG and BLG retain their relatively high conductivity after functionalization even at high conversion, as mobility losses are offset by increases in carrier concentration. For MLG, we find that band gap opening as measured during transport is linearly increased with respect to the <i>I</i>_<i>D</i>/<i>I</i>_<i>G</i> ratio but remains below 0.1 meV in magnitude for SiO₂ supported graphene. The largest transport band gap obtained in a suspended, highly functionalized (<i>I</i>_<i>D</i>/<i>I</i>_<i>G</i> = 4.5) graphene is about 1 meV, lower than our theoretical predictions considering the quantum interference effect between two neighboring S-regions and attributed to its population with midgap states. On the other hand, heavily functionalized BLG (<i>I</i>_<i>D</i>/<i>I</i>_<i>G</i> = 1.8) still retains its signature dual-gated band gap opening due to electric-field symmetry breaking. We find a notable asymmetric deflection of the charge neutrality point (CNP) under positive bias which increases the apparent on/off current ratio by 50%, suggesting that synergy between symmetry breaking, disorder, and quantum interference may allow the observation of new transistor phenomena. These important observations set definitive limits on the extent to which chemical modification can control graphene electronically

Graphene-Based Thermopile for Thermal Imaging Applications

In this work, we leverage graphene’s unique tunable Seebeck coefficient for the demonstration of a graphene-based thermal imaging system. By integrating graphene based photothermo-electric detectors with micromachined silicon nitride membranes, we are able to achieve room temperature responsivities on the order of ∼7–9 V/W (at λ = 10.6 μm), with a time constant of ∼23 ms. The large responsivities, due to the combination of thermal isolation and broadband infrared absorption from the underlying SiN membrane, have enabled detection as well as stand-off imaging of an incoherent blackbody target (300–500 K). By comparing the fundamental achievable performance of these graphene-based thermopiles with standard thermocouple materials, we extrapolate that graphene’s high carrier mobility can enable improved performances with respect to two main figures of merit for infrared detectors: detectivity (>8 × 10⁸ cm Hz^1/2 W^–1) and noise equivalent temperature difference (<100 mK). Furthermore, even average graphene carrier mobility (<1000 cm² V^–1 s^–1) is still sufficient to detect the emitted thermal radiation from a human target

Efficiency of Launching Highly Confined Polaritons by Infrared Light Incident on a Hyperbolic Material

We investigated phonon–polaritons in hexagonal boron nitridea naturally hyperbolic van der Waals materialby means of the scattering-type scanning near-field optical microscopy. Real-space nanoimages we have obtained detail how the polaritons are launched when the light incident on a thin hexagonal boron nitride slab is scattered by various intrinsic and extrinsic inhomogeneities, including sample edges, metallic nanodisks deposited on its top surface, random defects, and surface impurities. The scanned tip of the near-field microscope is itself a polariton launcher whose efficiency proves to be superior to all the other types of polariton launchers we studied. Our work may inform future development of polaritonic nanodevices as well as fundamental studies of collective modes in van der Waals materials