Bjarke Sørensen Jessen

Multi-terminal transport measurements of MoS2 using a van der Waals heterostructure device platform

Atomically thin two-dimensional semiconductors such as MoS2 hold great promise for electrical, optical and mechanical devices and display novel physical phenomena. However, the electron mobility of mono- and few-layer MoS2 has so far been substantially below theoretically predicted limits, which has hampered efforts to observe its intrinsic quantum transport behaviours. Potential sources of disorder and scattering include defects such as sulphur vacancies in the MoS2 itself as well as extrinsic sources such as charged impurities and remote optical phonons from oxide dielectrics. To reduce extrinsic scattering, we have developed here a van der Waals heterostructure device platform where MoS2 layers are fully encapsulated within hexagonal boron nitride and electrically contacted in a multi-terminal geometry using gate-tunable graphene electrodes. Magneto-transport measurements show dramatic improvements in performance, including a record-high Hall mobility reaching 34,000 cm(2) V(-1) s(-1) for six-layer MoS2 at low temperature, confirming that low-temperature performance in previous studies was limited by extrinsic interfacial impurities rather than bulk defects in the MoS2. We also observed Shubnikov-de Haas oscillations in high-mobility monolayer and few-layer MoS2. Modelling of potential scattering sources and quantum lifetime analysis indicate that a combination of short-range and long-range interfacial scattering limits the low-temperature mobility of MoS2.

The hot pick-up technique for batch assembly of van der Waals heterostructures

The assembly of individual two-dimensional materials into van der Waals heterostructures enables the construction of layered three-dimensional materials with desirable electronic and optical properties. A core problem in the fabrication of these structures is the formation of clean interfaces between the individual two-dimensional materials which would affect device performance. We present here a technique for the rapid batch fabrication of van der Waals heterostructures, demonstrated by the controlled production of 22 mono-, bi- and trilayer graphene stacks encapsulated in hexagonal boron nitride with close to 100% yield. For the monolayer devices, we found semiclassical mean-free paths up to 0.9 μm, with the narrowest samples showing clear indications of the transport being affected by boundary scattering. The presented method readily lends itself to fabrication of van der Waals heterostructures in both ambient and controlled atmospheres, while the ability to assemble pre-patterned layers paves the way for complex three-dimensional architectures.

Graphene mobility mapping

Carrier mobility and chemical doping level are essential figures of merit for graphene, and large-scale characterization of these properties and their uniformity is a prerequisite for commercialization of graphene for electronics and electrodes. However, existing mapping techniques cannot directly assess these vital parameters in a non-destructive way. By deconvoluting carrier mobility and density from non-contact terahertz spectroscopic measurements of conductance in graphene samples with terahertz-transparent backgates, we are able to present maps of the spatial variation of both quantities over large areas. The demonstrated non-contact approach provides a drastically more efficient alternative to measurements in contacted devices, with potential for aggressive scaling towards wafers/minute. The observed linear relation between conductance and carrier density in chemical vapour deposition graphene indicates dominance by charged scatterers. Unexpectedly, significant variations in mobility rather than doping are the cause of large conductance inhomogeneities, highlighting the importance of statistical approaches when assessing large-area graphene transport properties.

Electrically continuous graphene from single crystal copper verified by terahertz conductance spectroscopy and micro four-point probe.

The electrical performance of graphene synthesized by chemical vapor deposition and transferred to insulating surfaces may be compromised by extended defects, including for instance grain boundaries, cracks, wrinkles, and tears. In this study, we experimentally investigate and compare the nano- and microscale electrical continuity of single layer graphene grown on centimeter-sized single crystal copper with that of previously studied graphene films, grown on commercially available copper foil, after transfer to SiO2 surfaces. The electrical continuity of the graphene films is analyzed using two noninvasive conductance characterization methods: ultrabroadband terahertz time-domain spectroscopy and micro four-point probe, which probe the electrical properties of the graphene film on different length scales, 100 nm and 10 μm, respectively. Ultrabroadband terahertz time-domain spectroscopy allows for measurement of the complex conductance response in the frequency range 1-15 terahertz, covering the entire intraband conductance spectrum, and reveals that the conductance response for the graphene grown on single crystalline copper intimately follows the Drude model for a barrier-free conductor. In contrast, the graphene grown on commercial copper foil shows a distinctly non-Drude conductance spectrum that is better described by the Drude-Smith model, which incorporates the effect of preferential carrier backscattering associated with extended, electronic barriers with a typical separation on the order of 100 nm. Micro four-point probe resistance values measured on graphene grown on single crystalline copper in two different voltage-current configurations show close agreement with the expected distributions for a continuous 2D conductor, in contrast with previous observations on graphene grown on commercial copper foil. The terahertz and micro four-point probe conductance values of the graphene grown on single crystalline copper shows a close to unity correlation, in contrast with those of the graphene grown on commercial copper foil, which we explain by the absence of extended defects on the microscale in CVD graphene grown on single crystalline copper. The presented results demonstrate that the graphene grown on single crystal copper is electrically continuous on the nanoscopic, microscopic, as well as intermediate length scales.

Fabrication of CVD graphene-based devices via laser ablation for wafer-scale characterization

Selective laser ablation of a wafer-scale graphene film is shown to provide flexible, high speed (1 wafer/hour) device fabrication while avoiding the degradation of electrical properties associated with traditional lithographic methods. Picosecond laser pulses with single pulse peak fluences of 140 mJ cm−2 for 1064 nm, 40 mJ cm−2 for 532 nm, and 30 mJ cm−2 for 355 nm are sufficient to ablate the graphene film, while the ablation onset for Si/SiO2 (thicknesses 500 μm/302 nm) did not occur until 240 mJ cm−2, 150 mJ cm−2, and 135 mJ cm−2, respectively, allowing all wavelengths to be used for graphene ablation without detectable substrate damage. Optical microscopy and Raman Spectroscopy were used to assess the ablation of graphene, while stylus profilometery indicated that the SiO2 substrate was undamaged. CVD graphene devices were electrically characterized and showed comparable field-effect mobility, doping level, on–off ratio, and conductance minimum before and after laser ablation fabrication.

Quality assessment of graphene: Continuity, uniformity, and accuracy of mobility measurements

With the increasing availability of large-area graphene, the ability to rapidly and accurately assess the quality of the electrical properties has become critically important. For practical applications, spatial variability in carrier density and carrier mobility must be controlled and minimized. We present a simple framework for assessing the quality and homogeneity of large-area graphene devices. The field effect in both exfoliated graphene devices encapsulated in hexagonal boron nitride and chemical vapor-deposited (CVD) devices was measured in dual current–voltage configurations and used to derive a single, gate-dependent effective shape factor, β, for each device. β is a sensitive indicator of spatial homogeneity that can be obtained from samples of arbitrary shape. All 50 devices investigated in this study show a variation (up to tenfold) in β as a function of the gate bias. Finite element simulations suggest that spatial doping inhomogeneity, rather than mobility inhomogeneity, is the primary cause of the gate dependence of β, and that measurable variations of β can be caused by doping variations as small as 1010 cm−2. Our results suggest that local variations in the position of the Dirac point alter the current flow and thus the effective sample shape as a function of the gate bias. We also found that such variations lead to systematic errors in carrier mobility calculations, which can be revealed by inspecting the corresponding β factor.

Graphene antidot lattice transport measurements

We investigate graphene devices patterned with a narrow band of holes perpendicular to the current flow, a few-row graphene antidot lattice (FR-GAL). Theoretical reports suggest that a FR-GAL can have a bandgap with a relatively small reduction of the transmission compared to what is typical for antidot arrays devices. Graphene devices were fabricated using 100 keV electron beam lithography (EBL) for nanopatterning as well as for defining electrical contacts. Patterns with hole diameter and neck widths of order 30 nm were produced, which is the highest reported pattern density of antidot lattices in graphene reported defined by EBL. Electrical measurements showed that devices with one and five rows exhibited field effect mobility of ∼100 cm2/Vs, while a larger number of rows, around 40, led to a significant reduction of field effect mobility (<5 cm2/Vs). The carrier mobility was measured as a function of temperature, with the low-temperature behaviour being well described by variable range hopping, indicating the transport to be dominated by disorder.

Defect/oxygen assisted direct write technique for nanopatterning graphene

High resolution nanopatterning of graphene enables manipulation of electronic, optical and sensing properties of graphene. In this work we present a straightforward technique that does not require any lithographic mask to etch nanopatterns into graphene. The technique relies on the damaged graphene to be etched selectively in an oxygen rich environment with respect to non-damaged graphene. Sub-40 nm features were etched into graphene by selectively exposing it to a 100 keV electron beam and then etching the damaged areas away in a conventional oven. Raman spectroscopy was used to evaluate the extent of damage induced by the electron beam as well as the effects of the selective oxidative etching on the remaining graphene.

Raman spectral indicators of catalyst decoupling for transfer of CVD grown 2D materials

Through a combination of monitoring the Raman spectral characteristics of 2D materials grown on copper catalyst layers, and wafer scale automated detection of the fraction of transferred material, we reproducibly achieve transfers with over 97.5% monolayer hexagonal boron nitride and 99.7% monolayer graphene coverage, for up to 300 mm diameter wafers. We find a strong correlation between the transfer coverage obtained for graphene and the emergence of a lower wavenumber 2D− peak component, with the concurrent disappearance of the higher wavenumber 2D+ peak component during oxidation of the catalyst surface. The 2D peak characteristics can therefore act as an unambiguous predictor of the success of the transfer. The combined monitoring and transfer process presented here is highly scalable and amenable for roll-to-roll processing.

Quantitative optical mapping of two-dimensional materials

The pace of two-dimensional materials (2DM) research has been greatly accelerated by the ability to identify exfoliated thicknesses down to a monolayer from their optical contrast. Since this process requires time-consuming and error-prone manual assignment to avoid false-positives from image features with similar contrast, efforts towards fast and reliable automated assignments schemes is essential. We show that by modelling the expected 2DM contrast in digitally captured images, we can automatically identify candidate regions of 2DM. More importantly, we show a computationally-light machine vision strategy for eliminating false-positives from this set of 2DM candidates through the combined use of binary thresholding, opening and closing filters, and shape-analysis from edge detection. Calculation of data pyramids for arbitrarily high-resolution optical coverage maps of two-dimensional materials produced in this way allows the real-time presentation and processing of this image data in a zoomable interface, enabling large datasets to be explored and analysed with ease. The result is that a standard optical microscope with CCD camera can be used as an analysis tool able to accurately determine the coverage, residue/contamination concentration, and layer number for a wide range of presented 2DMs.