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

Charge-transfer Contact to a High-Mobility Monolayer Semiconductor

Two-dimensional (2D) semiconductors, such as the transition metal dichalcogenides, have demonstrated tremendous promise for the development of highly tunable quantum devices. Realizing this potential requires low-resistance electrical contacts that perform well at low temperatures and low densities where quantum properties are relevant. Here we present a new device architecture for 2D semiconductors that utilizes a charge-transfer layer to achieve large hole doping in the contact region, and implement this technique to measure magneto-transport properties of high-purity monolayer WSe$_2$. We measure a record-high hole mobility of 80,000 cm$^2$/Vs and access channel carrier densities as low as $1.6\times10^{11}$ cm$^{-2}$, an order of magnitude lower than previously achievable. Our ability to realize transparent contact to high-mobility devices at low density enables transport measurement of correlation-driven quantum phases including observation of a low temperature metal-insulator transition in a density and temperature regime where Wigner crystal formation is expected, and observation of the fractional quantum Hall effect under large magnetic fields. The charge transfer contact scheme paves the way for discovery and manipulation of new quantum phenomena in 2D semiconductors and their heterostructures

Single-crystalline gold nanodisks on WS2_2 mono- and multilayers: Strong coupling at room temperature

Engineering light-matter interactions up to the strong-coupling regime at room temperature is one of the cornerstones of modern nanophotonics. Achieving this goal will enable new platforms for potential applications such as quantum information processing, quantum light sources and even quantum metrology. Materials like transition metal dichalcogenides (TMDC) and in particular tungsten disulfide (WS$_2$) possess large transition dipole moments comparable to semiconductor-based quantum dots, and strong exciton binding energies allowing the detailed exploration of light-matter interactions at room temperature. Additionally, recent works have shown that coupling TMDCs to plasmonic nanocavities with light tightly focused on the nanometer scale can reach the strong-coupling regime at ambient conditions. Here, we use ultra-thin single-crystalline gold nanodisks featuring large in-plane electromagnetic dipole moments aligned with the exciton transition-dipole moments located in monolayer WS$_2$. Through scattering and reflection spectroscopy we demonstrate strong coupling at room temperature with a Rabi splitting of $\sim$108 meV. In order to go further into the strong-coupling regime and inspired by recent experimental work by St\"uhrenberg et al., we couple these nanodisks to multilayer WS$_2$. Due to an increase in the number of excitons coupled to our nanodisks, we achieve a Rabi splitting of $\sim$175 meV, a major increase of 62%. To our knowledge, this is the highest Rabi splitting reported for TMDCs coupled to open plasmonic cavities. Our results suggest that ultra-thin single-crystalline gold nanodisks coupled to WS$_2$ represent an exquisite platform to explore light-matter interactions

High-quality graphene flakes exfoliated on a flat hydrophobic polymer

We show that graphene supported on a hydrophobic and flat polymer surface results in flakes with extremely low doping and strain as assessed by their Raman spectroscopic characteristics. We exemplify this technique by micromechanical exfoliation of graphene on flat poly(methylmethacrylate) layers and demonstrate Raman peak intensity ratios I(2D)/I(G) approaching 10, similar to pristine freestanding graphene. We verify that these features are not an artifact of optical interference effects occurring at the substrate: they are similarly observed when varying the substrate thickness and are maintained when the environment of the graphene flake is completely changed, by encapsulating preselected flakes between hexagonal boron nitride layers. The exfoliation of clean, pristine graphene layers directly on flat polymer substrates enables high performance, supported, and non-encapsulated graphene devices for flexible and transparent optoelectronic studies. We additionally show that the access to a clean and supported graphene source leads to high-quality van der Waals heterostructures and devices with reproducible carrier mobilities exceeding 50 000 cm2V-1s-1at room temperature

Catalyst Interface Engineering for Improved 2D Film Lift-Off and Transfer

The mechanisms by which chemical vapor deposited (CVD) graphene and hexagonal boron nitride (h-BN) films can be released from a growth catalyst, such as widely used copper (Cu) foil, are systematically explored as a basis for an improved lift-off transfer. We show how intercalation processes allow the local Cu oxidation at the interface followed by selective oxide dissolution, which gently releases the 2D material (2DM) film. Interfacial composition change and selective dissolution can thereby be achieved in a single step or split into two individual process steps. We demonstrate that this method is not only highly versatile but also yields graphene and h-BN films of high quality regarding surface contamination, layer coherence, defects, and electronic properties, without requiring additional post-transfer annealing. We highlight how such transfers rely on targeted corrosion at the catalyst interface and discuss this in context of the wider CVD growth and 2DM transfer literature, thereby fostering an improved general understanding of widely used transfer processes, which is essential to numerous other applications.We acknowledge funding from the ERC (InsituNANO, grant 279342). R.W. acknowledges an EPSRC Doctoral Training Award (EP/M506485/1). During this work, S.T. was supported in parts by a DFG research fellowship under grant TA 1122/1-1:1. J.A.A.-W. acknowledges a Research Fellowship from Churchill College, Cambridge. Z.A.V.V. acknowledges funding from ESPRC grant EP/L016087/1. P.B. and B.S.J. thank the Danish National Research Foundation Centre for Nanostructured graphene, DNRF103, and EU Horizon 2020 “Graphene Flagship” 696656. T.J.B. and P.R.W. acknowledge financial support from EU FP7-6040007 “GLADIATOR” and Innovation Fund Denmark Da-Gate 0603-005668B. P.R.K. acknowledges a Lindemann Trust Fellowship

Nanometer-Scale Lateral p–n Junctions in Graphene/α-RuCl3 Heterostructures

[EN] The ability to create nanometer-scale lateral p-n junctions is essential for the next generation of two-dimensional (2D) devices. Using the charge-transfer heterostructure graphene/alpha-RuCl3, we realize nanoscale lateral p-n junctions in the vicinity of graphene nanobubbles. Our multipronged experimental approach incorporates scanning tunneling microscopy (STM) and spectroscopy (STS) and scattering-type scanning near-field optical microscopy (s-SNOM) to simultaneously probe the electronic and optical responses of nanobubble p-n junctions. Our STM/STS results reveal that p-n junctions with a band offset of 0.6 eV can be achieved with widths of 3 nm, giving rise to electric fields of order 108 V/m. Concurrent s-SNOM measurements validate a point-scatterer formalism for modeling the interaction of surface plasmon polaritons (SPPs) with nanobubbles. Ab initio density functional theory (DFT) calculations corroborate our experimental data and reveal the dependence of charge transfer on layer separation. Our study provides experimental and conceptual foundations for generating p-n nanojunctions in 2D materials.Research at Columbia University was supported as part of the Energy Frontier Research Center on Programmable Quantum Materials funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under Award No DE-SC0019443. Plasmonic nano-imaging at Columbia University was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under Award No DE-SC0018426. J.Z. and A.R. were supported by the European Research Council (ERC-2015-AdG694097), the Cluster of Excellence “Advanced Imaging of Matter” (AIM) EXC 2056-390715994, funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under RTG 2247, Grupos Consolidados (IT1249-19), and SFB925 “Light induced dynamics and control of correlated quantum systems”. J.Z. and A.R. would like to acknowledge Nicolas Tancogne-Dejean and Lede Xian for fruitful discussions and also acknowledge support by the Max Planck Institute-New York City Center for Non-Equilibrium Quantum Phenomena. The Flatiron Institute is a division of the Simons Foundation. J.Z. acknowledges funding received from the European Union Horizon 2020 research and innovation programme under Marie Skłodowska-Curie Grant Agreement 886291 (PeSD-NeSL). STM support was provided by the National Science Foundation via Grant DMR-2004691. C.R.-V. acknowledges funding from the European Union Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie Grant Agreement 844271. D.G.M. acknowledges support from the Gordon and Betty Moore Foundation’s EPiQS Initiative, Grant GBMF9069. J.Q.Y. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. S.E.N. acknowledges support from the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Division of Scientific User Facilities. Work at University of Tennessee was supported by NSF Grant 180896

Graphene/α\alpha-RuCl3_3: An Emergent 2D Plasmonic Interface

Work function-mediated charge transfer in graphene/$\alpha$-RuCl$_3$ heterostructures has been proposed as a strategy for generating highly-doped 2D interfaces. In this geometry, graphene should become sufficiently doped to host surface and edge plasmon-polaritons (SPPs and EPPs, respectively). Characterization of the SPP and EPP behavior as a function of frequency and temperature can be used to simultaneously probe the magnitude of interlayer charge transfer while extracting the optical response of the interfacial doped $\alpha$-RuCl$_3$. We accomplish this using scanning near-field optical microscopy (SNOM) in conjunction with first-principles DFT calculations. This reveals massive interlayer charge transfer (2.7 $\times$ 10$^{13}$ cm$^{-2}$) and enhanced optical conductivity in $\alpha$-RuCl$_3$ as a result of significant electron doping. Our results provide a general strategy for generating highly-doped plasmonic interfaces in the 2D limit in a scanning probe-accessible geometry without need of an electrostatic gate.Comment: 22 pages, 5 figure

Programming moir\'e patterns in 2D materials by bending

Moir\'e superlattices in twisted two-dimensional materials have generated tremendous excitement as a platform for achieving quantum properties on demand. However, the moir\'e pattern is highly sensitive to the interlayer atomic registry, and current assembly techniques suffer from imprecise control of the average twist angle, spatial inhomogeneity in the local twist angle, and distortions due to random strain. Here, we demonstrate a new way to manipulate the moir\'e patterns in hetero- and homo-bilayers through in-plane bending of monolayer ribbons, using the tip of an atomic force microscope. This technique achieves continuous variation of twist angles with improved twist-angle homogeneity and reduced random strain, resulting in moir\'e patterns with highly tunable wavelength and ultra-low disorder. Our results pave the way for detailed studies of ultra-low disorder moir\'e systems and the realization of precise strain-engineered devices

Nanometer-scale lateral p-n junctions in graphene/α-RuCl3 heterostructures

The ability to create nanometer-scale lateral p–n junctions is essential for the next generation of two-dimensional (2D) devices. Using the charge-transfer heterostructure graphene/α-RuCl3, we realize nanoscale lateral p–n junctions in the vicinity of graphene nanobubbles. Our multipronged experimental approach incorporates scanning tunneling microscopy (STM) and spectroscopy (STS) and scattering-type scanning near-field optical microscopy (s-SNOM) to simultaneously probe the electronic and optical responses of nanobubble p–n junctions. Our STM/STS results reveal that p–n junctions with a band offset of ∼0.6 eV can be achieved with widths of ∼3 nm, giving rise to electric fields of order 108 V/m. Concurrent s-SNOM measurements validate a point-scatterer formalism for modeling the interaction of surface plasmon polaritons (SPPs) with nanobubbles. Ab initio density functional theory (DFT) calculations corroborate our experimental data and reveal the dependence of charge transfer on layer separation. Our study provides experimental and conceptual foundations for generating p–n nanojunctions in 2D materials.Research at Columbia University was supported as part of the Energy Frontier Research Center on Programmable Quantum Materials funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under Award No DE-SC0019443. Plasmonic nano-imaging at Columbia University was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under Award No DE-SC0018426. J.Z. and A.R. were supported by the European Research Council (ERC-2015-AdG694097), the Cluster of Excellence “Advanced Imaging of Matter” (AIM) EXC 2056-390715994, funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under RTG 2247, Grupos Consolidados (IT1249-19), and SFB925 “Light induced dynamics and control of correlated quantum systems”. J.Z. and A.R. would like to acknowledge Nicolas Tancogne-Dejean and Lede Xian for fruitful discussions and also acknowledge support by the Max Planck Institute-New York City Center for Non-Equilibrium Quantum Phenomena. The Flatiron Institute is a division of the Simons Foundation. J.Z. acknowledges funding received from the European Union Horizon 2020 research and innovation programme under Marie Skłodowska-Curie Grant Agreement 886291 (PeSD-NeSL). STM support was provided by the National Science Foundation via Grant DMR-2004691. C.R.-V. acknowledges funding from the European Union Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie Grant Agreement 844271. D.G.M. acknowledges support from the Gordon and Betty Moore Foundation’s EPiQS Initiative, Grant GBMF9069. J.Q.Y. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. S.E.N. acknowledges support from the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Division of Scientific User Facilities. Work at University of Tennessee was supported by NSF Grant 180896.Peer reviewe