arXiv subjects

Joshua A. Robinson

Publications and source records attributed to Joshua A. Robinson.

At least 55 records · Page 3Linked to original sources

arXiv2020

Photo-physics and electronic structure of lateral graphene/MoS2 and metal/MoS2 junctions

Integration of semiconducting transition metal dichalcogenides (TMDs) into functional optoelectronic circuitries requires an understanding of the charge transfer across the interface between the TMD and the contacting material. Here, we use spatially resolved photocurrent microscopy to demonstrate electronic uniformity at the epitaxial graphene/molybdenum disulfide (EG/MoS2) interface. A 10x larger photocurrent is extracted at the EG/MoS2 interface when compared to metal (Ti/Au) /MoS2 interface. This is supported by semi-local density-functional theory (DFT), which predicts the Schottky barrier at the EG/MoS2 interface to be ~2x lower than Ti/MoS2. We provide a direct visualization of a 2D material Schottky barrier through combination of angle resolved photoemission spectroscopy with spatial resolution selected to be ~300 nm (nano-ARPES) and DFT calculations. A bending of ~500 meV over a length scale of ~2-3 micrometer in the valence band maximum of MoS2 is observed via nano-ARPES. We explicate a correlation between experimental demonstration and theoretical predictions of barriers at graphene/TMD interfaces. Spatially resolved photocurrent mapping allows for directly visualizing the uniformity of built-in electric fields at heterostructure interfaces, providing a guide for microscopic engineering of charge transport across heterointerfaces. This simple probe-based technique also speaks directly to the 2D synthesis community to elucidate electronic uniformity at domain boundaries alongside morphological uniformity over large areas.

physics.app-ph↗

arXiv2020

Flatbands and Mechanical Deformation Effects in the Moiré Superlattice of MoS$_2$-WSe$_2$ Heterobilayers

It has recently been shown that quantum-confined states can appear in epitaxially grown van der Waals material heterobilayers without a rotational misalignment ($θ=0^\circ$), associated with flat bands in the Brillouin zone of the moiré pattern formed due to the lattice mismatch of the two layers. Peaks in the local density of states and confinement in a MoS$_2$/WSe$_2$ system was qualitatively described only considering local stacking arrangements, which cause band edge energies to vary spatially. In this work, we report the presence of large in-plane strain variation across the moiré unit cell of a $θ=0^\circ$ MoS$_2$/WSe$_2$ heterobilayer, and show that inclusion of strain variation and out-of-plane displacement in density functional theory calculations greatly improves their agreement with the experimental data. We further explore the role of twist-angle by showing experimental data for a twisted MoS$_2$/WSe$_2$ heterobilayer structure with twist angle of $θ=15^\circ$, that exhibits a moiré pattern but no confinement.

cond-mat.mtrl-sci↗

arXiv2019

An Air-Stable and Atomically Thin Graphene/Gallium Superconducting Heterostructure

Two-dimensional layered and atomically thin elemental superconductors may be key ingredients in next-generation quantum technologies, if they can be stabilized and integrated into heterostructured devices under ambient conditions. However, atomically thin elemental superconductors are largely unexplored outside ultra-high vacuum due to rapid oxidation, and even 2D layered superconductors require complex encapsulation strategies to maintain material quality. Here we demonstrate environmentally stable, single-crystal, few-atom-thick superconducting gallium, 2D-Ga, produced by confinement heteroepitaxy (CHet) at the interface of epitaxial graphene (EG) and silicon carbide (SiC). 2D-Ga becomes superconducting at 4 K; this elevation over bulk alpha-Ga (Tc~1 K) is primarily attributed to an increased density of states at the Fermi level as the incipient Ga-Ga dimerization seen in alpha-Ga is suppressed by epitaxy to SiC. We also demonstrate the importance of controlling SiC surface morphology (i.e. step height) and defect-engineering in graphene layers prior to intercalation to achieve large-area uniform 2D-Ga layers with isotropic transport properties. This work demonstrates that unique 2D forms of 3D materials can be stabilized at the EG/SiC interface, which represents a scalable route towards air-stable crystalline 2D superconductors as a potential foundation for next-generation quantum technologies.

cond-mat.supr-con↗

arXiv2019

Epitaxial Graphene Intercalation: A Route to Graphene Modulation and Unique 2D Materials

Intercalation of atomic species through epitaxial graphene layers began only a few years following its initial report in 2004. The impact of intercalation on the electronic properties of the graphene is well known; however, the intercalant itself can also exhibit intriguing properties not found in nature. This suggests that a shift in the focus of epitaxial graphene intercalation studies may lead to fruitful exploration of many new forms of traditionally 3D materials. In the following forward-looking review, we summarize the primary techniques used to achieve and characterize EG intercalation, and introduce a new, facile approach to readily achieve metal intercalation at the graphene/silicon carbide interface. We show that simple thermal evaporation-based methods can effectively replace complicated synthesis techniques to realize large-scale intercalation of non-refractory metals. We also show that these methods can be extended to the formation of compound materials based on intercalation. Two-dimensional (2D) silver (2D-Ag) and large-scale 2D gallium nitride (2D-GaNx) are used to demonstrate these approaches.

cond-mat.mtrl-sci↗

arXiv2019

Contactless photo-induced carrier density control in nanocrystal MoS2 hybrids

The ultrathin nature of two-dimensional monolayer semiconductors yields optoelectronic properties which are highly responsive to changes in free-carrier density, making it imperative to masterfully control their doping levels. We report a new photo-doping scheme that quasi-permanently dopes the monolayer MoS2 to extents competing with electrostatic gating. The photo-doping is achieved by coupling monolayer MoS2 with indium tin oxide nanocrystals that can store multiple electrons per nanocrystal after UV illumination. In the hybrid structure, the photo-generated valence band holes in the nanocrystals are filled by MoS2 electrons, photo-doping the MoS2 with holes. Reductions in carrier density by ~6x10^12 cm^-2 are observed, equivalent to the storage of ~40 electrons per nanocrystal. Long-range changes proliferating up to 40 micrometers away from the localized photodoping result from local bandstructure variations in MoS2. These studies reveal novel all-optical carrier density control in monolayer semiconductors, enabling remote-control of local charge density and innovative energy storage technologies.

cond-mat.mes-hall↗

arXiv2018

Considerations for utilizing sodium chloride in epitaxial molybdenum disulfide

The utilization of alkali salts, such as NaCl and KI, have enabled the successful growth of large single domain and fully coalesced polycrystalline two-dimensional (2D) transition metal dichalcogenide layers. However, the impact of alkali salts on photonic and electronic properties are not fully established. In this work, we report alkali-free epitaxy of MoS2 on sapphire and benchmark the properties against alkali-assisted growth of MoS2. This study demonstrates that although NaCl can dramatically increase the domain size of monolayer MoS2 by 20 times, it can also induce strong optical and electronic heterogeneities in as-grown large-scale films. This work elucidates that utilization of NaCl can lead to variation in growth rates, loss of epitaxy, and a high density of nanoscale MoS2 particles (4/μm2). Such phenomena suggest that alkali atoms play an important role in Mo and S adatom mobility and strongly influence the 2D/sapphire interface during growth. Compared to alkali-free synthesis under the same growth conditions, MoS2 growth assisted by NaCl results in >1% tensile strain in as-grown domains, which reduces photoluminescence by ~20x and degrades transistor performance.

cond-mat.mtrl-sci↗

arXiv2018

Dynamics of liquid crystal on hexagonal lattice

Nematic liquid crystal (LC) molecules adsorbed on two dimensional materials are aligned along the crystal directions of the hexagonal lattice. It was demonstrated that short electric pulses can reorient the aligned LC molecules in the preferred armchair direction of hexagonal boron nitride (h-BN). Several states with a variety of colors were obtained by changing the direction and strength of the electric pulses. The ab initio calculations based on density functional theory was carried out to determine the favorable adsorption configurations of the LC molecules on the h-BN surface. A non-volatile display, in which pixel resolution can be determined by grains of hexagonal surface, is proposed, which can offer a pathway towards dynamic high-quality pixels with low power consumption, and could define a new paradigm for all non-volatile display applications.

cond-mat.soft↗

arXiv2018

Unique excitonic effects in tungsten disulphide monolayers on two-layer graphene

Light emission in atomically thin heterostructures is known to depend on the type of materials, number and stacking sequence of the constituent layers. Here we show that the thickness of a two-dimensional substrate can be crucial in modulating the light emission. We study the layer-dependent charge transfer in vertical heterostructures built from monolayer tungsten disulphide (WS2) on one- and two-layer epitaxial graphene, unravelling the effect that the interlayer electronic coupling has on the excitonic properties of such heterostructures. We bring evidence that the excitonic properties of WS2 can be effectively tuned by the number of supporting graphene layers. Integrating WS2 monolayers with two-layer graphene leads to a significant enhancement of the photoluminescence response, up to one order of magnitude higher compared to WS2 supported on one-layer graphene. Our findings highlight the importance of substrate engineering when constructing atomically thin layered heterostructures.

cond-mat.mtrl-sci↗

arXiv2018

Quantum-Confined Electronic States arising from Moiré Pattern of MoS2-WSe2 Hetero-bilayers

A two-dimensional (2D) hetero-bilayer system consisting of MoS2 on WSe2, deposited on epitaxial graphene, is studied by scanning tunneling microscopy and spectroscopy at temperatures of 5 and 80 K. A moiré pattern is observed, arising from lattice mismatch of 3.7% between the MoS2 and WSe2. Significant energy shifts are observed in tunneling spectra observed at the maxima of the moiré corrugation, as compared with spectra obtained at corrugation minima, consistent with prior work. Furthermore, at the minima of the moiré corrugation, sharp peaks in the spectra at energies near the band edges are observed, for spectra acquired at 5 K. The peaks correspond to discrete states that are confined within the moiré unit cells. Conductance mapping is employed to reveal the detailed structure of the wave functions of the states. For measurements at 80 K, the sharp peaks in the spectra are absent, and conductance maps of the band edges reveal little structure.

cond-mat.mes-hall↗

arXiv2016

Magnetic brightening and control of dark excitons in monolayer WSe2

Monolayer transition metal dichalcogenide (TMDC) crystals, as direct-gap materials with unusually strong light-matter interaction, have attracted much recent attention. In contrast to the initial understanding, the minima of the conduction band are predicted to be spin split. Because of this splitting and the spin-polarized character of the valence bands, the lowest-lying excitonic states in WX2 (X=S, Se) are expected to be spin-forbidden and optically dark. To date, however, there has been no direct experimental probe of these dark band-edge excitons, which strongly influence the light emission properties of the material. Here we show how an in-plane magnetic field can brighten the dark excitonic states and allow their properties to be revealed experimentally in monolayer WSe2. In particular, precise energy levels for both the neutral and charged dark excitons were obtained and compared with ab-initio calculations using the GW-BSE approach. Greatly increased emission and valley lifetimes were observed for the brightened dark states as a result of their spin configuration. These studies directly probe the excitonic spin manifold and provide a new route to tune the optical and valley properties of these prototypical two-dimensional semiconductors.

cond-mat.mes-hall↗

arXiv2016

Thickness characterization of atomically-thin WSe$_2$ on epitaxial graphene by low-energy electron reflectivity oscillations

In this work, low-energy electron microscopy is employed to probe structural as well as electronic information in few-layer WSe$_2$ on epitaxial graphene on SiC. The emergence of unoccupied states in the WSe$_2$--graphene heterostructures are studied using spectroscopic low-energy electron reflectivity. Reflectivity minima corresponding to specific WSe$_2$ states that are localized between the monolayers of each vertical heterostructure are shown to reveal the number of layers for each point on the surface. A theory for the origin of these states is developed and utilized to explain the experimentally observed featured in the WSe$_2$ electron reflectivity.

cond-mat.mes-hall↗

arXiv2016

Zone-center phonons of bulk, few-layer, and monolayer 1T-TaS$_2$: Detection of the commensurate charge density wave phase through Raman scattering

We present first-principles calculations of the vibrational properties of the transition metal dichalcogenide 1T-TaS$_2$ for various thicknesses in the high-temperature (undistorted) phase and the low-temperature commensurate charge density wave (CDW) phase. We also present measurements of the Raman spectra for bulk, few-layer, and monolayer samples at temperatures well below that of the bulk transition to the commensurate phase. Through our calculations, we identify the low-frequency folded-back acoustic modes as a convenient signature of the commensurate CDW wave structure in vibrational spectra. In our measured Raman spectra, this signature is clearly evident in all of the samples, indicating that the commensurate phase remains the ground state as the material is thinned, even down to a single layer. This is in contrast to some previous studies which suggest a suppression of the commensurate CDW transition in thin flakes. We also use polarized Raman spectroscopy to probe c-axis orbital texture in the low-T phase, which has recently been suggested as playing a role in the metal-insulator transition that accompanies the structural transition to the commensurate CDW phase.

cond-mat.mtrl-sci↗

arXiv2016

Graphene stabilization of two-dimensional gallium nitride

The spectrum of two-dimensional (2D) materials beyond graphene offers a remarkable platform to study new phenomena in condensed matter physics. Among these materials, layered hexagonal boron nitride (hBN), with its wide bandgap energy (~5.0-6.0 eV), has clearly established that 2D nitrides are key to advancing novel devices1. A gap, however, remains between the theoretical prediction of 2D nitrides beyond hBN and experimental realization of such structures. Here we demonstrate the synthesis of 2D gallium nitride (GaN) via a novel migration-enhanced encapsulated growth (MEEG) technique utilizing epitaxial graphene. We theoretically predict and experimentally validate that the atomic structure of 2D GaN grown via MEEG is notably different from reported theory. Moreover, we establish that graphene plays a critical role in stabilizing the direct-bandgap (nearly 5.0 eV), 2D buckled structure. Our results provide a foundation for discovery and stabilization of novel 2D nitrides that are difficult to prepare via traditional synthesis.

cond-mat.mtrl-sci↗

arXiv2016

Formation of hexagonal Boron Nitride on Graphene-covered Copper Surfaces

Graphene-covered copper surfaces have been exposed to borazine, (BH)3(NH)3, with the resulting surfaces characterized by low-energy electron microscopy. Although the intent of the experiment was to form hexagonal boron nitride (h-BN) on top of the graphene, such layers were not obtained. Rather, in isolated surface areas, h-BN is found to form micrometer-size islands that substitute for the graphene. Additionally, over nearly the entire surface, the properties of the layer that was originally graphene is observed to change in a manner that is consistent with the formation of a mixed h-BN/graphene alloy, i.e. h-BNC alloy. Furthermore, following the deposition of the borazine, a small fraction of the surface is found to consist of bare copper, indicating etching of the overlying graphene. The inability to form h-BN layers on top of graphene is discussed in terms of the catalytic behavior of the underlying copper surface and the decomposition of the borazine on top of the graphene.

cond-mat.mtrl-sci↗

arXiv2015

Atomically Thin Resonant Tunnel Diodes built from Synthetic van der Waals Heterostructures

Vertical integration of two-dimensional van der Waals materials is predicted to lead to novel electronic and optical properties not found in the constituent layers. Here, we present the direct synthesis of two unique, atomically thin, multi-junction heterostructures by combining graphene with the monolayer transition-metal dichalocogenides: MoS2, MoSe2, and WSe2.The realization of MoS2-WSe2-Graphene and WSe2-MoSe2-Graphene heterostructures leads toresonant tunneling in an atomically thin stack with spectrally narrow room temperature negative differential resistance characteristics.

cond-mat.mtrl-sci↗

arXiv2013

Graphene Nanoribbon Field-Effect Transistors on Wafer-Scale Epitaxial Graphene on SiC substrates

We report the realization of top-gated graphene nanoribbon field effect transistors (GNRFETs) of ~10 nm width on large-area epitaxial graphene exhibiting the opening of a band gap of ~0.14 eV. Contrary to prior observations of disordered transport and severe edge-roughness effects of GNRs, the experimental results presented here clearly show that the transport mechanism in carefully fabricated GNRFETs is conventional band-transport at room temperature, and inter-band tunneling at low temperature. The entire space of temperature, size, and geometry dependent transport properties and electrostatics of the GNRFETs are explained by a conventional thermionic emission and tunneling current model. Our combined experimental and modeling work proves that carefully fabricated narrow GNRs behave as conventional semiconductors, and remain potential candidates for electronic switching devices.

cond-mat.mes-hall↗

arXiv2013

Prospects of Direct Growth Boron Nitride Films as Substrates for Graphene Electronics

We present a route for direct growth of boron nitride via a polyborazylene to h-BN conversion process. This two-step growth process ultimately leads to a >25x reduction in the RMS surface roughness of h-BN films when compared to a high temperature growth on Al2O3(0001) and Si(111) substrates. Additionally, the stoichiometry is shown to be highly dependent on the initial polyborazylene deposition temperature. Importantly, CVD graphene transferred to direct-grown boron nitride films on Al2O3 at 400°C results in a >1.5x and >2.5x improvement in mobility compared to CVD graphene transferred to Al2O3 and SiO2 substrates, respectively, which is attributed to the combined reduction of remote charged impurity scattering and surface roughness scattering. Simulation of mobility versus carrier concentration confirms the importance of limiting the introduction of charged impurities in the h-BN film and highlights the importance of these results in producing optimized h-BN substrates for high performance graphene and TMD devices.

cond-mat.mtrl-sci↗

arXiv2011

Technology ready use of single layer graphene as a transparent electrode for hybrid photovoltaic devices

Graphene has been used recently as a replacement for indium tin oxide (ITO) for the transparent electrode of an organic photovoltaic device. Due to its limited supply, ITO is considered as a limiting factor for the commercialization of organic solar cells. We explored the use of large-area graphene grown on copper by chemical vapor deposition (CVD) and then transferred to a glass substrate as an alternative transparent electrode. The transferred film was shown by scanning Raman spectroscopy measurements to consist of >90% single layer graphene. Optical spectroscopy measurements showed that the layer-transferred graphene has an optical absorbance of 1.23% at a wavelength of 532 nm. We fabricated organic hybrid solar cells utilizing this material as an electrode and compared their performance with ITO devices fabricated using the same procedure. We demonstrated power conversion efficiency up to 3.98%, higher than that of the ITO device (3.86%), showing that layer-transferred graphene promises to be a high quality, low-cost, flexible material for transparent electrodes in solar cell technology.

cond-mat.mtrl-sci↗