Fabrication and transport properties of graphene-based nanostructures

In this work fabrication and studies of transistor structures based on an atomic sheet of graphite, graphene, are described. Since graphene technology is in its early stages, the development and optimisation of the fabrication process are very important. In this work the impact of various fabrication conditions on the quality of graphene devices is investigated, in particular the effects on the carrier mobility of the details of the mechanical exfoliation procedure, such as environmental conditions and humidity, source of graphite and wafer cleaning procedure. In addition, a comparison is made between the conventional e-beam lithorgaphy and lithography-free fabrication of samples. It was also demonstrated that water and other environmental species play an important role in graphene-to-substrate adhesion and can also contribute to the carrier scattering in graphene. A technique for creating suspended metal gates was developed for the fabrication of graphene p-n-p structures, and charge transport has been studied in such top-gated graphene devices. Depending on the relation between the carrier mean free path and the length of the top-gate we have realized three distinct transport regimes through the p-n-p structure: a) diffusive across the structure; b) ballistic in the regions of p-n junctions but diffusive in the n-region; c) ballistic across the whole p-n-p structure. The second regime has revealed the chiral nature of carriers in graphene. This was demonstrated by comparing the experimental resistance of a single p-n junction with results of electrostatic modeling in the diffusive model. In the third regime we have observed oscillations of the device resistance as a function of carrier concentration in the n-region, which are also dependent on magnetic field. These oscillations have been demonstrated to be a direct consequence of a Fabri-Perot-like interference effect in the graphene p-n-p structures.ORSAS award schem

Optical second harmonic generation in encapsulated single-layer InSe

We report the observation of optical second harmonic generation (SHG) in single-layer indium selenide (InSe). We measure a second harmonic signal of $>10^3$ $\textrm{cts/s}$ under nonresonant excitation using a home-built confocal microscope and a standard pulsed pico-second laser. We demonstrate that polarization-resolved SHG serves as a fast, non-invasive tool to determine the crystal axes in single-layer InSe and to relate the sharp edges of the flake to the armchair and zigzag edges of the crystal structure. Our experiment determines these angles to an accuracy better than $\pm$ $0.2^{\circ}$. Treating the two-dimensional material as a nonlinear polarizable sheet, we determine a second-order nonlinear sheet polarizability $| \chi_{\textrm{sheet}}^{(2)}|=(17.9 \pm 11.0)\times 10^{-20}$ $\textrm{m}^2 \textrm{V}^{-1}$ for single-layer InSe, corresponding to an effective nonlinear susceptibility value of $| \chi_\textrm{eff}^{(2)}| \approx (223 \pm 138) \times 10^{-12}$ $\textrm{m} \textrm{V}^{-1}$ accounting for the sheet thickness ($\textrm{d} \approx 0.8$ $\textrm{nm}$). We demonstrate that the SHG technique can also be applied to encapsulated samples to probe their crystal orientations. The method is therefore suitable for creating high quality van der Waals heterostructures with control over the crystal directions

Electrostatically confined monolayer graphene quantum dots with orbital and valley splittings

The electrostatic confinement of massless charge carriers is hampered by Klein tunneling. Circumventing this problem in graphene mainly relies on carving out nanostructures or applying electric displacement fields to open a band gap in bilayer graphene. So far, these approaches suffer from edge disorder or insufficiently controlled localization of electrons. Here we realize an alternative strategy in monolayer graphene, by combining a homogeneous magnetic field and electrostatic confinement. Using the tip of a scanning tunneling microscope, we induce a confining potential in the Landau gaps of bulk graphene without the need for physical edges. Gating the localized states towards the Fermi energy leads to regular charging sequences with more than 40 Coulomb peaks exhibiting typical addition energies of 7-20 meV. Orbital splittings of 4-10 meV and a valley splitting of about 3 meV for the first orbital state can be deduced. These experimental observations are quantitatively reproduced by tight binding calculations, which include the interactions of the graphene with the aligned hexagonal boron nitride substrate. The demonstrated confinement approach appears suitable to create quantum dots with well-defined wave function properties beyond the reach of traditional techniques

Unusual suppression of the superconducting energy gap and critical temperature in atomically thin NbSe2

It is well known that superconductivity in thin films is generally suppressed with decreasing thickness. This suppression is normally governed by either disorder-induced localization of Cooper pairs, weakening of Coulomb screening, or generation and unbinding of vortex-antivortex pairs as described by the Berezinskii-Kosterlitz-Thouless (BKT) theory. Defying general expectations, few-layer NbSe2 - an archetypal example of ultrathin superconductors - has been found to remain superconducting down to monolayer thickness. Here we report measurements of both the superconducting energy gap and critical temperature in high-quality monocrystals of few-layer NbSe2, using planar-junction tunneling spectroscopy and lateral transport. We observe a fully developed gap that rapidly reduces for devices with the number of layers N < 5, as does their ctitical temperature. We show that the observed reduction cannot be explained by disorder, and the BKT mechanism is also excluded by measuring its transition temperature that for all N remains very close to Tc. We attribute the observed behavior to changes in the electronic band structure predicted for mono- and bi- layer NbSe2 combined with inevitable suppression of the Cooper pair density at the superconductor-vacuum interface. Our experimental results for N > 2 are in good agreement with the dependences of the gap and Tc expected in the latter case while the effect of band-structure reconstruction is evidenced by a stronger suppression of the gap and the disappearance of its anisotropy for N = 2. The spatial scale involved in the surface suppression of the density of states is only a few angstroms but cannot be ignored for atomically thin superconductors.Comment: 21 pages, including supporting informatio

Vertical Field Effect Transistor based on Graphene-WS2 Heterostructures for flexible and transparent electronics

The celebrated electronic properties of graphene have opened way for materials just one-atom-thick to be used in the post-silicon electronic era. An important milestone was the creation of heterostructures based on graphene and other two-dimensional (2D) crystals, which can be assembled in 3D stacks with atomic layer precision. These layered structures have already led to a range of fascinating physical phenomena, and also have been used in demonstrating a prototype field effect tunnelling transistor - a candidate for post-CMOS technology. The range of possible materials which could be incorporated into such stacks is very large. Indeed, there are many other materials where layers are linked by weak van der Waals forces, which can be exfoliated and combined together to create novel highly-tailored heterostructures. Here we describe a new generation of field effect vertical tunnelling transistors where 2D tungsten disulphide serves as an atomically thin barrier between two layers of either mechanically exfoliated or CVD-grown graphene. Our devices have unprecedented current modulation exceeding one million at room temperature and can also operate on transparent and flexible substrates

Water Induced Ferroelectric Switching: The Crucial Role of Collective Dynamics

The interaction mechanisms of water with nanoscale geometries remain poorly understood. This study focuses on behaviour of water clusters under varying external electric fields with a particular focus on molecular ferroelectric devices. We employ a two-fold approach, combining experiments with large-scale molecular dynamics simulations on graphene nanoribbon field effect transistors. We show that bilayer graphene nanoribbons provide stable anchoring of water clusters on the oxygenated edges, resulting in a ferroelectric effect. A molecular dynamics model is then used to investigate water cluster behaviour under varying external electric fields. Finally, we show that these nanoribbons exhibit significant and persistent remanent fields that can be employed in ferroelectric heterostructures and neuromorphic circuits

In Situ TEM Imaging of Solution‐Phase Chemical Reactions Using 2D‐Heterostructure Mixing Cells

From Wiley via Jisc Publications RouterHistory: received 2021-01-26, rev-recd 2021-03-31, pub-electronic 2021-06-09Article version: VoRPublication status: PublishedFunder: Engineering and Physical Sciences Research Council (UK) EPSRC; Grant(s): EP/M010619/1, EP/S021531/1, EP/P009050/1Funder: European Commission H2020 ERC Starter grant EvoluTEM; Grant(s): 715502Funder: Henry Royce Institute for Advanced MaterialsFunder: EPSRC; Id: http://dx.doi.org/10.13039/501100000266; Grant(s): EP/R00661X/1, EP/S019367/1, EP/P025021/1, EP/P025498/1Funder: Royal Society FellowshipAbstract: Liquid‐phase transmission electron microscopy is used to study a wide range of chemical processes, where its unique combination of spatial and temporal resolution provides countless insights into nanoscale reaction dynamics. However, achieving sub‐nanometer resolution has proved difficult due to limitations in the current liquid cell designs. Here, a novel experimental platform for in situ mixing using a specially developed 2D heterostructure‐based liquid cell is presented. The technique facilitates in situ atomic resolution imaging and elemental analysis, with mixing achieved within the immediate viewing area via controllable nanofracture of an atomically thin separation membrane. This novel technique is used to investigate the time evolution of calcium carbonate synthesis, from the earliest stages of nanodroplet precursors to crystalline calcite in a single experiment. The observations provide the first direct visual confirmation of the recently developed liquid‐liquid phase separation theory, while the technological advancements open an avenue for many other studies of early stage solution‐phase reactions of great interest for both the exploration of fundamental science and developing applications