Publications

The chemical stability of graphene and other free-standing two-dimensional crystals means that they can be stacked in different combinations to produce a new class of functional materials, designed for specific device applications. Here we report resonant tunnelling of Dirac fermions through a boron nitride barrier, a few atomic layers thick, sandwiched between two graphene electrodes. The resonant peak in the device characteristics occurs when the electronic spectra of the two electrodes are aligned. The resulting negative differential conductance persists up to room temperature and is gate voltage-tuneable due to graphene's unique Dirac-like spectrum. Whereas conventional resonant tunnelling devices comprising a quantum well sandwiched between two tunnel barriers are tens of nanometres thick, the tunnelling carriers in our devices cross only a few atomic layers, offering the prospect of ultra-fast transit times. This feature, combined with the multi-valued form of the device characteristics, has potential for applications in high-frequency and logic devices.

Abstract The Mermin-Wagner theorem~\cite{Mermin1966} states that long-range {magnetic} order does not exist in one- or two-dimensional (2D) isotropic magnets with short-ranged interactions. The theorem has been a milestone on magnetism and has been driving the research of recently discovered 2D van der waals (vdW) magnetic materials\cite{gong_discovery_2017,firstCrI3} from fundamentals up to potential applications\cite{Genome22}. In such systems, the existence of magnetic ordering is typically attributed to the presence of a significant magnetic anisotropy, which is known to introduce a spin-wave gap and circumvent the core assumption of the theorem\cite{Bogolyubov,Mermin1966,Hohenberg}. Here we show that in finite-size 2D vdW magnets typically found in lab setups ({\it e.g.,} within millimetres), short-range interactions can be large enough to allow the stabilisation of magnetic order at finite temperatures without any magnetic anisotropy for practical implementations. We demonstrate that magnetic ordering can be created in flakes of 2D materials despite of the lattice symmetry due to the intrinsic nature of the spin exchange interactions and finite-size effects in two-dimensions. Surprisingly we find that the crossover temperature, where the intrinsic magnetisation changes from superparamagnetic to a completely disordered paramagnetic regime, is weakly dependent on the system length requiring giant sizes ({\it e.g.,} of the order of the observable universe $\sim$10$^{26}$ m) to be reconcilable with the Mermin-Wagner theorem for zero magnetic ordering at finite temperatures. Our findings indicate exchange interactions as the main driving force behind the stabilisation of short-range order in 2D magnetism and broaden the horizons of possibilities for exploration of compounds with low anisotropy at an atomically thin level.

Quantum dots of around 20 nm in size are fabricated using local anodic oxidation. The behavior of the smallest dots in a magnetic field (see image) allows the identification of the charge-neutrality point and distinguishing of the states with one electron, no charge, and one hole left inside the quantum dot.

A micro apparatus for electrochemical studies on individual high quality graphene flakes is presented. A microinjection-micromanipulator system has been employed to deposit droplets of aqueous solutions containing redox-active species directly on selected micro-scale areas of mechanically exfoliated graphene layers on polymer coated silicon wafers. This approach allows the clear distinction between the electrochemical activity of pristine basal planes and the edges (defects) or steps to be measured. Voltammetric measurements were performed in a two-electrode configuration, and the standard heterogeneous electron transfer rate (k°) for reduction of hexachloroiridate (IrCl62−) was estimated. The kinetics of electron transfer were evaluated for several types of graphene: mono, bi, and few layer basal planes, and the k° was estimated for an edge/step between two few layer graphene flakes. As a comparison, the kinetic behaviour of graphite basal planes was measured for the deposited aqueous droplets. The appearance of ruptures on the graphene monolayer was observed after deposition of the aqueous solution for the case of graphene on a bare silicon/silicon oxide substrate.

Topological materials may exhibit Hall-like currents flowing transversely to the applied electric field even in the absence of a magnetic field. In graphene superlattices, which have broken inversion symmetry, topological currents originating from graphene's two valleys are predicted to flow in opposite directions and combine to produce long-range charge neutral flow. We observed this effect as a nonlocal voltage at zero magnetic field in a narrow energy range near Dirac points at distances as large as several micrometers away from the nominal current path. Locally, topological currents are comparable in strength with the applied current, indicating large valley-Hall angles. The long-range character of topological currents and their transistor-like control by means of gate voltage can be exploited for information processing based on valley degrees of freedom.

Formation, evolution and vanishing of bubbles are common phenomena in nature, which can be easily observed in boiling or falling water, carbonated drinks, gas-forming electrochemical reactions and so on. However, the morphology and the growth dynamics of the bubbles at nanoscale have not been fully investigated owing to the lack of proper imaging tools that can visualize nanoscale objects in the liquid phase. Here, we demonstrate for the first time that the nanobubbles in water encapsulated by graphene membrane can be visualized by in-situ ultra-high vacuum transmission electron microscopy. Our microscopic results indicate two distinct growth mechanisms of merging nanobubbles and the existence of a critical radius of nanobubbles that determines the unusually long stability of nanobubbles. Interestingly, the gas transport through ultrathin water membranes at nanobubble interface is free from dissolution, which is clearly different from conventional gas transport that includes condensation, transmission and evaporation.

We present infrared spectra 0.1–1 eV of electrostatically gated bilayer graphene as a function of doping and compare it with tight-binding calculations. All major spectral features corresponding to the expected interband transitions are identified in the spectra: a strong peak due to transitions between parallel split-off bands and two onset-like features due to transitions between valence and conduction bands. A strong gate voltage dependence of these structures and a significant electron-hole asymmetry are observed that we use to extract several band parameters. The structures related to the gate-induced band gap are less pronounced in the experiment than predicted by the tight-binding model that uses parameters obtained from previous experiments on graphite and recent self-consistent band-gap calculations.

Abstract Graphene has received much attention due to its monoatomic, unique two-dimensional structure, which results in remarkable mechanical, physical, and electrical properties. However, synthesizing high-quality graphene-based composites with high conductivity and ionic mobility remains challenging. Here, we report an allotrope to the nanocarbon family, Graphene-P-phenyl-Graphene, synthesized by inserting π-π-conjugated p-phenyls between graphene layers and connecting them via C–C σ bonds. Graphene-P-phenyl-Graphene is thermally and dynamically stable, as verified by density functional theory and molecular dynamics, and can be produced at kilogram scale. The p-phenyl bridges swell the layer spacing from ~0.34 to ~0.56 nm, reducing van der Waals forces and enhancing electron delocalization. Electrons in these separated graphene layers benefit from low mass and efficient 3D screening of charge scattering, resulting in high Hall mobility (10,000–13,000 cm² V⁻¹ s⁻¹) in freestanding films. The expanded spacing also enables decoupling of layer electrons and rapid ion storage and transport—even for large ions. For example, potassium-ion batteries using Graphene-P-phenyl-Graphene exhibit high reversible capacity, long-term stability, and high charge-discharge rates. Graphene-P-phenyl-Graphene holds promise for large-scale, portable, high-performance electronics with energy storage capabilities.

We propose programed potential modulation strategies to balance the ion intercalation/deintercalation, surface tailoring and bubbling dispersion processes in the electrochemical exfoliation of graphite, resulting in high-quality graphene with high crystallinity, low oxidation degree, uniform size distribution and few layers.

We present the first Raman spectroscopic study of Bernal bilayer graphene flakes under uniaxial tension. Apart from a purely mechanical behavior in flake regions where both layers are strained evenly, certain effects stem from inhomogeneous stress distribution across the layers. These phenomena such as the removal of inversion symmetry in bilayer graphene may have important implications in the band gap engineering, providing an alternative route to induce the formation of a band gap.

No abstract is provided for this article.

Free-space circularly polarized light (CPL) detection, requiring polarizers and waveplates, has been well established, while such spatial degree of freedom is unfortunately absent in integrated on-chip optoelectronics. So far, those reported filterless CPL photodetectors suffer from the intrinsic small discrimination ratio, vulnerability to the non-CPL field components, and low responsivity. Here, we report a distinct paradigm of geometric photodetectors in mid-infrared exhibiting colossal discrimination ratio, close-to-perfect CPL-specific response, a zero-bias responsivity of 392 V/W at room temperature, and a detectivity of ellipticity down to 0.03$^o$ Hz$^{-1/2}$. Our approach employs plasmonic nanostructures array with judiciously designed symmetry, assisted by graphene ribbons to electrically read their near-field optical information. This geometry-empowered recipe for infrared photodetectors provides a robust, direct, strict, and high-quality solution to on-chip filterless CPL detection and unlocks new opportunities for integrated functional optoelectronic devices.

The temperature dependence of the mobility in suspended graphene samples is investigated. In clean samples, flexural phonons become the leading scattering mechanism at temperature $T \gtrsim 10\,\,$K, and the resistivity increases quadratically with $T$. Flexural phonons limit the intrinsic mobility down to a few $\text{m}^2/\text{Vs}$ at room $T$. Their effect can be eliminated by applying strain or placing graphene on a substrate.