Unraveling Heat Transport and Dissipation in Suspended MoSe2 from Bulk to Monolayer.

Understanding heat flow in layered transition metal dichalcogenide (TMD) crystals is crucial for applications exploiting these materials. Despite significant efforts, several basic thermal transport properties of TMDs are currently not well understood, in particular how transport is affected by material thickness and the material's environment. This combined experimental-theoretical study establishes a unifying physical picture of the intrinsic lattice thermal conductivity of the representative TMD MoSe2 . Thermal conductivity measurements using Raman thermometry on a large set of clean, crystalline, suspended crystals with systematically varied thickness are combined with ab initio simulations with phonons at finite temperature. The results show that phonon dispersions and lifetimes change strongly with thickness, yet the thinnest TMD films exhibit an in-plane thermal conductivity that is only marginally smaller than that of bulk crystals. This is the result of compensating phonon contributions, in particular heat-carrying modes around ≈0.1 THz in (sub)nanometer thin films, with a surprisingly long mean free path of several micrometers. This behavior arises directly from the layered nature of the material. Furthermore, out-of-plane heat dissipation to air molecules is remarkably efficient, in particular for the thinnest crystals, increasing the apparent thermal conductivity of monolayer MoSe2 by an order of magnitude. These results are crucial for the design of (flexible) TMD-based (opto-)electronic applications.

Hot-Carrier Cooling in High-Quality Graphene Is Intrinsically Limited by Optical Phonons.

Many promising optoelectronic devices, such as broadband photodetectors, nonlinear frequency converters, and building blocks for data communication systems, exploit photoexcited charge carriers in graphene. For these systems, it is essential to understand the relaxation dynamics after photoexcitation. These dynamics contain a sub-100 fs thermalization phase, which occurs through carrier-carrier scattering and leads to a carrier distribution with an elevated temperature. This is followed by a picosecond cooling phase, where different phonon systems play a role: graphene acoustic and optical phonons, and substrate phonons. Here, we address the cooling pathway of two technologically relevant systems, both consisting of high-quality graphene with a mobility >10 000 cm2 V-1 s-1 and environments that do not efficiently take up electronic heat from graphene: WSe2-encapsulated graphene and suspended graphene. We study the cooling dynamics using ultrafast pump-probe spectroscopy at room temperature. Cooling via disorder-assisted acoustic phonon scattering and out-of-plane heat transfer to substrate phonons is relatively inefficient in these systems, suggesting a cooling time of tens of picoseconds. However, we observe much faster cooling, on a time scale of a few picoseconds. We attribute this to an intrinsic cooling mechanism, where carriers in the high-energy tail of the hot-carrier distribution emit optical phonons. This creates a permanent heat sink, as carriers efficiently rethermalize. We develop a macroscopic model that explains the observed dynamics, where cooling is eventually limited by optical-to-acoustic phonon coupling. These fundamental insights will guide the development of graphene-based optoelectronic devices.

Strain-Engineering of Twist-Angle in Graphene/hBN Superlattice Devices.

The observation of novel physical phenomena such as Hofstadter's butterfly, topological currents, and unconventional superconductivity in graphene has been enabled by the replacement of SiO2 with hexagonal boron nitride (hBN) as a substrate and by the ability to form superlattices in graphene/hBN heterostructures. These devices are commonly made by etching the graphene into a Hall-bar shape with metal contacts. The deposition of metal electrodes, the design, and specific configuration of contacts can have profound effects on the electronic properties of the devices possibly even affecting the alignment of graphene/hBN superlattices. In this work, we probe the strain configuration of graphene on hBN in contact with two types of metal contacts, two-dimensional (2D) top-contacts and one-dimensional edge-contacts. We show that top-contacts induce strain in the graphene layer along two opposing leads, leading to a complex strain pattern across the device channel. Edge-contacts, on the contrary, do not show such strain pattern. A finite-elements modeling simulation is used to confirm that the observed strain pattern is generated by the mechanical action of the metal contacts clamped to the graphene. Thermal annealing is shown to reduce the overall doping while increasing the overall strain, indicating an increased interaction between graphene and hBN. Surprisingly, we find that the two contact configurations lead to different twist-angles in graphene/hBN superlattices, which converge to the same value after thermal annealing. This observation confirms the self-locking mechanism of graphene/hBN superlattices also in the presence of strain gradients. Our experiments may have profound implications in the development of future electronic devices based on heterostructures and provide a new mechanism to induce complex strain patterns in 2D materials.

Graphene-Based Light Sensing: Fabrication, Characterisation, Physical Properties and Performance.

Graphene and graphene-based materials exhibit exceptional optical and electrical properties with great promise for novel applications in light detection. However, several challenges prevent the full exploitation of these properties in commercial devices. Such challenges include the limited linear dynamic range (LDR) of graphene-based photodetectors, the lack of efficient generation and extraction of photoexcited charges, the smearing of photoactive junctions due to hot-carriers effects, large-scale fabrication and ultimately the environmental stability of the constituent materials. In order to overcome the aforementioned limits, different approaches to tune the properties of graphene have been explored. A new class of graphene-based devices has emerged where chemical functionalisation, hybridisation with light-sensitising materials and the formation of heterostructures with other 2D materials have led to improved performance, stability or versatility. For example, intercalation of graphene with FeCl 3 is highly stable in ambient conditions and can be used to define photo-active junctions characterized by an unprecedented LDR while graphene oxide (GO) is a very scalable and versatile material which supports the photodetection from UV to THz frequencies. Nanoparticles and quantum dots have been used to enhance the absorption of pristine graphene and to enable high gain thanks to the photogating effect. In the same way, hybrid detectors made from stacked sequences of graphene and layered transition-metal dichalcogenides enabled a class of devices with high gain and responsivity. In this work, we will review the performance and advances in functionalised graphene and hybrid photodetectors, with particular focus on the physical mechanisms governing the photoresponse, the performance and possible future paths of investigation.

Novel circuit design for high-impedance and non-local electrical measurements of two-dimensional materials.

Two-dimensional materials offer a novel platform for the development of future quantum technologies. However, the electrical characterisation of topological insulating states, non-local resistance, and bandgap tuning in atomically thin materials can be strongly affected by spurious signals arising from the measuring electronics. Common-mode voltages, dielectric leakage in the coaxial cables, and the limited input impedance of alternate-current amplifiers can mask the true nature of such high-impedance states. Here, we present an optical isolator circuit which grants access to such states by electrically decoupling the current-injection from the voltage-sensing circuitry. We benchmark our apparatus against two state-of-the-art measurements: the non-local resistance of a graphene Hall bar and the transfer characteristic of a WS2 field-effect transistor. Our system allows the quick characterisation of novel insulating states in two-dimensional materials with potential applications in future quantum technologies.

High-Mobility and High-Optical Quality Atomically Thin WS 2.

The rise of atomically thin materials has the potential to enable a paradigm shift in modern technologies by introducing multi-functional materials in the semiconductor industry. To date the growth of high quality atomically thin semiconductors (e.g. WS2) is one of the most pressing challenges to unleash the potential of these materials and the growth of mono- or bi-layers with high crystal quality is yet to see its full realization. Here, we show that the novel use of molecular precursors in the controlled synthesis of mono- and bi-layer WS2 leads to superior material quality compared to the widely used direct sulfidization of WO3-based precursors. Record high room temperature charge carrier mobility up to 52 cm2/Vs and ultra-sharp photoluminescence linewidth of just 36 meV over submillimeter areas demonstrate that the quality of this material supersedes also that of naturally occurring materials. By exploiting surface diffusion kinetics of W and S species adsorbed onto a substrate, a deterministic layer thickness control has also been achieved promoting the design of scalable synthesis routes.

Fast and Highly Sensitive Ionic-Polymer-Gated WS2 -Graphene Photodetectors.

The combination of graphene with semiconductor materials in heterostructure photodetectors enables amplified detection of femtowatt light signals using micrometer-scale electronic devices. Presently, long-lived charge traps limit the speed of such detectors, and impractical strategies, e.g., the use of large gate-voltage pulses, have been employed to achieve bandwidths suitable for applications such as video-frame-rate imaging. Here, atomically thin graphene-WS2 heterostructure photodetectors encapsulated in an ionic polymer are reported, which are uniquely able to operate at bandwidths up to 1.5 kHz whilst maintaining internal gain as large as 106 . Highly mobile ions and the nanometer-scale Debye length of the ionic polymer are used to screen charge traps and tune the Fermi level of the graphene over an unprecedented range at the interface with WS2 . Responsivity R = 106 A W-1 and detectivity D* = 3.8 × 1011 Jones are observed, approaching that of single-photon counters. The combination of both high responsivity and fast response times makes these photodetectors suitable for video-frame-rate imaging applications.