arXiv subjects

Stiven Forti

Publications and source records attributed to Stiven Forti.

At least 37 records · Page 2Linked to original sources

arXiv2023

Growth and applications of two-dimensional single crystals

Two-dimensional (2D) materials have received extensive research attentions over the past two decades due to their intriguing physical properties (such as the ultrahigh mobility and strong light-matter interaction at atomic thickness) and a broad range of potential applications (especially in the fields of electronics and optoelectronics). The growth of single-crystal 2D materials is the prerequisite to realize 2D-based high-performance applications. In this review, we aim to provide an in-depth analysis of the state-of-the-art technology for the growth and applications of 2D materials, with particular emphasis on single crystals. We first summarize the major growth strategies for monolayer 2D single crystals. Following that, we discuss the growth of multilayer single crystals, including the control of thickness, stacking sequence, and heterostructure composition. Then we highlight the exploration of 2D single crystals in electronic and optoelectronic devices. Finally, a perspective is given to outline the research opportunities and the remaining challenges in this field.

cond-mat.mtrl-sci↗

arXiv2023

Link between interlayer hybridization and ultrafast charge transfer in WS$_2$-graphene heterostructures

Ultrafast charge separation after photoexcitation is a common phenomenon in various van-der-Waals (vdW) heterostructures with great relevance for future applications in light harvesting and detection. Theoretical understanding of this phenomenon converges towards a coherent mechanism through charge transfer states accompanied by energy dissipation into strongly coupled phonons. The detailed microscopic pathways are material specific as they sensitively depend on the band structures of the individual layers, the relative band alignment in the heterostructure, the twist angle between the layers, and interlayer interactions resulting in hybridization. We used time- and angle-resolved photoemission spectroscopy combined with tight binding and density functional theory electronic structure calculations to investigate ultrafast charge separation and recombination in WS$_2$-graphene vdW heterostructures. We identify several avoided crossings in the band structure and discuss their relevance for ultrafast charge transfer. We relate our own observations to existing theoretical models and propose a unified picture for ultrafast charge transfer in vdW heterostructures where band alignment and twist angle emerge as the most important control parameters.

cond-mat.mtrl-sci↗

arXiv2022

Industrial graphene coating of low-voltage copper wires for power distribution

Copper (Cu) is the electrical conductor of choice in many categories of electrical wiring, with household and building installations being the major market of this metal. This work demonstrates the coating of Cu wires - with diameters relevant for low voltage (LV) applications - with graphene. The chemical vapor deposition (CVD) coating process is rapid, safe, scalable and industrially compatible. Graphene-coated Cu wires display oxidation resistance and increased electrical conductivity (up to 1% immediately after coating and up to 3% after 24 months), allowing for wire diameter reduction and thus significant savings in wire production costs. Combined spectroscopic and diffraction analysis indicate that the conductivity increase is due to a change in Cu crystallinity, induced by the coating process conditions, while electrical testing of aged wires shows that graphene plays a major role in maintaining improved electrical performances over long periods of time. Finally, graphene coating of Cu wires using an ambient pressure roll-to-roll (R2R) CVD reactor is demonstrated. This enables the in-line production of graphene-coated metallic wires as required for industrial scale-up.

physics.app-ph↗

arXiv2022

Black Phosphorus n-type doping by Cu: a microscopic surface investigation

We study surface charge transfer doping of exfoliated black phosphorus (bP) flakes by copper using scanning tunneling microscopy (STM) and spectroscopy (STS) at room temperature. The tunneling spectra reveal a gap in correspondence of Cu islands, which is attributed to Coulomb blockade phenomena. Moreover, using line spectroscopic measurements across small copper islands, we exploit the potential of the local investigation, showing that the n-type doping effect of copper on bP is short-ranged. These experimental results are substantiated by first-principles simulations, which quantify the role of cluster size for an effective n-type doping of bP and explain the Coulomb blockade by an electronic decoupling of the topmost bP layer from the underlying layers driven by the copper cluster. Our results provide novel understanding, difficult to retrieve by transport measurements, of the doping of bP by copper, which appears promising for the implementation of ultra-sharp p-n junctions in bP.

cond-mat.mtrl-sci↗

arXiv2021

Ultra-clean high-mobility graphene on technologically relevant substrates

Graphene grown via chemical vapour deposition (CVD) on copper foil has emerged as a high-quality, scalable material, that can be easily integrated on technologically relevant platforms to develop promising applications in the fields of optoelectronics and photonics. Most of these applications require low-contaminated high-mobility graphene (i.e., approaching 10 000 $cm^2 V^{-1} s^{-1}$) at room temperature) to reduce device losses and implement compact device design. To date, these mobility values are only obtained when suspending or encapsulating graphene. Here, we demonstrate a rapid, facile, and scalable cleaning process, that yields high-mobility graphene directly on the most common technologically relevant substrate: silicon dioxide on silicon (SiO$_2$/Si). Atomic force microscopy (AFM) and spatially-resolved X-ray photoelectron spectroscopy (XPS) demonstrate that this approach is instrumental to rapidly eliminate most of the polymeric residues which remain on graphene after transfer and fabrication and that have adverse effects on its electrical properties. Raman measurements show a significant reduction of graphene doping and strain. Transport measurements of 50 Hall bars (HBs) yield hole mobility $μ_h$ up to 9000 $cm^2 V^{-1} s^{-1}$ and electron mobility $μ_e$ up to 8000 $cm^2 V^{-1} s^{-1}$, with average values $μ_h$ 7500 $cm^2 V^{-1} s^{-1}$ and $μ_e$ 6300 $cm^2 V^{-1} s^{-1}$. The carrier mobility of ultraclean graphene reach values nearly double of that measured in graphene HBs processed with acetone cleaning, which is the method widely adopted in the field. Notably, these mobility values are obtained over large-scale and without encapsulation, thus paving the way to the adoption of graphene in optoelectronics and photonics.

cond-mat.mtrl-sci↗

arXiv2021

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, and eventually control, the cooling dynamics of the photoinduced hot-carrier distribution. There is, however, still an active debate on the different mechanisms that contribute to hot-carrier cooling. In particular, the intrinsic cooling mechanism that ultimately limits the cooling dynamics remains an open question. Here, we address this question by studying two technologically relevant systems, consisting of high-quality graphene with a mobility >10,000 cm$^2$V$^{-1}$s$^{-1}$ and environments that do not efficiently take up electronic heat from graphene: WSe$_2$-encapsulated graphene and suspended graphene. We study the cooling dynamics of these two high-quality graphene systems using ultrafast pump-probe spectroscopy at room temperature. Cooling via disorder-assisted acoustic phonon scattering and out-of-plane heat transfer to the environment is relatively inefficient in these systems, predicting a cooling time of tens of picoseconds. However, we observe much faster cooling, on a timescale of a few picoseconds. We attribute this to an intrinsic cooling mechanism, where carriers in the hot-carrier distribution with enough kinetic energy emit optical phonons. During phonon emission, the electronic system continuously re-thermalizes, re-creating carriers with enough energy to emit optical phonons. We develop an analytical model that explains the observed dynamics, where cooling is eventually limited by optical-to-acoustic phonon coupling. These fundamental insights into the intrinsic cooling mechanism of hot carriers in graphene will play a key role in guiding the development of graphene-based optoelectronic devices.

cond-mat.mes-hall↗

arXiv2020

Thermal stability of monolayer $WS_2$ in BEOL conditions

Monolayer tungsten disulfide ($WS_2$) has recently attracted large interest as a promising material for advanced electronic and optoelectronic devices such as photodetectors, modulators, and sensors. Since these devices can be integrated in a silicon (Si) chip via back-end-of-line (BEOL) processes, the stability of monolayer $WS_2$ in BEOL fabrication conditions should be studied. In this work, the thermal stability of monolayer single-crystal $WS_2$ at typical BEOL conditions is investigated; namely (i) heating temperature of $300$ $^\circ C$, (ii) pressures in the medium- ($10^{-3}$ mbar) and high- ($10^{-8}$ mbar) vacuum range; (iii) heating times from $30$ minutes to $20$ hours. Structural, optical and chemical analyses of $WS_2$ are performed via scanning electron microscopy (SEM), Raman spectroscopy, photoluminescence (PL) and X-ray photoelectron spectroscopy (XPS). It is found that monolayer single-crystal $WS_2$ is intrinsically stable at these temperature and pressures, even after $20$ hours of thermal treatment. The thermal stability of $WS_2$ is also preserved after exposure to low-current electron beam ($12$ pA) or low-fluence laser ($0.9$ $mJ/μm^2$), while higher laser fluencies cause photo-activated degradation upon thermal treatment. These results are instrumental to define fabrication and in-line monitoring procedures that allow the integration of $WS_2$ in device fabrication flows without compromising the material quality.

cond-mat.mes-hall↗

arXiv2020

Ultrafast, Zero-Bias, Graphene Photodetectors with Polymeric Gate Dielectric on Passive Photonic Waveguides

We report compact, scalable, high-performance, waveguide integrated graphene-based photodetectors (GPDs) for telecom and datacom applications, not affected by dark current. To exploit the photothermoelectric (PTE) effect, our devices rely on a graphene-polymer-graphene stack with static top split gates. The polymeric dielectric, poly(vinyl alcohol) (PVA), allows us to preserve graphene quality and to generate a controllable p-n junction. Both graphene layers are fabricated using aligned single-crystal graphene arrays grown by chemical vapor deposition. The use of PVA yields a low charge inhomogeneity 8 x 10$^{10}$ $cm^{-2}$ at the charge neutrality point, and a large Seebeck coefficient 140 $μ$V K$^{-1}$, enhancing the PTE effect. Our devices are the fastest GPDs operating with zero dark current, showing a flat frequency response up to 67 GHz without roll-off. This performance is achieved on a passive, low-cost, photonic platform, and does not rely on nanoscale plasmonic structures. This, combined with scalability and ease of integration, makes our GPDs a promising building block for next-generation optical communication devices.

physics.app-ph↗

arXiv2020

Stress-strain in electron-beam activated polymeric micro-actuators

Actuation of thin polymeric films via electron irradiation is a promising avenue to realize devices based on strain engineered two dimensional (2D) materials. Complex strain profiles demand a deep understanding of the mechanics of the polymeric layer under electron irradiation; in this article we report a detailed investigation on electron-induced stress on poly-methyl-methacrylate (PMMA) thin film material. After an assessment of stress values using a method based on dielectric cantilevers, we directly investigate the lateral shrinkage of PMMA patterns on epitaxial graphene, which reveals a universal behavior, independent of the electron acceleration energy. By knowing the stress-strain curve, we finally estimate an effective Young's modulus of PMMA on top of graphene which is a relevant parameter for PMMA based electron-beam lithography and strain engineering applications.

cond-mat.mes-hall↗

arXiv2020

Synthesis of large-area rhombohedral few-layer graphene by chemical vapor deposition on copper

Rhombohedral-stacked few-layer graphene (FLG) has been receiving an ever-increasing attention owing to its peculiar electronic properties that could lead to enticing phenomena such as superconductivity and magnetic ordering. Up to now, experimental studies on such material have been mainly limited by the difficulty in isolating it in thickness exceeding 3 atomic layers with device-compatible size. In this work, rhombohedral graphene with thickness up to 9 layers and areas up to ~50 micrometers square is grown via chemical vapor deposition (CVD) on suspended Cu foils and transferred onto target substrates via etch-free delamination. The domains of rhombohedral FLG are identified by Raman spectroscopy and are found to alternate with domains of Bernal-stacked FLG within the same crystal in a stripe-like configuration. A combined analysis of micro-Raman mapping, atomic force microscopy and optical microscopy indicates that the formation of rhombohedral-stacked FLG is strongly correlated to the copper substrate morphology. Cu step bunching results in bending of FLG and interlayer displacement along preferential crystallographic orientations, as determined experimentally by electron microscopy, thus inducing the stripe-like domains. The growth and transfer of rhombohedral FLG with the reported thickness and size shall facilitate the observation of predicted unconventional physics and ultimately add to its technological relevance.

cond-mat.mtrl-sci↗

arXiv2020

30$^\circ$-twisted bilayer graphene quasicrystals from chemical vapor deposition

The artificial stacking of atomically thin crystals suffers from intrinsic limitations in terms of control and reproducibility of the relative orientation of exfoliated flakes. This drawback is particularly severe when the properties of the system critically depend on the twist angle, as in the case of the dodecagonal quasicrystal formed by two graphene layers rotated by 30$^\circ$. Here we show that large-area 30$^\circ$-rotated bilayer graphene can be grown deterministically by chemical vapor deposition on Cu, eliminating the need of artificial assembly. The quasicrystals are easily transferred to arbitrary substrates and integrated in high-quality hBN-encapsulated heterostructures, which we process into dual-gated devices exhibiting carrier mobility up to $10^5$ cm$^2$/Vs. From low-temperature magnetotransport, we find that the graphene quasicrystals effectively behave as uncoupled graphene layers, showing 8-fold degenerate quantum Hall states: this result indicates that the Dirac cones replica detected by previous photo-emission experiments do not contribute to the electrical transport.

cond-mat.mes-hall↗

arXiv2019

Semiconductor to metal transition in two-dimensional gold and its van der Waals heterostack with graphene

The synthesis of transition metals in a two-dimensional (2D) fashion has attracted growing attention for both fundamental and application-oriented investigations, such as 2D magnetism, nanoplasmonics and non-linear optics. However, the large-area synthesis of this class of materials in a single-layer form poses non-trivial difficulties. Here we present the synthesis of a large-area 2D gold layer, stabilized in between silicon carbide and monolayer (ML) graphene. We show that the 2D-Au ML is a semiconductor with the valence band maximum 50 meV below the Fermi level. The graphene and gold layers are largely non-interacting, thereby defining a novel class of van der Waals heterostructure. The 2D-Au bands, exhibit a 225 meV spin-orbit splitting along the {ΓK} direction, making it appealing for spin-related applications. By tuning the amount of gold at the SiC/graphene interface, we induce a semiconductor to metal transition in the 2D-Au, which was never observed before and hosts great interest for fundamental physics.

cond-mat.mtrl-sci↗

arXiv2019

Local tuning of WS2 photoluminescence using polymeric micro-actuators in a monolithic van der Waals heterostructure

The control of the local strain profile in 2D materials offers an invaluable tool for tailoring the electronic and photonic properties of solid-state devices. In this paper, we demonstrate a local engineering of the exciton photoluminescence (PL) energy of monolayer tungsten disulfide (WS2) by means of strain. We apply a local uniaxial stress to WS2 by exploiting electron-beam patterned and actuated polymeric micrometric artificial muscles (MAMs), which we implement onto monolithic synthetic WS2/graphene heterostructures. We show that MAMs are able to induce an in-plane stress to the top WS2 layer of the van der Waals heterostructure and that the latter can slide on the graphene underneath with negligible friction. As a proof of concept for the local strain-induced PL shift experiments, we exploit a two-MAM configuration in order to apply uniaxial tensile stress on well-defined micrometric regions of WS2. Remarkably, our architecture does not require the adoption of fragile suspended microstructures. We observe a spatial modulation of the excitonic PL energy of the WS2 monolayers under stress, which agrees with the expected strain profile and attains a maximum redshift of about 40 meV at the maximum strain intensity point. After the actuation, a time-dependent PL blueshift is observed in agreement with the viscoelastic properties of the polymeric MAMs. Our approach enables inducing local and arbitrary deformation profiles and circumvents some key limitations and technical challenges of alternative strain engineering methods requiring the 2D material transfer and production of suspended membranes.

cond-mat.mes-hall↗

arXiv2019

Deterministic direct growth of WS2 on CVD graphene arrays

The combination of the exciting properties of graphene with those of monolayer tungsten disulfide (WS2) makes this heterostack of great interest for electronic, optoelectronic and spintronic applications. The scalable synthesis of graphene/WS2 heterostructures on technologically attractive substrates like SiO2 would greatly facilitate the implementation of novel two-dimensional (2D) devices. In this work, we report the direct growth of monolayer WS2 via chemical vapor deposition (CVD) on single-crystal graphene arrays on SiO2. Remarkably, spectroscopic and microscopic characterization reveals that WS2 grows only on top of the graphene crystals so that the vertical heterostack is selectively obtained in a bottom-up fashion. Spectroscopic characterization indicates that, after WS2 synthesis, graphene undergoes compressive strain and hole doping. Tailored experiments show that such hole doping is caused by the modification of the SiO2 stoichiometry at the graphene/SiO2 interface during the WS2 growth. Electrical transport measurements reveal that the heterostructure behaves like an electron-blocking layer at large positive gate voltage, which makes it a suitable candidate for the development of unipolar optoelectronic components.

cond-mat.mtrl-sci↗

arXiv2019

Weak localization measurements of electronic scattering rates in Li-doped epitaxial graphene

Early experiments on alkali-doped graphene demonstrated that the dopant adatoms modify the conductivity of graphene significantly, as extra carriers enhance conductivity while Coulomb scattering off the adatoms suppresses it. However, conductivity probes the overall scattering rate, so a dominant channel associated with long-range Coulomb scattering will mask weaker short-range channels. We present weak localization measurements of epitaxial graphene with lithium adatoms that separately quantify intra- and intervalley scattering rates, then compare the measurements to tight-binding calculations of expected rates for this system. The intravalley rate is strongly enhanced by Li deposition, consistent with Coulomb scattering off the Li adatoms. A simultaneous enhancement of intervalley scattering is partially explained by extra carriers in the graphene interacting with residual disorder. But differences between measured and calculated rates at high Li coverage may indicate adatom-induced modifications to the band structure that go beyond the applied model. Similar adatom-induced modifications of the graphene bands have recently been observed in ARPES, but a full theoretical understanding of these effects is still in development.

cond-mat.mes-hall↗

arXiv2019

Superlubricity of epitaxial monolayer WS2 on graphene

We report on the superlubric sliding of monolayer tungsten disulfide (WS2) on epitaxial graphene (EG) on silicon carbide (SiC). WS2 single-crystalline flakes with lateral size of hundreds of nanometers are obtained via chemical vapor deposition (CVD) on EG and microscopic and diffraction analyses indicate that the WS2/EG stack is predominantly aligned with zero azimuthal rotation. Our experimental findings show that the WS2 flakes are prone to slide over graphene surfaces at room temperature when perturbed by a scanning probe microscopy (SPM) tip. Atomistic force field based molecular dynamics simulations indicate that through local physical deformation of the WS2 flake, the scanning tip releases enough energy to the flake to overcome the motion activation barrier and to trigger an ultra-low friction roto-translational displacement, that is superlubric. Experimental observations indicate that after the sliding, the WS2 flakes rest with a rotation of npi/3 with respect to graphene. Atomically resolved investigations show that the interface is atomically sharp and that the WS2 lattice is strain-free. These results help to shed light on nanotribological phenomena in van der Waals (vdW) heterostacks and suggest that the applicative potential of the WS2/graphene heterostructure can be extended by novel mechanical prospects.

cond-mat.mtrl-sci↗

arXiv2017

Electronic properties of WS$_2$ on epitaxial graphene on SiC(0001)

This work reports an electronic and micro-structural study of an appealing system for optoelectronics: tungsten disulphide WS$_2$ on epitaxial graphene (EG) on SiC(0001). The WS$_2$ is grown via chemical vapor deposition (CVD) onto the EG. Low-energy electron diffraction (LEED) measurements assign the zero-degree orientation as the preferential azimuthal alignment for WS$_2$/EG. The valence-band (VB) structure emerging from this alignment is investigated by means of photoelectron spectroscopy measurements, with both high space and energy resolution. We find that the spin-orbit splitting of monolayer WS$_2$ on graphene is of 462 meV, larger than what is reported to date for other substrates. We determine the value of the work function for the WS$_2$/EG to be 4.5$\pm$0.1 eV. A large shift of the WS$_2$ VB maximum is observed as well , due to the lowering of the WS$_2$ work function caused by the donor-like interfacial states of EG. Density functional theory (DFT) calculations carried out on a coincidence supercell confirm the experimental band structure to an excellent degree. X-ray photoemission electron microscopy (XPEEM) measurements performed on single WS$_2$ crystals confirm the van der Waals nature of the interface coupling between the two layers. In virtue of its band alignment and large spin-orbit splitting, this system gains strong appeal for optical spin-injection experiments and opto-spintronic applications in general.

cond-mat.mes-hall↗

arXiv2016

Alkali doping of graphene: the crucial role of high temperature annealing

The doping efficiency of lithium deposited at cryogenic temperatures on epitaxial and CVD monolayer graphene has been investigated under ultra-high vacuum conditions. Change of charge carrier density was monitored by gate voltage shift of the Dirac point and by Hall measurements, in low and high doping regimes. It was found that pre-annealing the graphene greatly enhanced the maximum levels of doping that could be achieved: doping saturated at $Δn = 2\times 10^{13}$ e$^-$/cm$^2$ without annealing, independent of sample type or previous processing; after a 900 K anneal, the saturated doping rose one order of magnitude to $Δn = 2\times 10^{14}$ e$^-$/cm$^2$.

cond-mat.mes-hall↗